Updated on 2024/03/30

写真a

 
IKENAGA,Naoki
 
Organization
Faculty of Environmental and Urban Engineering Professor
Title
Professor
Contact information
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Degree

  • Doctor of Engineering ( 1991.9 )

  • Master of Engineering ( 1988.3 )

Research Areas

  • Manufacturing Technology (Mechanical Engineering, Electrical and Electronic Engineering, Chemical Engineering) / Catalyst and resource chemical process

Education

  • Kansai University   Graduate School, Division of Engineering

    1991

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    Country: Japan

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  • Kansai University   Faculty of Engineering

    - 1986

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    Country: Japan

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Professional Memberships

Committee Memberships

  • 石油学会   ジョニアソサイアティ代表  

    2003.4 - 2005.3   

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  • 石油学会   ジョニアソサイアティ幹事  

    1988.4 - 2003.3   

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Papers

  • Oxidative dehydrogenation of n-butene to buta-1,3-diene with novel iron oxide-based catalyst: Effect of iron oxide crystalline structure Reviewed

    KIYOKAWA, Takayasu, IKENAGA,Naoki

    Mol. Catal.   507, 111560-111566   2021.5

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  • Oxidative Dehydrogenation of But-1-ene to Buta-1,3-diene with V-Mg Complex Oxide Catalysts Reviewed

    IKENAGA,Naoki

    J. Jpn. Petrol. Inst.   63(5), 1-10   2020.11

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  • Photocatalytic H2O2 production from O2 under visible light irradiation over phosphate ion-coated Pd nanoparticles-supported BiVO4 Reviewed

    FUKU, Kojiro, TAKIOKA, R., IWAMURA, K., TODOROKI, M., SAYAMA, K., IKENAGA,Naoki

    Appl. Catal. B: Environ.   272, 119003-119010   2020.4

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  • Effect of Metal Addition to V-Based Complex Oxide Catalysts on Oxidative Dehydrogenation of But-1-ene Reviewed

    IKENAGA,Naoki, HATAYAMA, Junsuke, FUKU, Kojiro

    SIENCE and TECHNOLOGY REPORTS of KANSAI UNIVERSITY   62, 29-48   2020.3

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  • Oxidative Dehydrogenation of n-Butene with V-Mg Complex Oxide with Added Trivalent Metal Oxide Reviewed

    KIYOKAWA, Takayasu, HAGIHARA, Takashi, IKENAGA,Naoki

    ChemistrySelect   4   2019.2

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  • Oxidative Dehydrogenation of But-1-ene at Low Temperature with Copper Ferrite Catalysts Reviewed

    KIYOKAWA,Takayasu, IKENAGA,Naoki

    ChemistrySelect   3(23) 6426-6433   2018.8

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  • Oxidative dehydrogenation of but-1-ene with lattice oxygen in ferrite catalysts

    Takayasu Kiyokawa, Naoki Ikenaga

    Applied Catalysis A: General   536   97 - 103   2017

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:Elsevier B.V.  

    The oxidative dehydrogenation (ODH) of but-1-ene was carried out using the lattice oxygen in ferrite catalysts in the temperature range of 200–300 °C with a fixed-bed flow reactor at atmospheric pressure. Various ferrite catalysts, such as NiFe2O4/AC-500, ZnFe2O4/AC-500, CoFe2O4/AC-500, and CuFe2O4/AC-500, -400, -300, -280, were prepared in the presence of activated carbon in the calcination temperature range of 280–500 °C. When but-1-ene-TPR was measured using various ferrite catalysts, CuFe2O4/AC-500 progressed the ODH of but-1-ene at 200–300 °C. Among the catalysts, CuFe2O4/AC-500 showed the highest Buta-1,3-diene (BD) yield, at 270 °C. XRD and XPS analyses of the catalyst after the ODH suggested that the lattice oxygen in Cu-O bonded to the tetrahedral site (Cu2+ T) of the ferrite structure was used for the ODH. In addition, the used catalyst was recovered by re-oxidation with molecular O2. Moreover, CuFe2O4/AC-280, which calcined at 280 °C, had the highest specific surface area and improved the BD yield with an increase in contact area with but-1-ene. In the repeated ODH (reaction and regeneration cycle), CuFe2O4/AC-500 and -280 catalysts maintained BD yields of 7.5% and 11.3%, respectively. BD production is thought to be related to the amount of Cu2+ T.

    DOI: 10.1016/j.apcata.2017.02.004

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  • Preparation of Isolated VO43- Species in Silica Framework by Alkoxy-exchange Reactions between Metal Alkoxides and Polyethylene Glycol

    Kenta Fukudome, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    JOURNAL OF THE JAPAN PETROLEUM INSTITUTE   58 ( 3 )   153 - 164   2015.5

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:JAPAN PETROLEUM INST  

    Isolated VOx, species incorporated in an SiO2-framework were synthesized by alkoxy-exchange reactions between Si(OEt)(4), V(Ot-Bu)(3)O, and polyethylene glycol (PEG). Similar alkoxy-exchange rates between alkoxides of vanadium and silicon with PEG were necessary to obtain isolated VOx species in the SiO2-framework. Gel was formed during the exchange reaction occurring with heating from 50 to 160 degrees C, liberating ethanol and t-butanol, and the obtained gel was calcined in air at 600 degrees C. The calcined samples were characterized by N-2 adsorption, XRD, Raman, FT-IR, H-2-TPR, and NMR techniques. Adsorption-desorption isotherms of N2 of the obtained samples exhibited H-4-type hysteresis patterns, indicating the presence of narrow neck pores. In addition, the presence of micropores was confirmed. The samples had high surface areas of approximately 1000 m(2)/g, and isolated VO43- species were present in the SiO2-framework. Oxidative dehydrogenation of ethylbenzene was performed as a test reaction, using CO2 as a mild oxidant. The reaction proceeded on the isolated VO43- species in the silica framework with high ethylbenzene conversion and high selectivity for styrene.

    DOI: 10.1627/jpi.58.153

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  • Use of Trickle Bed Reactor for Fischer-Tropsch Reaction over Co-Mn/Oxidized Diamond Catalyst

    Atsuo Nishizawa, Tetsushi Kitano, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    JOURNAL OF THE JAPAN PETROLEUM INSTITUTE   57 ( 3 )   109 - 117   2014.5

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:JAPAN PETROLEUM INST  

    Fischer-Tropsch synthesis (FTS) using a Co-Mn/oxidized diamond (O-Dia) catalyst was compared among a fixed bed reactor (FBR), a trickle bed reactor (TBR), and a slurry phase reactor (SPR). For TBR and SPR, hexadecane was employed as a solvent. Regardless of the reactor, the addition of 10 mol% of Mn to Co/O-Dia catalyst greatly increased CO conversion without changing selectivity to C-5 + liquid products. The highest initial CO conversion was obtained with FBR. However, with an increase in the time on stream, CO conversion decreased, due mainly to the accumulation of high molecular weight hydrocarbons (wax) on the catalyst bed. Although with TBR the initial CO conversion was 5 % lower than that with FBR, at a feed rate of the solvent from 3 to 12 mL/(g-catalyst h), CO conversion did not decrease during a prolonged run. SPR maintained the initial CO conversion for 24 h on stream, but the CO conversion was half of that with TBR. From these findings, we propose that TBR is the most appropriate reactor type for FTS.

    DOI: 10.1627/jpi.57.109

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  • Oxidative dehydrogenation of alkanes over vanadium oxide prepared with V(t-BuO)(3)O and Si(OEt)(4) in the presence of polyethyleneglycol

    Kenta Fukudome, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    CATALYSIS TODAY   203   10 - 16   2013.3

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:ELSEVIER SCIENCE BV  

    To obtain a higher concentration of isolated VOx species, VOx species incorporated into an SiO2-frame were first synthesized by the alkoxy-exchange reaction between metal alkoxides and polyethyleneglycol. After the calcination of the synthesized samples, they were characterized by N-2 adsorption and Raman spectroscopy. The catalysts have mesopores and very high surface areas up to ca. 1000 m(2)/g, which can be controlled by the degree of polymerization of polyethyleneglycol.
    Oxidative dehydrogenation of propane using lattice oxygen of VOx incorporated into an SiO2-frame was carried out with a fix-bed flow reactor at 450 degrees C under atmospheric pressure. The catalytic activity of VOx incorporated into SiO2 was compared with that of VOx loaded onto SiO2 with similar VOx loadings. VOx incorporated into SiO2 showed higher selectivity to propylene than VOx loaded onto SiO2. The higher propylene selectivity could be ascribed to isolated VO43- species in the silica framework. (C) 2012 Elsevier B. V. All rights reserved.

    DOI: 10.1016/j.cattod.2012.04.042

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  • Steam Reforming of Glycerin Using Ni-based Catalysts Loaded on CaO-ZrO2 Solid Solution

    Susumu Kitamura, Takuya Su-enaga, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    CATALYSIS LETTERS   141 ( 6 )   895 - 905   2011.6

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:SPRINGER  

    Steam reforming of glycerin on Ni-loaded catalyst was performed using a ZrO2-based support material. The addition of CaO to ZrO2 improved the catalyst performance, and NiO/CaO-ZrO2 afforded glycerin conversion of 88.9% with an H-2 yield of 75.3% at 600 A degrees C. Carbon formation decreased from 4.2 to 2.0% with CaO-added catalyst. Solid solution was formed with the addition of CaO to ZrO2, and it exhibited basic characteristics. Further reduction of carbon formation during the reforming reaction was achieved by using a quaternary complex oxide catalyst NiO-CeO2/CaO-ZrO2, where glycerin conversion of 96.1% and a H-2 yield of 83.7% were achieved with carbon formation of 0.7% at 600 A degrees C.

    DOI: 10.1007/s10562-011-0587-1

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  • The Oxidative Dehydrogenation of Propane over NiO-ZrO2 Catalyst

    Kenta Fukudome, Aki Kanno, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    CATALYSIS LETTERS   141 ( 1 )   68 - 77   2011.1

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:SPRINGER  

    The oxidative dehydrogenation of propane (ODHP) over NiO-Bi2O3-ZrO2 catalyst was carried out with a fixed-bed flow reactor at 400 degrees C under atmospheric pressure. NiO-Bi2O3-ZrO2 prepared by the co-precipitation method afforded moderate propane conversion of 18.6% and propylene selectivity of 56.1% at 400 degrees C. From XPS analyses of the used catalysts, NiO/ZrO2 prepared by the impregnation method exhibited reduced metallic Ni species after the ODHP for 1 h. On the other hand, NiO-ZrO2 and NiO-Bi2O3-ZrO2 prepared by the co-precipitation method exhibited predominantly NiO and Ni2O3 together with a minor amount of metallic Ni. From TPR and TPO, it was suggested that propylene was formed by the reaction with adsorbed oxygen species on NiOx, in contrast, metallic Ni promoted complete oxidation of propane to decrease propylene selectivity. Thus, to maintain Ni species in the oxidized state was crucial for the high selectivity to propylene. The additive effect of Bi2O3 is ascribed to have kept NiO in the solid solution less reducible state. In addition, once metallic Ni was formed, it could easily be oxidized to NiO or Ni2O3.

    DOI: 10.1007/s10562-010-0461-6

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  • Effect of mineral matters in biomass on the gasification rate of their chars

    Toshimitsu Suzuki, Hiroshi Nakajima, Na-oki Ikenaga, Hirokazu Oda, Takanori Miyake

    Biomass Conversion and Biorefinery   1 ( 1 )   17 - 28   2011

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:Springer Verlag  

    In order to develop the effective utilization of biomass, the gasification behavior (changes in gasification rates against conversion) of various chars prepared from biomass at 1,000°C was studied. The gasification rate of char with CO2 measured at 900°C by a thermogravimetric balance was affected by the content of indigenous mineral matter such as calcium and potassium. The gasification behavior of chars were classified into following three groups: (1) the gasification rate reached a maximum in the higher conversion region, (2) the gasification rate profile showed two peaks around char conversion of 0. 2 and 0. 6 or higher, (3) the gasification rate profile fitted the random pore model. An increase in the gasification rate in a higher char conversion region was attributed to the promotion effect of the potassium catalyst. The number of active centers in the char was obtained by the O2 uptake at 200°C using pulse technique. The number of active sites was increased by potassium and calcium in biomass and the amount of O2 uptake well correlated the char gasification rate. © 2011 Springer-Verlag.

    DOI: 10.1007/s13399-011-0006-2

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  • Oxidative dehydrogenation of propane using lattice oxygen of vanadium oxides on silica

    Kenta Fukudome, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    CATALYSIS SCIENCE & TECHNOLOGY   1 ( 6 )   987 - 998   2011

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:ROYAL SOC CHEMISTRY  

    Oxidative dehydrogenation of propane using lattice oxygen of vanadium oxide was carried out with a fix-bed flow reactor at 450 degrees C under atmospheric pressure. Vanadium oxide loaded on SiO(2) from V(t-BuO)(3)O afforded a high propylene selectivity of 88.3% with a propane conversion of 26.5% based on the lattice oxygen of vanadium oxide. The catalyst prepared with V(t-BuO)(3)O exhibited higher propane conversion and propylene selectivity than that prepared with NH(4)VO(3). Raman, XPS, and XRD analyses revealed that isolated VO(4)(3-) species seem to be active sites in the ODHP. For the dehydrogenation of propane, the lattice oxygen of the isolated VO(4)(3-) species was used to give propylene and H(2)O. The isolated VO(4)(3-) species was reduced to the isolated V(3+) species and was regenerated by oxidation with oxygen. The activity was maintained for at least 10 repeated cycles, suggesting that VO(x)/SiO(2) would be a promising catalyst for ODHP.

    DOI: 10.1039/c1cy00115a

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  • Oxydative dehydrogenation of 1-butene over Cr-Ce/SiO2 in the presence of CO2

    Ohnishi Syo, Sakitani Kazutaka, Miyake Takanori, Ikenaga Naoki

    Proceeding of Annual/Fall Meetings of the Japan Petroleum Institute   2011   157 - 157   2011

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    DOI: 10.11523/sekiyu.2011f.0.157.0

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  • Oxidative dehydrogenation of alkanes over VOx-SiO<SUB>2</SUB> prepared in the presence of polyethyleneglycol

    Fukudome Kenta, Ikenaga Naoki, Suzuki Toshimitsu, Miyake Takanori

    Proceeding of Annual/Fall Meetings of the Japan Petroleum Institute   2011   158 - 158   2011

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    DOI: 10.11523/sekiyu.2011f.0.158.0

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  • Oxidative Dehydrogenation of Ethane over NiO-loaded High Surface Area ZrO2 Catalysts

    Kazuki Sakitani, Ken-ichi Nakamura, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    JOURNAL OF THE JAPAN PETROLEUM INSTITUTE   53 ( 6 )   327 - 335   2010.11

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:JAPAN PETROLEUM INST  

    The oxidative dehydrogenation of ethane (ODHE) over POn/NiO/ZrO2 (High Surface area Zirconia HSZ) catalyst was carried out with a fix-bed flow reactor at 450 degrees C under atmospheric pressure The ODHE without dilution of reactants with inert gas resulted in ethane conversion of 32 1%, with a high ethene selectivily of 64 2% and an ethene yield of 20 6% In addition, the catalytic activity did not decrease for at least 12 h In XPS analysis Ni species of NiO/HSZ catalyst after the reaction exhibited partly reduced metallic NI In contrast in POn/NiO/HSZ Ni species exhibited mostly the NiO form after the reaction It was found to be important for high ethane conversion and ethene selectivity the Ni species not to be reduced to metallic NI during the ODHE mac lion The addition of a small amount of POn to NiO/HSZ catalyst significantly contributed to the resistance to the facile reduction of NiO

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  • Selective oxidation of alcohols with molecular oxygen over Ru/CaO-ZrO2 catalyst

    Takashi Yasu-eda, Susumu Kitamura, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL   323 ( 1-2 )   7 - 15   2010.5

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:ELSEVIER SCIENCE BV  

    Selective oxidation of alcohols to carbonyl compounds with molecular oxygen was carried out over ruthenium supported on a CaO-ZrO2 solid solution prepared by the co-precipitation method. In the oxidation of benzyl alcohol, the Ru/CaO-ZrO2 catalyst gave benzaldehyde in a yield higher than 98% at 90 degrees C, and the turnover frequency reached 224 h(-1). The Ru/CaO-ZrO2 catalyst also exhibited high catalytic activities and selectivities to carbonyl compounds in the oxidation of aromatic ring-substituted benzylic, allylic, and aliphatic alcohols. Moreover, this catalyst exhibited high activities in the oxidation of alcohols at a low temperature (40 degrees C). The catalytic activity and oxidation state of ruthenium depended on the Ca/Zr molar ratio of the support, and the highest catalytic activity was obtained with Ca/Zr = 0.125. DRIFT and XPS analyses revealed that Run+-OH (n=3, 4) on the surface of CaO-ZrO2 were likely the active species in the oxidation of alcohols. (C) 2010 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.molcata.2010.03.018

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  • Role of Lattice Oxygen of Metal Oxides in the Dehydrogenation of Ethylbenzene under a Carbon Dioxide Atmosphere

    Kazuhiro Saito, Kazumi Okuda, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    JOURNAL OF PHYSICAL CHEMISTRY A   114 ( 11 )   3845 - 3854   2010.3

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:AMER CHEMICAL SOC  

    The mechanism for the dehydrogenation of ethylbenzene over V, Cr, and Fe oxides loaded oil activated carbon, powdered diamond, Al(2)O(3), and MgO was studied in the presence of CO(2). Vanadium oxide-loaded catalysts provided higher Styrene yields Wider CO(2) than Ar flow. The transient response method was carried out to understand the reaction behaviors of lattice oxygen of various metal oxides on the support. The results showed that lattice oxygen of vanadium oxide (V=O) was consumed in the dehydrogenation reaction and that reduced vanadium oxide was reoxidized with CO(2). A similar redox cycle was observed oil iron oxide-loaded activated carbon catalyst. Spectroscopic characterization revealed that vanadium oxide and iron oxide on the Support were reduced to a low valence state during the dehydrogenation reaction, and the CO(2) could oxidize the reduced Metal Oxides. In contrast. chromium(III) oxide Was not reduced during dehydrogenation Front these findings, the redox cycle over vanadium oxide- and iron oxide-loaded catalysts was concluded to be all important factor in promoting the catalytic activity with CO(2).

    DOI: 10.1021/jp906166u

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  • Production of Synthesis Gas from Methane Using Lattice Oxygen of NiO-Cr2O3-MgO Complex Oxide

    O. Nakayama, N. Ikenaga, T. Miyake, E. Yagasaki, T. Suzuki

    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH   49 ( 2 )   526 - 534   2010.1

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:AMER CHEMICAL SOC  

    To produce nitrogen-free synthesis gas or hydrogen by the partial oxidation of methane using air as ail oxidant, NiO-Cr2O3-MgO complex oxide was proposed as ail effective one. Lattice oxygen of NiO in the complex oxide was effectively transferred to CH4 to give H-2 and CO in the ratio of 2-3:1 at 700 degrees C. NiO was reduced to metallic Ni during the Course of the reaction with CH4, and the reduced Ni was successfully oxidized to NiO with air at 700 degrees C. Repeated cycles of the reaction and oxidation were carried out without any loss of activity. The role of Cr2O3 seemed to weaken the Ni-O bond in NiO-MgO complex oxide, in which NiO is less reducible with CH4 at 700 degrees C. In addition, the surface oxidation state of Ni was increased to Ni3+ with Cr2O3.

    DOI: 10.1021/ie9013474

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  • Palladium-loaded oxidized diamond catalysis for the selective oxidation of alcohols

    Takashi Yasu-eda, Ryo Se-ike, Na-oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL   306 ( 1-2 )   136 - 142   2009.7

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:ELSEVIER SCIENCE BV  

    Oxidation of alcohols (benzyl alcohol, 1-phenylethanol and cinnamyl alcohol) using oxidized diamond (O-Dia)supported Pd catalyst was studied. The O-Dia supported catalyst exhibited a high catalytic activity among the support materials of Pd-loaded catalysts in the oxidation of benzyl alcohol at 85 C, showing TOFs of 850 h(-1). The addition of small amount of CeO2 to O-Dia supports further improved catalytic activity in the oxidation of 1-phenylethanol with molecular oxygen. The promotion effect of CeO2 was the suppression of acidic properties of the Pd/O-Dia, leading to dehydration and hydrogenolysis reactions of 1-phenylethanol. In addition, the Pd/CeO2/O-Dia catalyst showed a higher catalytic activity in the oxidation of various alcohols than that of Pd/O-Dia. Moreover, the basic metal oxide-promoted catalysts exhibited high catalytic activity in the dehydrogenation of 1-phenylethanol without molecular oxygen at 120 degrees C. (C) 2009 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.molcata.2009.02.039

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  • Preferential oxidation of CO in H<SUB>2</SUB>-rich gas stream over Ru/carbon aerogel catalyst

    Horiuchi Nobuhiko, Isino Yousuke, Miyake Takanori, Suzuki Toshimitsu, Ikenaga Naoki

    Proceeding of Annual/Fall Meetings of the Japan Petroleum Institute   2009   58 - 58   2009

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    DOI: 10.11523/sekiyu.2009f.0.58.0

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  • Partial oxidation of CH(4) with air to produce pure hydrogen and syngas

    Osami Nakayama, Na-oki Ikenaga, Takanori Miyake, Eriko Yagasaki, Toshimitsu Suzuki

    CATALYSIS TODAY   138 ( 3-4 )   141 - 146   2008.11

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    The gas-solid reaction between methane and the lattice oxygen of Ni, Co, and Fe-oxides loaded on various support materials produced a synthesis gas (hydrogen and carbon monoxide) at 600-800 degrees C. Metal oxides were reduced to metals or lower valence oxides, and they were re-oxidized to oxides by introducing air after the reaction. Thus, production of hydrogen or synthesis gas free from nitrogen can be achieved alternatively without using pure oxygen. As a metal oxide, Fe(2)O(3) and Rh(2)O(3)-loaded on Y(2)O(3) exhibited the highest H(2) selectivity of 60.1% with a moderate CH(4) conversion of 54% and a high lattice oxygen utilization of 84% at 800 degrees C. (C) 2008 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.cattod.2008.05.013

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  • Liquid-phase hydrogenation of alkenes and aromatic compounds with Pd-loaded oxidized diamond catalyst

    Na-Oki Ikenaga, Tomonari Kiyomi, Itaru Yonezawa, Chieko Yukawa, Toshimitsu Suzuki

    RESEARCH ON CHEMICAL INTERMEDIATES   34 ( 5-7 )   603 - 615   2008

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:VSP BV  

    Hydrogenation reactions of alkenes (cyclohexene, ethyl acrylate, styrene and 1,5-cyclo-octadiene) and aromatic compounds (o-, m- and p-xylene) were carried out in order to examine the activity of palladium-loaded surface-oxidized diamond (Pd/O-Dia) catalyst in liquid-phase hydrogenation. The catalytic performance was compared to commercial palladium-loaded activated carbon (Pd/C) catalyst. The catalyst activities were evaluated by conversions of reactants and H-2 uptake rates in the early stage of the reaction. In all the hydrogenation reactions of alkenes and aromatic compounds, the activity of Pd/O-Dia was almost the same as or slightly higher than that of Pd/C. Dispersion of Pd metal was measured by a CO-pulsed adsorption technique and TEM observations of the catalysts. Pd dispersions were on the same order of magnitude according to the CO-pulsed adsorption technique, although the Pd/C catalyst had a higher surface area (718 m(2)/g) than that of Pd/O-Dia (23 m(2)/g). The Pd particle sizes on O-Dia measured by TEM observation were slightly smaller than those on the activated carbon. Such highly dispersed Pd particles on O-Dia would contribute to higher activity for the hydrogenation reaction of alkenes and aromatic compounds.

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  • Oxidative dehydrogenation of propane on Ni-Bi-ZrO<SUB>2</SUB> prepared by coprecipitation

    Fukudome Kenta, Kanno Aki, Ikenaga Naoki, Miyake Takanori, Suzuki Toshimitsu

    Proceeding of Annual/Fall Meetings of the Japan Petroleum Institute   2008   26 - 26   2008

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    DOI: 10.11523/sekiyu.2008.0.26.0

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  • Oxidative dehydrogenation of ethane over P/Ni/ZrO<SUB>2</SUB> catalyst

    Sakitani Kazutaka, Nakamura Kenichi, Ikenaga Naoki, Miyake Takanori, Suzuki Toshimitsu

    Proceeding of Annual/Fall Meetings of the Japan Petroleum Institute   2008   27 - 27   2008

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    DOI: 10.11523/sekiyu.2008.0.27.0

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  • Preparation of an alumina-wall tube reactor and its catalytic performance in the steam-reforming of methanol

    Fumihiko Naka-O, Na-Oki Ikenaga, Takanori Miyake, Toshimitsu Suzuki

    CHEMISTRY LETTERS   36 ( 11 )   1342 - 1343   2007.11

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:CHEMICAL SOC JAPAN  

    The inner wall of a narrow-bore aluminum tube was successfully oxidized to give a thin alumina wall by electrolysis. A Cu-Zn-loaded alumina-wall tube reactor afforded high performance in the steam reforming of CH3OH to supply H-2.

    DOI: 10.1246/cl.2007.1342

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  • Selective oxidation of alcohols over Pd and metal oxide loaded oxidized diamond catalyst

    Yasueda Takashi, Seike Ryo, Ikenaga Na-oki, Miyake Takanori, Suzuki Toshimitsu

    Proceeding of Annual/Fall Meetings of the Japan Petroleum Institute   2007   187 - 187   2007

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    Language:Japanese   Publisher:The Japan Petroleum Institute  

    DOI: 10.11523/sekiyu.2007f.0.187.0

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  • Oxidative dehydrogenation of ethane to ethylene over NiO loaded on high surface area MgO

    Ken-ichi Nakamura, Takanori Miyake, Toru Konishi, Toshimitsu Suzuki

    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL   260 ( 1-2 )   144 - 151   2006.12

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    Language:English   Publishing type:Research paper (scientific journal)   Publisher:ELSEVIER SCIENCE BV  

    The oxidative dehydrogenation of ethane over NiO-loaded MgO with high surface area was carried out using a fixed-bed flow reactor at 600 degrees C under atmospheric pressure.
    At 600 degrees C, the oxidative dehydrogenation of ethane (C2H6/O-2 = 1) without dilution with an inert gas resulted in C2H6 conversion of 68.8% and a high C2H4 selectivity of 52.8%, which corresponds to a C2H4 yield of 36.3%. In addition, the catalytic activity did not decrease for at least 10 h. X-ray photoelectron spectra of the catalysts after the reaction exhibited that the initial valence state of Ni2+ (NiO) was maintained during the oxidative dehydrogenation of ethane. However, when NiO-Ioaded MgO was reduced with H-2 prior to the reaction, C2H4 selectivity decreased to nearly zero and high CO and H-2 selectivities were observed with the C2H6 conversion of 50 %, indicating that partial oxidation of C2H6 proceeded. Therefore, it seems important to keep Ni species as an oxide phase on the support, and for this purpose, use of the high surface area of MgO is essential. (c) 2006 Elsevier B.V All rights reserved.

    DOI: 10.1016/j.molcata.2006.06.058

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  • Selective oxidation of methane to formaldehyde over antimony oxide-loaded catalyst

    H Matsumura, K Okumura, T Shimamura, N Ikenaga, T Miyake, T Suzuki

    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL   250 ( 1-2 )   122 - 130   2006.5

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    A possibility of antimony oxide as a catalyst for the selective oxidation of methane with oxygen to formaldehyde was investigated. The activity measurement was carried out at an atmospheric pressure and at 873 K, where the homogeneous gas-phase reaction was negligible. Oxidized diamond (O-Dia)-supported antimony oxide catalyst produced 1.3 mmol h(-1) g-cat(-1) of formaldehyde with a formaldehyde selectivity of 23%. On the other hand, SiO2 supported antimony oxide catalyst exhibited negligible catalytic activity. XRD and UV-vis analyses revealed that alpha-Sb2O4 was formed on the oxidized diamond while Sb6O13 was formed on SiO2. Selective oxidation of methane to formaldehyde seemed to proceed on alpha-Sb2O4 with moderate activity and selectivity to formaldehyde, via a redox cycle of alpha-Sb2O4 and Sb2O4-x. On the other hand, Sb6O13 on SiO2 was stable under the reaction conditions and the selective oxidation occurred only slightly. (c) 2006 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.molcata.2006.01.043

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  • Carbon nanofiber formation on iron group metal loaded on SiO2

    Yasuzumi Yamada, Yu-ki Hosono, Nobuyuki Murakoshi, Na-oki Higashi, Hiro-aki Ichi-oka, Takanori Miyake, Na-oki Ikenaga, Toshimitu Suzuki

    DIAMOND AND RELATED MATERIALS   15 ( 4-8 )   1080 - 1084   2006.4

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    Systematic and quantitative approaches for carbon nanofiber (CNF) synthesis with catalytic chemical vapor deposition (CCVD) method were performed. Ni, Co and Fe metals were impregnated from aqueous solutions of respective acetate onto spherical SiO2. The catalyst was reduced at a temperature range from 500 to 700 degrees C just before the reaction, and CH4, C2H6 or C2H4 was decomposed at 400 to 650 degrees C. On Co and Ni loaded catalyst the amount of CNF increased with an increase in the reaction temperature and showed maxima, irrespective of hydrocarbon sources. However, at a reaction temperature of 600 or 700 degrees C, on Co and Ni no CNF was obtained. Dispersion of Co metals on SiO2 was greatly affected by H-2 reduction temperature. At the higher reduction temperature, the amount of CNFs decreased on CO/SiO2 and CNF formation behavior was significantly affected by the hydrocarbon source, but on Ni/SiO2 the effects of reduction temperatures were not significant on the amounts of CNF. With all the hydrocarbon sources, the amounts of CNFs obtained at optimal conditions were as follows: Ni &gt; Co &gt;&gt; Fe. TEM observation of the catalysts and CNFs grown under different conditions clarified CNF growth process, for the iron group metal loaded on SiO2. (c) 2005 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.diamond.2005.11.025

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  • Synthesis of Fe2O3 in the capillary-tube reactor

    T Miyake, T Ueda, N Ikenaga, H Oda, M Sano

    JOURNAL OF MATERIALS SCIENCE   40 ( 18 )   5011 - 5013   2005.9

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    DOI: 10.1007/s10853-005-1810-5

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  • Synthesis of Fe2O3 in the capillary-tube reactor

    T Miyake, T Ueda, N Ikenaga, H Oda, M Sano

    JOURNAL OF MATERIALS SCIENCE   40 ( 18 )   5011 - 5013   2005.9

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    DOI: 10.1007/s10853-005-1810-5

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  • Partial oxidation of methane to synthesis gas over oxidized diamond supported catalysts - Catalytic behavior of nickel and cobalt species

    H Nishimoto, N Ikenaga, K Nakagawa, T Konishi, T Suzuki

    JOURNAL OF THE JAPAN PETROLEUM INSTITUTE   48 ( 5 )   290 - 300   2005.9

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    Characterization of nickel and cobalt catalysts supported on oxidized diamond (O-dia) in the partial oxidation of methane to synthesis gas was carried out by X-ray photoelectron spectroscopy (XPS) and the transient response pulse technique. Carbon deposition occurred on nickel/O-dia, but not on cobalt/O-dia catalyst at 873 K throughout prolonged reaction. XPS analyses observed partially reduced nickel oxides on nickel/O-dia catalyst after reaction with methane/oxygen (5/1) at 873 K. Co(0), partially reduced cobalt oxide, and Co(M) oxide phases were found on cobalt/O-dia catalyst after reaction at 873 K. Transient response methane/oxygen (2/1) pulse studies found a large amount of hydrogen production occurred immediately at 873 K over the nickel/O-dia catalyst. However, a very small amount of hydrogen production was seen over the cobalt/O-dia catalyst, indicating that nickel and cobalt species supported on O-dia exhibited different behavior. Transient response of the catalyst bed temperature found that endothermic reaction occurred on the nickel/O-dia catalyst at 873 K, but exothermic reaction proceeded on the cobalt/O-dia catalyst. These results suggest that methane decomposition to hydrogen is the primary reaction path over nickel/O-dia catalyst, whereas complete oxidation is the primary reaction followed by steam and carbon dioxide reforming to produce synthesis gas over the cobalt/O-dia catalyst.

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  • Production of hydrogen by steam reforming of glycerin on ruthenium catalyst

    T Hirai, N Ikenaga, T Miyake, T Suzuki

    ENERGY & FUELS   19 ( 4 )   1761 - 1762   2005.7

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    DOI: 10.1021/ef050121q

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  • Carbon nanotube formation on Ni- or Pd-loaded diamond catalysts

    N Higashi, N Ikenaga, T Miyake, T Suzuki

    DIAMOND AND RELATED MATERIALS   14 ( 3-7 )   820 - 824   2005.3

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    A new approach to synthesizing carbon nanotubes (CNTs) on the powdered diamond by catalytic chemical vapor deposition (CVD) was proposed. The catalyst was prepared by impregnating an aqueous solution of Ni(NO3)(2) or an acetone solution of Pd(CH3COO)(2) onto surface-oxidized fine powdered diamond (Ni/O-Dia, Pd/O-Dia). CNTs were obtained on the diamond by the decomposition of CH4 or C2H6 over Ni/O-Dia or Pd/O-Dia at 400-800 degrees C. CNTs on Ni/O-Dia from CH4 showed comparably straight structure to that from C2H6. CNTs on Pd/O-Dia from C2H6 at 800 degrees C exhibited uniform, thick (80-130 nm), and morphologically straight structure, which were consisted of a large numbers of thin filamentous carbons. (c) 2004 Elsevier B.V. All rights reserved.

    DOI: 10.1016/j.diamond.204.10.024

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  • H2S absorption behavior of calcium ferrite prepared in the presence of coal

    N Ikenaga, Y Ohgaito, T Suzuki

    ENERGY & FUELS   19 ( 1 )   170 - 179   2005.1

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    Calcium ferrite (CaFe2O4) absorbents of hydrogen sulfide (H2S) for hot-gas cleaning were prepared in the presence of Yallourn coal (YL). Calcium and iron nitrates in aqueous solution were impregnated onto YL, which was then dried at 70degreesC in vacuo and calcined at various temperatures in air. The performance of the absorbent was evaluated using a fixed-bed flow-type reactor that was equipped with a quadrupole mass spectrometer. The surface area of the YL char-loaded CaFe2O4 (CaFe2O4/YL) was ca. 25 m(2)/g, and its value was the same order of magnitude as those of unloaded ferrites that had been prepared by a coprecipitation method. The morphological structures of CaFe2O4/YL showed a rough surface with a macroporous structure; however, the surface of unloaded ferrites prepared by the dry process and the coprecipitation method was smooth and flat. When the absorption behaviors of CaFe2O4/YL for H2S were measured at 500degreesC, the absorption capacity of H2S with CaFe2O4/YL exhibited almost 100% of the stoichiometric amount of loaded metal species and could efficiently remove 4000 ppm of H2S to a level of &lt; 1 ppm under a space velocity of 2800 h(-1).

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  • Partial oxidation of methane to synthesis gas over oxidized diamond catalysts

    H Nishimoto, K Nakagawa, N Ikenaga, M Nishitani-Gamo, T Ando, T Suzuki

    APPLIED CATALYSIS A-GENERAL   264 ( 1 )   65 - 72   2004.6

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    Oxidized diamond (O-dia) acted as an excellent support material for the partial oxidation of methane to synthesis gas. The O-dia gave the best performance among the support materials of Ni- and Co-loaded catalysts for the partial oxidation of methane at a low temperature. A nickel (3 wt.%)/O-dia catalyst afforded a high CH4 conversion of 26.5% at a CH4 to O-2 ratio of 5 to give nearly a 1 to 2 ratio of CO and H-2 with selectivities of 70% at 873 K. Cobalt (3 wt.%)/O-dia catalyst exhibited a slightly lower catalytic activity than that of Ni (3 wt.%)/O-dia catalyst, where CH4 conversion was 23.0%. No change in the support was observed in the oxidation atmosphere at a high temperature. Carbon deposition of the catalyst surface in the reaction of CH4 was examined by thermogravimetric analyses. Carbon deposition occurred on the nickel (3 wt.%)/O-dia catalyst at below 923 K, and above this temperature no carbon deposition was seen. However, on the cobalt-loaded catalyst no carbon deposition was observed at any reaction temperature. (C) 2004 Elsevier B.V. All rights reserved.

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  • Preparation of zinc ferrite in the presence of carbon material and its application to hot-gas cleaning

    N Ikenaga, Y Ohgaito, H Matsushima, T Suzuki

    FUEL   83 ( 6 )   661 - 669   2004.4

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    In order to develop an efficient absorbent of H,S in coal gasification, zinc ferrite (ZnFe2O4) was prepared in the presence of carbon materials such as activated carbon (AC), activated carbon fiber (ACF), and Yallourn coal (YL). The absorption behavior of absorbents for H2S was examined using a fixed-bed flow type reactor equipped with a quadrupole mass spectrometer. Carbon material-supported ZnFe2O4 exhibited larger desulfurization capacity for H2S than unsupported ferrites. They could efficiently remove H2S from 4000 ppm levels in a simulated coal gasification gas to less than I ppm at 500 degreesC. The absorption capacity of H2S with ZnFe2O4/AC, ZnFe2O4/ACF, and ZnFe2O4/YL exhibited nearly 100% of stoichiometric amount of loaded metal species. They could be regenerated by an air oxidation in O-2-Ar (50 vol%) at 450 degreesC for 30 min. The regenerated ferrite can be used for repeated absorption of H2S with a very slight decrease in the absorption capacity. (C) 2003 Elsevier Ltd. All rights reserved.

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  • Direct formation of formaldehyde from methane and carbon dioxide over vanadium oxide catalysts

    T Shimamura, K Okumura, K Nakagawa, T Ando, NO Ikenga, T Suzuki

    JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL   211 ( 1-2 )   97 - 102   2004.3

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    The possibility of CO2 as an alternative oxidant for the direct conversion of CH4 to formaldehyde was investigated. The activity of the catalyst was measured at an atmospheric pressure and temperatures at which the homogeneous gas-phase reactions were negligible. Among various metal oxides loaded on SiO2 catalysts, only vanadium oxide produced the desired product. V2O5/SiO2 and V2O5/oxidized diamond catalysts, the most effective catalysts for formaldehyde synthesis, afforded about 500 mumol h(-1) g-cat(-1) and 300 mumol h(-1) g-cat(-1) of formaldehyde at 973 K, respectively. When the reaction of CH4 was carried out in Ar atmosphere, both of the V2O5/SiO2 and V2O5/oxidized diamond catalysts lost the catalytic activity as soon as the lattice oxygen of vanadium oxide was consumed. However, the activity recovered by switching the atmosphere from Ar to CO2. These results strongly suggest that CO2 acts as an oxidant for selective oxidation of CH4 to formaldehyde via the lattice oxygen of vanadium oxide. (C) 2003 Elsevier B.V. All rights reserved.

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  • 活性炭繊維布の表面官能基の修飾とその電気二重層キャパシタ電極への応用 Reviewed

    山下 曜, 箕浦 晋作, 三宅 孝典, 池永 直樹, 小田 廣和

    炭素   (214),194―201   2004

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  • Direct formation of acetaldehyde from ethane using carbon dioxide as a novel oxidant over oxidized diamond-supported catalysts

    K Okumura, K Nakagawa, T Shimamura, NO Ikenaga, M Nishitani-Gamo, T Ando, T Kobayashi, T Suzuki

    JOURNAL OF PHYSICAL CHEMISTRY B   107 ( 48 )   13419 - 13424   2003.12

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    We have developed a novel method of producing acetaldehyde directly from ethane using carbon dioxide. The selective oxidation of C2H6 using CO2 as an oxidant was studied over various metal oxide-loaded catalysts. Among metal oxides, vanadium oxide afforded the highest activity toward CH3CHO when it was loaded on the oxidized diamond. With a V2O5 loading level of 3 wt % on oxidized diamond, 140 mumol/h.g of catalyst of CH3CHO was obtained at 923 K with C2H6 and CO2 (1:1 mixed gas) in SV of 18 000 mL/h.g of catalyst. C2H4 and HCHO were obtained as byproducts. In the absence of CO2, no aldehydes were obtained, indicating that oxygen was supplied from CO2 through the vanadium oxide surface.

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  • Oxidized diamond as a simultaneous production medium of carbon nanomaterials and hydrogen for fuel cell

    K Nakagawa, MA Yamagishi, H Nishimoto, N Ikenaga, T Suzuki, T Kobayashi, M Nishitani-Gamo, T Ando

    CHEMISTRY OF MATERIALS   15 ( 24 )   4571 - 4575   2003.12

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    High yields of hydrogen and carbon nanomaterials can be obtained by the decomposition of methane using oxidized diamond-supported Ni and Pd catalysts at 873 K. This is the first report to show that oxidized diamond can serve as an active support material. The simultaneous synthesis of carbon nanomaterials and hydrogen is especially interesting. Oxidized diamond is proposed as a novel catalytic means for the synthesis of hydrogen and carbon nanomaterials, and it is suggested that oxidized diamond may catalyze unique reactions of importance in nanomaterial synthesis.

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  • Novel selective oxidation of light alkanes using carbon dioxide. Oxidized diamond as a novel catalytic medium

    K Nakagawa, K Okumura, T Shimamura, N Ikenaga, T Suzuki, T Kobayashi, M Nishitani-Gamo, T Ando

    CHEMISTRY LETTERS   32 ( 9 )   866 - 867   2003.9

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    Carbon dioxide is an effective oxidant for the conversion of alkanes to chemical feedstocks. Oxidized diamond is useful as a novel catalytic support material. Oxidized diamond provided catalytic sites for the activation of alkanes under CO2 atmosphere. The present findings also suggest that the surface-properties of oxidized diamond may facilitate unique catalytic reactions, such as alkanes conversion in the presence of CO2.

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  • Dehydrogenation of light alkanes over oxidized diamond-supported catalysts in the presence of carbon dioxide

    K Nakagawa, C Kajita, N Ikenaga, M Nishitani-Gamo, T Ando, T Suzuki

    CATALYSIS TODAY   84 ( 3-4 )   149 - 157   2003.9

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    Oxidized diamond demonstrated excellent support for the dehydrogenation of light alkanes to alkenes in the presence of CO2. Oxidized diamond-supported Cr2O3 and V2O5 catalysts exhibited comparatively higher catalytic activities in the dehydrogenation of lower alkanes in the presence of CO2. In the dehydrogenation of propane, the oxidized diamond-supported Cr2O3 and V2O5 catalysts in the presence of CO2 afforded nearly twofold higher activities than that in the absence of CO2. The activity of the oxidized diamond-supported V2O5 catalyst in the dehydrogenation of propane increased with increasing reaction temperatures. Furthermore, in the dehydrogenation of n-butane and iso-butane, a promoting effect of CO2 on butane conversion and butenes yields was observed over the oxidized diannond-supported Cr2O3 and V2O5 catalysts, though the promotion effect was small.
    UV-Vis analyses of the fresh and the reacted catalysts in the presence and absence of CO2 revealed that CO2 kept the surface V2O5 and Cr2O3 in a state of oxidation slightly higher than that in the absence of CO2. (C) 2003 Elsevier B.V. All rights reserved.

    DOI: 10.1016/S0920-5861(03)00268-2

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  • Synthesis gas production from methane using oxidized-diamond-supported group VIII metal catalysts

    K Nakagawa, H Nishimoto, M Kikuchi, S Egashira, Y Enoki, N Ikenaga, T Suzuki, M Nishitani-Gamo, T Kobayashi, T Ando

    ENERGY & FUELS   17 ( 4 )   971 - 976   2003.7

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    We performed partial oxidation, steam reforming, and CO2 reforming of CH4 to Synthesis gas, using oxidized-diamond-supported group VIII metal catalysts, to investigate the properties of oxidized diamond as a support material and to avoid carbon deposition on a metal-loaded catalyst. Nickel (5 wt %)/oxidized diamond afforded the highest CH4 conversion of 24% (CH4/O-2 = 5), giving CO and H-2 at 873 K for the partial oxidation of CH4. No carbon deposition was observed with a supported oxidized-diamond catalyst (5 wt % nickel loading level) in the partial oxidation of CH4 at &gt; 923 K. In the steam reforming of CH4, ruthenium (5 wt %)/oxidized diamond afforded a CH4 conversion of 63% (CH4/H2O = 0.33), giving CO and H-2 at 873 K. Nickel, palladium, ruthenium, and rhodium (5 wt %)/oxidized diamond showed high catalytic activities for CO2 reforming of CH4 (CH4/CO2 = 1) at 873 K.

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  • The role of chemisorbed oxygen on diamond surfaces for the dehydrogenation of ethane in the presence of carbon dioxide

    K Nakagawa, C Kajita, N Ikenaga, T Suzuki, T Kobayashi, M Nishitani-Gamo, T Ando

    JOURNAL OF PHYSICAL CHEMISTRY B   107 ( 17 )   4048 - 4056   2003.5

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    Oxidized diamond played a significant role as an efficient support for a Cr2O3-loaded catalyst during the dehydrogenation Of C2H6 to C2H4 in the presence of carbon dioxide at 923 K, giving a 22.5% C2H4 yield with a 87.7% C2H4 selectivity. The activity of the oxidized diamond-supported Cr2O3 catalyst in the presence of CO2 was about 3 times higher than that in the absence Of CO2. The activity of the oxidized diamond-supported Cr2O3 catalyst increased with increasing CO2 Partial pressures. XPS analyses of the fresh and the reacted catalysts in the presence and absence Of CO2 revealed that CO2 maintained the surface Cr2O3 at a higher-oxidation state than the reaction in the absence Of CO2. On the other hand, bulk of Cr2O3 was not reduced in either atmosphere.

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  • Partial oxidation of methane to synthesis gas over Ru-loaded Y2O3 catalysts Reviewed

    IKENAGA Naoki, Nishimoto H., Nakagawa K., Suzuki T.

    Catal. Lett.   vol.82, 161-167   2003

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  • Steam reforming of dodecane over supported iridium catalysts

    T Ando, N Ikenaga, K Nakagawa, T Suzuki

    JOURNAL OF THE JAPAN PETROLEUM INSTITUTE   45 ( 6 )   409 - 413   2002.11

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    In order to discuss the possibility of steam reforming of kerosene to produce hydrogen for the on-site fuel cell co-generation system, steam reforming of dodecane, as a model compound of kerosene, was carried out in the presence or absence of oxygen at 773-1073 K using a fixed bed flow reactor. The catalytic performance of Ru, Rh, and Ir-loaded catalysts was compared.
    In the steam reforming of dodecane, Rh/La2O3 and Ru/La2O3 afforded higher dodecane conversions and hydrogen yields than those with Ir/La2O3. Dodecane conversion, however, increased with the addition of a small amount of oxygen together with steam over Ir/La2O3 catalyst, and the conversion of dodecane reached those obtained over Rh and Ru/La2O3 catalysts. Basic support La2O3 exhibited the best performance for the steam reforming in the presence of oxygen using Ir catalyst among the supports tested.

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  • Promoting effect of sulfur compounds on the degradation of polyethylene

    T Shiro, T Kanno, K Aratani, Y Katsura, N Ikenaga, T Suzuki

    ENERGY & FUELS   16 ( 5 )   1314 - 1320   2002.9

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    The liquefaction of low-density polyethylene was studied in several solvents with or without sulfur as an additive. With the addition of molecular sulfur in the liquefaction of polyethylene in 1-methylnaphthalene, the conversion increased from 77.8% to 100%, and the oil yield increased from 62.4% to 78.7% at 673 K, as compared to the conversion and yield results of the run in the absence of sulfur. The molecular weight distributions of the oil fraction, obtained in the presence of sulfur, shifted to the lower molecular weight side as compared to that obtained without sulfur. At an elevated temperature, molecular sulfur would generate sulfur radical, which abstracts hydrogen from polyethylene to initiate the chain reactions involved in the degradation of polyethylene. The promoting effect of sulfur on the degradation of polyethylene was affected by the chemical structure of the solvent. The promoting effect of sulfur was significant in aromatic and non-hydrogen donating compounds such as 1-metliylnaphtlialene, naphthalene, and toluene. However, in tetralin no promoting effect of sulfur was observed because the sulfur radical would abstract hydrogen from the solvent and polyethylene competitively.

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  • Preparation of activated carbon-supported ferrite for absorbent of hydrogen sulfide at a low temperature

    N Ikenaga, N Chiyoda, H Matsushima, T Suzuki

    FUEL   81 ( 11-12 )   1569 - 1576   2002.7

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    An efficient absorbent of hydrogen sulfide for hot gas cleaning was developed. In order to increase the efficiency of the absorbent, activated carbon-supported ferrite was prepared and the absorption behavior of the absorbent was examined using a fixed-bed reactor and a thermogravimetric balance.
    Activated carbon-supported ferrites could be prepared at a much lower calcination temperature (400degreesC) than the typical preparation temperature of ca. 1000degreesC for a dry process, These ferrites have high surface areas up to 663 m(2)/g. Breakthrough behavior was obtained with a fixed-bed flow reactor, with almost complete absorption of hydrogen sulfide from 5000 ppm to nearly zero level being achieved at an absorption temperature of 400degreesC. The results obtained with a thermogravimetric balance indicated that the initial hydrogen sulfide absorption rate of the activated carbon-supported ferrite was about ten times higher than that of the ferrite prepared by the dry process. (C) 2002 Elsevier Science Ltd. All rights reserved.

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  • Dehydrogenation of ethylbenzene over vanadium oxide-loaded MgO catalyst: Promoting effect of carbon dioxide

    Y Sakurai, T Suzaki, K Nakagawa, N Ikenaga, H Aota, T Suzuki

    JOURNAL OF CATALYSIS   209 ( 1 )   16 - 24   2002.7

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    The dehydrogenation of ethylbenzene over a vanadium oxide-loaded MgO catalyst was investigated using carbon dioxide. The styrene yield in the presence of carbon dioxide was 2.5 times higher than that in the absence of carbon dioxide (argon atmosphere) at 823 K, indicating that carbon dioxide markedly promoted the dehydrogenation of ethylbenzene. At 873 K, the same catalyst afforded the highest styrene yield, 73.8% with a selectivity of 90.1%, in the presence of carbon dioxide. In order to elucidate the role of carbon dioxide in this reaction, characterization of the catalyst was carried out via methods such as temperature-programmed reduction, temperature-programmed reaction with carbon dioxide, and UV-visible, FT-IR, and XRD spectroscopies. Carbon dioxide behaved as an oxidant for the vanadium species, and the surface vanadium species were kept in a high oxidation state with carbon dioxide during the dehydrogenation reaction. Active phases of vanadium in the dehydrogenation reaction were believed to be V5+ species in V2O5 or Mg3V2O8 on highly dispersed MgO. The reduced species, V4+ and V3+, were less reactive sites for the dehydrogenation. (C) 2002 Elsevier Science (USA).

    DOI: 10.1006/jcat.2002.3593

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  • Diamond-supported metal catalyst: a novel medium for hydrogen production from methanol decomposition

    K Nakagawa, T Hashida, C Kajita, N Ikenaga, T Kobayashi, M Nishitani-Gamo, T Suzuki, T Ando

    CATALYSIS LETTERS   80 ( 3-4 )   161 - 164   2002

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    Oxidized diamond-supported Ni catalysts gave the best performance among the oxidized diamond-supported various metal catalysts for the decomposition of methanol to synthesis gas. Ni (5 wt%)/oxidized diamond afforded 82.5% conversion of methanol to give a CO to H-2 ratio of 1.7 at 573 K.

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  • CO2 Reforming of Methane over Ru-Loaded Lanthanoid Oxide Catalysts Reviewed

    IKENAGA Naoki, Nakagawa K., Hideshima S., Akamatsu N., Matsui N., Suzuki T.

    ACS Symposium Series   vol.809, 205-223   2002

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  • Oxidized diamond as a new catalyst support

    T Suzuki, K Nakagawa, NO Ikenaga, T Ando

    SCIENTIFIC BASES FOR THE PREPARATION OF HETEROGENEOUS CATALYSTS   143   1073 - 1079   2002

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  • Role of carbon dioxide in the dehydrogenation of ethane over gallium-loaded catalysts

    K Nakagawa, C Kajita, K Okumura, N Ikenaga, M Nishitani-Gamo, T Ando, T Kobayashi, T Suzuki

    JOURNAL OF CATALYSIS   203 ( 1 )   87 - 93   2001.10

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    The role of CO2 in the dehydrogenation of ethane over Ga2O3-loaded catalysts was examined. Ga2O3/TiO2 catalyst was found to be the most effective for the dehydrogenation of ethane to ethene in the presence of CO2 at 923 K. The activity of the Ga2O3/TiO2 catalyst in the presence Of CO2 increased with increases in the partial pressure of CO2. To maintain high catalytic activity, cofeeding of CO2 and steam was effective in the case of the Ga2O3/TiO2 catalyst. Over the Ga2O3/TiO2 catalyst, the presence of CO2 markedly promoted the dehydrogenation of ethane as compared with the absence of CO2. Using a pulsed reaction technique, the use of CO2 in the dehydrogenation of ethane was found to reduce carbon deposition over the catalyst and to assist in the rapid desorption of the product (ethene) from the catalyst's surface. (C) 2001 Academic Press.

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  • Oxidized diamond supported Ni catalyst for synthesis gas formation from methane

    K Nakagawa, H Nishimoto, Y Enoki, S Egashira, NO Ikenaga, T Kobayashi, M Nishitani-Gamo, T Ando, T Suzuki

    CHEMISTRY LETTERS   460-461 ( 5 )   460 - 461   2001.5

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    Oxidized diamond gave the best performance among the support materials of Ni loaded catalysts for the partial oxidation of methane. Ni(5 wt%)/oxidized diamond afforded 20% conversion of methane (CH4/O-2 = 5) to give CO and H-2 ratio of 2.0 at 873 K. Ni(5 wt%)/oxidized diamond also showed high catalytic activity for the CO2 reforming of methane.

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  • Alumina plate-loaded ruthenium catalyst for coal liquefaction

    K Kondo, T Kawanishi, N Ikenaga, T Suzuki

    FUEL   80 ( 7 )   1015 - 1020   2001.5

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    To prevent the plugging of a catalyst bed in a fixed bed-catalyzed coal liquefaction process. ruthenium loaded on an alumina plate catalyst is proposed. Coal slurry could pass through wide channels between plate type catalysts without leaving residue or ash. The alumina plate was prepared by anodic oxidation of an aluminum plate, and then the ruthenium was loaded onto the alumina plate from aqueous ruthenium (III) chloride solution. In the liquefaction of Tanito Harum coal with only the alumina plate in the absence of ruthenium, coal conversion of 49.4 wt% and oil yield of 29.7 wt% were obtained. The coal conversion and oil yield increased with the loading of ruthenium onto the alumina plate, and they reached maxima (conversion: 86.5 wt%, oil yield: 40.3 wt%) when 0.6 mmol of ruthenium was loaded. The ruthenium loaded on an alumina plate exhibited higher activity for coal liquefaction than ruthenium (Ru = 0.6 mmol, 5 wt%) loaded on alumina powder (conversion: 69.7 wt%, oil yield: 36.9 wt%). (C) 2001 Elsevier Science Ltd. All rights reserved.

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  • Co-liquefaction of micro algae with coal using coal liquefaction catalysts

    N Ikenaga, C Ueda, T Matsui, M Ohtsuki, T Suzuki

    ENERGY & FUELS   15 ( 2 )   350 - 355   2001.3

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    Co-liquefaction of micro algae (Chlorella, Spirulina, and Littorale) with coal (Australian Yallourn brown coal and Illinois No. 6 coal) was carried out under pressurized Hz in l-methylnaphthalene at 350-400 degreesC for 60 min with various catalysts. Co-liquefaction of Chlorella with Yallourn coal was successfully achieved with excess sulfur to iron (S/Fe = 4), where sufficient amount of Fe1-xS, which is believed to be the active species in the coal liquefaction, was produced. The conversion and the yield of the hexane-soluble fraction were close to the values calculated from the additivity of the product yields of the respective home-reactions. In the reaction with a one-to-one mixture of Chlorella and Yallourn coal, 99.8% of conversion and 65.5% of hexane-soluble fraction were obtained at 400 degreesC with Fe(CO)(5) at S/Fe = 4. When Littorale and Spirulina were used as micro algae, a similar tendency was observed with the iron catalyst. On the other hand, in the coliquefaction with Illinois No. 6 coal, which is known to contain a large amount of sulfur in the form of catalytically active pyrite, the oil yield in the co-liquefaction was close to the additivity of the respective reaction with Fe(CO)(5)-S, even at S/Fe = 2. Ru-3(CO)(12) was also effective for the. co-liquefaction of micro algae with coal.

    DOI: 10.1021/ef000129u

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  • Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported group VIII metal catalysts

    K Nakagawa, NO Ikenaga, T Kobayashi, T Suzuki

    CATALYSIS TODAY   64 ( 1-2 )   31 - 41   2001.1

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    Mechanisms of partial oxidation of methane to synthesis gas were studied using a pulsed reaction technique and temperature jump measurement. Catalyst bed temperatures were directly measured by introducing 1 and 3 ml pulses of a mixture of CH4 and O-2 (2/1). With Ir, Pt and Ni/TiO2 catalysts, a sudden temperature increase at the front edge of the catalyst bed was observed upon introduction of the pulse. The synthesis gas production basically proceeded via two-step paths consisting of highly exothermic complete methane oxidation to give H2O and CO2 followed by the endothermic reforming of methane with H2O and CO2. In contrast, with the Rh and Pd/TiO2 catalysts, the temperature at the front edge of the catalyst bed decreased upon introduction of the CH4/O-2 (2/1) pulse and a small increase in the temperature at the rear end was observed, Initially, the endothermic decomposition of CH4 to H-2 and deposited carbon or CHx probably took place at the front edge of the catalyst bed, after which the deposited carbon or generated CHx species would be oxidized into COx. When the Ru/TiO2 catalyst was used, a temperature increase at the front edge of the catalyst bed was observed upon introduction of the 3 mi pulse of CH4/O-2, In contrast, the temperature drop at the front edge of the catalyst bed was observed for a 1 ml pulse of CH4/O-2. These results seemed to exhibit two possibilities for a synthesis gas formation route over the Ru/TiO2 catalyst, The reaction pathway of the partial oxidation of methane with group VIII metal-loaded catalysts depended strongly upon the metal species and reaction conditions. (C) 2001 Elsevier Science B.V. All rights reserved.

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  • Alkylation of benzene with ethane over platinum-loaded zeolite catalyst Reviewed

    S Kato, K Nakagawa, N Ikenaga, T Suzuki

    CATALYSIS LETTERS   73 ( 2-4 )   175 - 180   2001

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    Alkylation of benzene with ethane was carried out using various zeolite catalysts at temperature ranges of 400-550 degreesC. Loading of platinum onto zeolite greatly enhanced the yield of ethylbenzene. Among the zeolites tested, H-ZSM5 and H-MCM22 showed catalytic activities. By contrast, mordenite did not yield ethylbenzene. Moderate acid strength distribution is the key factor of zeolite catalysts. Optimum catalyst and conditions for this reaction are as follows. The platinum-loaded H-ZSM5 catalyst containing 6.8 wt% Pt, at a reaction temperature of 500 degreesC, afforded ethylbenzene and styrene formation rates of 14.2 and 0.8 mmol h(-1) g-cat(-1), respectively (benzene-based yields 7.3 and 0.4%). In the alkylation of benzene with ethane over platinum-loaded H-ZSM5. ethene was initially formed from ethane over the metallic platinum. Then the alkylation proceeded over the acid sites of H-ZSM5.

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  • Reactivity of carbon species formed on supported noble metal catalysts in methane conversion reactions

    N Matsui, K Nakagawa, N Ikenaga, T Suzuki

    JOURNAL OF CATALYSIS   194 ( 1 )   115 - 121   2000.8

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    The reactivity of carbon species formed from methane decomposition over supported noble metal catalysts was examined. In the Ru-loaded case, the rate of formation of CHx species in the decomposition of CH4 and the amount of CHx species over Ru are independent of the type of support. However, the carbon species on Ru/La2O3 seems to be more uniform and reactive than that on Ru/Al2O3. After the decomposition of CH4 over Ru-loaded catalysts was carried out at 700 degrees C, a temperature-programmed reaction with D-2 was carried out. CD4 was the major product on all the supports, and only slight amounts of CH3D, CH2D2, and CHD3 were detected over La2O3, ZrO2, and Y2O3 supports. The reactivity of CHx species on Ru strongly depends on the supports. The reactivity of CHx species on Ru and Rh loaded on La2O3 can be divided into two categories, These categories are not based on the differences in the number of x in CHx species. On Ru, x in the CHx species is equal to nearly 0, with a very small portion having x = 2. On the other hand, x is almost exclusively 0 on Rh. It seems that Rh leads to a higher rate of decomposition for methane than does Ru. (C) 2000 Academic Press.

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  • Coliquefaction of coal with polyethylene using Fe(CO)(5)-S as catalyst

    T Kanno, M Kimura, N Ikenaga, T Suzuki

    ENERGY & FUELS   14 ( 3 )   612 - 617   2000.5

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    The coliquefaction of Yallourn coal (YL) with polyethylene (PE) was carried out at 400 or 425 degrees C under pressurized H-2 in 1-methylnaphthalene or tetralin. In the coliquefaction without a catalyst, the conversion and the oil yield increased by 11-12% as compared to that of expected value from the additive values of respective runs. We considered that free radicals produced from YL coal were stabilized by the hydrogen abstraction from PE during the coliquefaction, and as a result beta-scission of PE markedly proceeded. The addition of a large amount of Fe(CO)(5)-S catalyst (Fe = 1.0 mmol, 2.79 wt %, S/Fe = 2) increased the conversion and the hexane soluble oil yield in the homoliquefaction of YL coal or PE, except for the conversion of PE in the reaction with TL. However, this catalyst did not promote the conversion and the hexane-soluble oil yield in the coliquefaction of YL coal with PE. When the amount of the iron catalyst was decreased to 0.4 mmol (1.12 wt %) against the same amount of coal and PE, the conversion and the oil yield in the coliquefaction run increased as compared to the reaction without or with the large amount of catalyst (Fe = 1.0 mmol). Since the excess amount of the catalyst rapidly provided hydrogen from the gas phase to YL coal-derived free radicals, hydrogen transfer from PE to YL coal decreased greatly.

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  • Dehydrogenation of ethylbenzene with carbon dioxide using activated carbon-supported catalysts

    N Ikenaga, T Tsuruda, K Senma, T Yamaguchi, Y Sakurai, T Suzuki

    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH   39 ( 5 )   1228 - 1234   2000.5

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    Dehydrogenation of ethylbenzene to styrene under excess carbon dioxide flow was carried out over activated carbon-supported metal oxide catalysts (Cr, Mn, Co, Ni, Mo, Ru, La, and Ce) at 823 K and W/F = 35 g of catalyst.h/mol. The highest yield of styrene (about 40%) with selectivity of above 80% was obtained using activated carbon-support-ed chromium oxide (Cr/AC) and cerium oxide (Ce/AC) catalysts. The initial activities of the Cr/AC and Ce/AC catalysts were comparable to that of an iron-loaded activated carbon catalyst reported previously. Only chromium(III) oxide and cerium(IV) oxide were detected by X-ray diffraction before and after reactions at higher loading levels, and these species might have been active forms. However, a reduced chromium oxide species was detected by X-ray photoelectron spectroscopy after reaction under argon. In addition to the produced styrene, equivalent amounts of carbon monoxide and water were formed. These results suggest that the dehydrogenation of ethylbenzene to styrene proceeds via two reaction paths. One is the simple dehydrogenation and an oxidation reaction of hydrogen formed with carbon dioxide. The other is the oxidative dehydrogenation of ethylbenzene through the redox cycle of chromium(III) oxide.

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  • Oxidation capability of carbon dioxide in the dehydrogenation of ethylbenzene over vanadium oxide-loaded MgO catalyst

    Y Sakurai, T Suzaki, K Nakagawa, N Ikenaga, H Aota, T Suzuki

    CHEMISTRY LETTERS   526-527 ( 5 )   526 - 527   2000.5

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    Carbon dioxide could oxidize the reduced vanadium oxide species on MgO and keep vanadium species at a high oxidation state, during the dehydrogenation of ethylbenzene to styrene under carbon dioxide, giving a markedly high yield and selectivity of styrene.

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  • Dehydrogenation of ethylbenzene with an activated carbon-supported vanadium catalyst

    Y Sakurai, T Suzaki, N Ikenaga, T Suzuki

    APPLIED CATALYSIS A-GENERAL   192 ( 2 )   281 - 288   2000.2

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    Dehydrogenation of ethylbenzene over supported vanadium catalysts was carried out at 723-923 K, W/F of 35-105 g-cat h/mol in a carbon dioxide atmosphere (carbon dioxide/ethylbenzene of 50-70 mmol/mmol) and in an argon atmosphere. The catalyst, 1.0 mmol of vanadium loaded on 1 g of activated carbon, afforded the highest ethylbenzene conversion of 67.1%, a styrene yield of 54.2% and a styrene selectivity of 80.8% at 550 K with a W/F of 70 g-cat h/mol of ethylbenzene in carbon dioxide. Ethylbenzene conversion and styrene yield in the presence of carbon dioxide were 14.0% higher than those in argon. During the course of the reaction, carbon dioxide was reduced to the corresponding amount of carbon monoxide against the styrene yield. As a result, the same amount of water was produced. (C) 2000 Elsevier Science B.V. All rights reserved.

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  • Sulfiding behavior of iron based coal liquefaction catalyst

    N Ikenaga, H Taniguchi, A Watanabe, T Suzuki

    FUEL   79 ( 3-4 )   273 - 283   2000.2

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    In order to understand the transformation mechanisms of iron-sulfur catalyst systems to pyrrhotite, the iron catalysts (gamma-FeOOH, alpha-FeOOH, Fe(CO)(5) and Fe-3(CO)(12)) and sulfur compounds (S and H2S) were heat-treated at 150-420 degrees C with or without an activated carbon, and then subjected to XRD and XPS analyses. Pyrrhotite (Fe1-xS) was the major phase above 200 degrees C in the XRD profiles of all iron-sulfur catalyst systems. However, the formation of pyrite (FeS2) from gamma-FeOOH and gamma-FeOOH on the catalyst surface was observed at 150-325 degrees C by XPS analyses. This result seems to indicate that active species (Fe1-xS) would be transformed through FeS2 as an intermediate, but iron carbonyl complexes were directly transformed into pyrrhotite without the formation of FeS2. (C) 2000 Elsevier Science Ltd. All rights reserved.

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  • Dehydrogenation of isopropylbenzene with vanadium-oxide-loaded activated carbon catalyst in the presence of carbon dioxide

    Y Sakurai, T Suzaki, K Nakagawa, N Ikenaga, T Suzuki

    CATALYSIS LETTERS   69 ( 1-2 )   59 - 64   2000

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    Dehydrogenation of isopropylbenzene to alpha-methylstyrene was carried out using various supported metal oxide catalysts in the presence of carbon dioxide. An activated carbon-supported vanadium oxide catalyst afforded a high activity in carbon dioxide atmosphere: the alpha-methylstyrene yield in carbon dioxide atmosphere was two times greater than that in an argon atmosphere at 723 K. In order to investigate the role of carbon dioxide in this reaction, we carried out temperature-programmed reduction (TPR) studies using both fresh and used catalysts. The TPR profiles clearly indicate that carbon dioxide could keep the surface of vanadium oxide at a high oxidation state.

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  • Promoting effect of carbon dioxide on the dehydrogenation and aromatization of ethane over gallium-loaded catalysts

    K Nakagawa, C Kajita, Y Ide, M Okamura, S Kato, H Kasuya, N Ikenaga, T Kobayashi, T Suzuki

    CATALYSIS LETTERS   64 ( 2-4 )   215 - 221   2000

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    Ga2O3 and Ga2O3/TiO2 catalysts were found to be effective agents for the dehydrogenation of ethane to ethene in the presence of carbon dioxide at 650 C-degrees. The activity of the Ga2O3 and Ga2O3/TiO2 catalysts in the presence of CO2 was 2-4 times higher than that without CO2. Ethene yields reached ca. 20-25% and selectivity was ca. 70-90% at 650 C-degrees in the 17% ethane and 83% CO2 feed at an SV of 9,000 ml/(g-cat h). The presence of CO2 markedly promoted dehydrogenation of ethane over Ga2O3 and Ga2O3/TiO2 catalysts. Furthermore, the promoting effect of CO2 on the aromatization of ethane and ethene over a Ga2O3+H/ZSM-5 catalyst was also observed above 650 C-degrees. Aromatics yields were higher than those without CO2.

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  • Transient response of catalyst bed temperature in the pulsed reaction of partial oxidation of methane to synthesis gas over supported rhodium and iridium catalysts

    K Nakagawa, N Ikenaga, YH Teng, T Kobayashi, T Suzuki

    JOURNAL OF CATALYSIS   186 ( 2 )   405 - 413   1999.9

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    Mechanisms of partial oxidation of methane were studied using a pulsed reaction technique and temperature jump measurement. Catalyst bed temperatures were directly measured by introducing a pulse of a mixture of methane and oxygen (2/1), With Ir/TiO2 catalyst, a sudden temperature increase at the front edge of the catalyst bed was observed upon introduction of the pulse, but the temperature of the rear end of the catalyst bed increased only slightly. The synthesis gas production basically proceeded via a two-step path consisting of highly exothermic methane complete oxidation to give H2O and CO2, followed by the endothermic reforming of methane with H2O and CO2 over Ir/TiO2 catalyst. However, with Rh/TiO2 and Rh/Al2O3 catalysts, the temperature at the front edge of the catalyst bed decreased upon introduction of the CH4/O-2 (2/1) pulse, and a small increase in the temperature at the rear end was observed. At first, endothermic decomposition of CH4 to H-2 and deposited carbon or CHx probably took place at the front edge of the catalyst bed and then deposited carbon or generated CHx species would be oxidized into COx. However, on Rh/SiO2, synthesis gas was produced via a two-step path similar to the case of Ir/TiO2 catalyst. The reaction pathway of partial oxidation of methane with Rh-loaded catalysts depended strongly on the support materials. (C) 1999 Academic Press.

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  • Reaction mechanisms of carbon dioxide reforming of methane with Ru-loaded lanthanum oxide catalyst

    N Matsui, K Anzai, N Akamatsu, K Nakagawa, N Ikenaga, T Suzuki

    APPLIED CATALYSIS A-GENERAL   179 ( 1-2 )   247 - 256   1999.4

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    A pulsed reaction technique was applied to discuss the effect of support on the activities and mechanisms in the CO2 reforming of methane over Ru catalyst. The reaction was carried out using a fixed bed reactor equipped with an on-line mass spectrometer. Four supports: La2O3, Y2O3 and ZrO2 which showed high activity and Al2O3, commonly used one in the reforming reaction, were compared when loaded with Ru.
    After feeding CO2 at 600 degrees C, we introduced a pulse of CH4 over Ru/La2O3 catalyst under Ar steady flow. We observed the response of CO which was generated from the reaction with CHx on the ruthenium and the Ru-O-x formed during CO2 treatment or during the reaction of Ru-CHx with adsorbed CO2 onto the La2O3. Over Ru/Al2O3 catalyst, however, very small response of CO was observed. A pulse of (CO2)-C-13 was introduced under CH4 steady flow over Ru/La2O3, Ru/Y2O3 and Ru/ZrO2 catalysts. Symmetrical (CO)-C-13 responses were observed, but a small response of (CO)-C-12 from (CHx)-C-12 continued to evolve after generation of (CO)-C-13 from (CO2)-C-13 ceased.
    The following reaction cycle is believed to occur in the CO2 reforming of methane on active supports: A part of metallic ruthenium reacted with CH4 to give Ru-CHx; simultaneously ruthenium metal could be oxidized with CO2 to give Ru-O-x and CO; and then, oxygen transfer from Ru-O-x to Ru-CHx took place to give CO and metallic ruthenium.
    Distinct temperature increases in the catalyst bed for La2O3, Y2O3 and ZrO2 supports were observed with the introduction of CO2 pulses under Ar flow. On the other hand, a very small increase in the temperature of the catalyst bed was observed on Al2O3 These results indicate that CO2 reforming of CH4 with ruthenium loaded catalysts was strongly assisted by the activation of CO2 adsorbed on the basic sites. (C) 1999 Elsevier Science B.V. All rights reserved.

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  • Partial oxidation of methane to synthesis gas over iridium-nickel bimetallic catalysts

    K Nakagawa, N Ikenaga, YH Teng, T Kobayashi, T Suzuki

    APPLIED CATALYSIS A-GENERAL   180 ( 1-2 )   183 - 193   1999.4

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    Partial oxidation of methane to synthesis gas was carried out using supported iridium-nickel bimetallic catalysts, in order to reduce loading levels of iridium and nickel, and to avoid carbon deposition on nickel-based catalysts by adding iridium. The performance of supported iridium-nickel bimetallic catalysts in synthesis gas formation depended strongly upon the support materials. La2O3 gave the best performance among the support materials tested. Ir(0.25 wt%)-Ni(0.5 wt%)/La2O3 afforded 36% conversion of methane (CH4/O-2=5) to give CO and H-2 with the selectivities of above 90% at 800 degrees C, and those at 600 degrees C were 25.3% conversion of methane and CO and H-2 selectivities of about 80%, respectively. Reduced monometallic Ir(0.25 wt%)/La2O3 and Ni(0.5 wt%)/La2O3 catalysts did not produce synthesis gas at 600 degrees C. A higher conversion of methane was obtained by synergistic effects. The product concentrations of CO, H-2, and CO2, and CH4 conversion were maintained in high values, even increasing the space velocity of feed gas over Ir-Ni/La2O3 catalyst, indicating that rapid reaction takes place. As a by-product, a small amount of carbon deposition was observed, but carbon formation decreased with increasing the space velocity. On the other hand, with reduced monometallic Ni(10 wt%)/La2O3 catalyst, yield of synthesis gas and carbon decreased with increasing the space velocity. (C) 1999 Elsevier Science B.V. All rights reserved.

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  • Alkylation of benzene with ethane over platinum-loaded H-ZSM5 catalyst

    S Kato, K Nakagawa, N Ikenaga, T Suzuki

    CHEMISTRY LETTERS   207-208 ( 3 )   207 - 208   1999.3

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    Ethylbenzene was prepared from benzene and ethane, using platinum-loaded H-ZSM5 catalyst at 500 degrees C, giving the ethylbenzene and styrene space lime yields of 14.2 and 0.8 mmol h(-1) g(-1) of catalyst, respectively (benzene-based yields 6.9 and 0.4%).

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  • Co-liquefaction of coal with polyethylene in two stages Reviewed

    N Ikenaga, R Miyake, T Kanno, T Suzuki

    PROSPECTS FOR COAL SCIENCE IN THE 21ST CENTURY   1111 - 1114   1999

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    Language:English   Publishing type:Research paper (international conference proceedings)   Publisher:SHANXI SCIENCE & TECHNOLOGY PRESS  

    Co-liquefaction of Yallourn coal (YL) with polyethylene (PE) was carried out in two stages at 250 - 425 degrees C under pressurized hydrogen with or without Fe(CO)(5)-S in 1-methylnaphthalene.
    The product distribution (conversion : 73.0 %, preasphaltene : 3.8 %, asphaltene : 4.0 %, oil : 54.3 %, and gas : 11.0 %) was obtained in the two stage co-liquefaction without a catalyst at 350 degrees C for 30 min and at 425 degrees C for 30 min. As compared to single stage co-liquefaction at 425 degrees C for 60 min, the oil yield increased and the gas yield decreased. In the co-liquefaction with Fe(CO)(5)-S in two stages, the conversion (89.0 %) and the oil yield (59.8 %) were higher than those obtained in the co-liquefaction without the catalyst and in the single stage co-liquefaction with the catalyst.
    These results seemed to show that the oil fraction produced from PE at 350 degrees C acted as a good solvent for the coal liquefaction at 425 degrees C with or even without the catalyst.

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  • Dehydrogenation of ethane over gallium oxide in the presence of carbon dioxide

    K Nakagawa, M Okamura, N Ikenaga, T Suzuki, T Kobayashi

    CHEMICAL COMMUNICATIONS   1025-1026 ( 9 )   1025 - 1026   1998.5

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    Gallium oxide is found to be an effective catalyst for the dehydrogenation of ethane to ethene in the presence of carbon dioxide at 650 degrees C, giving 18.6% ethene yield with a selectivity of 94.5%.

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  • Dehydrogenation of isobutane to isobutene with iron-loaded activated carbon catalyst

    H Shimada, T Akazawa, N Ikenaga, T Suzuki

    APPLIED CATALYSIS A-GENERAL   168 ( 2 )   243 - 250   1998.3

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    Dehydrogenation of isobutane to isobutene was successufully carried out on iron loaded activated carbon catalyst at 873 K. Isobutane conversion of 48%, the yield of 40% and selctivity 80% were obtained with 0.3 mmol iron loaded on Ig of activated carbon, at 873 K with W/F of 25 g-cat-h/mol of isobutane. Cofeeding of carbon dioxide promoted dehydrogenation as compared to feeding bulk isobutane or isobutane and argon mixture. Hydrogen produced by dehydrogenation was transformed into water in the presence of carbon dioxide, and carbon dioxide was reduced to carbon monoxide. A redox cycle of Fe3O4 and metallic iron is suggested for the catalytic cycle in carbon dioxide by analyzing XRD and XPS. Carbon deposition was reduced under a carbon dioxide stream as compared with the reaction under argon atmosphere. (C) 1998 Elsevier Science B.V.

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  • Partial oxidation methane to synthesis gas over supported iridium catalysts Reviewed

    IKENAGA Naoki, K.Nakagwa, T.Suzuki, T.Kobayashi, M.Haruta

    Applied Catalysis   169, 281-290   1998

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  • Coal hydroliquefaction using highly dispersed catalyst precursors Reviewed

    IKENAGA Naoki, S.Kan-nan, T.Sakoda, T.Suzuki

    Catalysis Today   39巻99頁   1998

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    In order to discuss the hydrogen transfer process in coal liquefaction with a catalyst in the presence of a donor solvent, hydroliquefaction of Yallourn, Wyoming, Illinois No.6, and Mi-ike coals and cracking of benzyl phenyl ether (BPE) were carried out in tetralin or tetralin/naphthalene mixed solvent under a hydrogen atmosphere with highly dispersed catalyst precursors such as Fe(CO)5-S, Mo(CO)6-S, and Ru3(CO)12. In the absence of the catalyst, more than 70 % of hydrogen was transferred from tetralin, as determined by the formation of naphthalene.In the presence of Mo(CO)6-S and Ru3(CO)12, however, the amount of hydrogen transferred from tetralin decreased to 15 - 40 % of the total hydrogen and that from gas phase increased to 60 - 85 % of the hydrogen required to stabilize coal fragment radicals even with an excess amount of tetralin.When the reaction was carried out in the tetralin/naphthalene mixed solvent, little hydrogenation of naphthaleneoccurred even with the active catalyst.This strongly supports the assertion that a decrease in the amount of naphthalene in the catalyzed liquefaction of coal in tetralin with a catalyst can be ascribed to the direct hydrogen transfer from molecular hydrogen to coal fragment radicals.In the presence of coal or benzyl phenyl ether, little or no hydrogenation of naphthalene occurred.

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  • Effect of support on the conversion of methane to synthesis gas over supported iridium catalysts

    K Nakagawa, K Anzai, N Matsui, N Ikenaga, T Suzuki, YH Teng, T Kobayashi, M Haruta

    CATALYSIS LETTERS   51 ( 3-4 )   163 - 167   1998

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    A partial oxidation of methane was carried our using iridium catalysts supported on several metal oxides. The productivity of the synthesis gas from methane was strongly affected by the choice of support oxides for the catalysts. The synthesis gas production proceeded basically via a two-step reaction consisting of methane combustion to give H2O and CO2, followed by the reforming of methane from CO2 and steam. Although the combustion and the reforming of methane from steam did not depend upon the catalyst support, a large variation in the catalytic activity fbr the reforming of methane from CO2 was observed over Ir catalysts with different supports. The support activity order in the reforming of methane from CO2 with iridium catalysts was as follows: TiO2 greater than or equal to ZrO2 greater than or equal to Y2O3 &gt; La2O3 &gt; MgO greater than or equal to Al2O3 &gt; SiO2. The same order was observed in the synthesis gas production from the partial oxidation of methane.

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  • Liquefaction of micro-algae with iron catalyst

    TO Matsui, A Nishihara, C Ueda, M Ohtsuki, NO Ikenaga, T Suzuki

    FUEL   76 ( 11 )   1043 - 1048   1997.9

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    Liquefaction of Spirulina, a high-protein microalga, afforded &gt; 90 wt% of THF-soluble products and 60 wt% of hexane-soluble fractions, in the temperature range 300-425 degrees C under hydrogen in various organic solvents with highly dispersed catalysts. The oil yield increased from 52.3 to 66.9 wt% With Fe(CO)(5)-S catalyst at 350 degrees C for 60 min in tetralin under 5.0 MPa of hydrogen. Hydrogen activated by the dispersed catalyst contributed to an increase in oil yield. Liquefaction in water as solvent gave a higher oil yield of 783 wt% at 350 degrees C even under nitrogen. Liquefaction in toluene gave oil fractions of high carbon content and lower oxygen content, with a heating value of 32-33 MJ kg(-1). On the contrary, oil fractions obtained in water had a lower carbon content and higher oxygen content, with a lower heating value of 26 MJ kg(-1). The presence of moderate amount of water is considered to be effective for the production of oil of high heating value in high yield. FT-i.r. spectroscopy and gel permeation chromatograph, showed that production of oil fractions proceeded via thermal decomposition of polypeptides and hydrolysis by water produced during liquefaction in organic solvents. (C) 1997 Elsevier Science Ltd.

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  • Reactions of coal model compounds in the presence of hydrogen donor solvents and highly dispersed catalysts

    N Ikenaga, T Sakoda, T Matsui, K Ohno, T Suzuki

    ENERGY & FUELS   11 ( 1 )   183 - 189   1997.1

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    Reactions of 1,2-(1,1'-)dinaphthylethane (DNE) and 1,2-diphenylethane (DPE) in a hydrogen donor solvent in the absence or in the presence of highly dispersed catalysts such as Mo(CO)(6)-S and Ru(acac)(3) were carried out at 658 or 698 K under a hydrogen atmosphere in order to investigate quantitative hydrogen transfer process in the cracking of C-C bond in coal. Dinaphthylethane mainly produced 1-methylnaphthalene, and diphenylethane afforded benzene, toluene, and ethylbenzene as the major low molecular weight products. In addition, hydrogenation of DNE and DPE occurred. In the absence of a catalyst, more than 70 mol % of hydrogen was transferred from the hydrogen donor solvent. In the presence of Mo and Ru catalyst, the hydrogen required for stabilizing free radicals and hydrogenating aromatic rings was predominantly derived from gas phase without or with a small amount of the solvent. However, the amount of hydrogen transferred from gas phase considerably decreased and the amounts of hydrogenated products and decomposed products of DNE and DPE lowered with increasing concentration of the hydrogen donor solvent even with the dispersed Mo or Ru catalyst. The hydrogen donor solvent retarded the catalyzed cracking of DNE and DPE because of competitive adsorption of the model compound and the hydrogen donor solvent on the catalyst surface.

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  • CO2 reforming of heptane using ruthenium-loaded lanthanum oxide catalyst

    Satoshi Fujimura, Kiyoharu Nakagawa, Naoki Ikenaga, Toshimitsu Suzuki

    Sekiyu Gakkaishi (Journal of the Japan Petroleum Institute)   40 ( 3 )   179 - 184   1997

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    Reforming of heptane with CO2, using Ni and Ru catalysts was carried out. Ruthenium, supported on La2O3 exhibited high catalytic activity at 600°C in the CO2 reforming of heptane, but the activity decreased rapidly. Deactivation of the catalyst during reaction was reduced by adding LiOH(Li/Ru=3) to the catalyst, which eliminated carbon deposition. Ratio of CO/H2 was greater than that expected from the stoichiometric reaction of CO2 and C7H16. This is considered to be caused by the reverse water gas shift reaction, giving CO by reducing CO2 with H2 produced. To maintain higher catalytic activity, the formation of La2O2CO3 seems to be essential.

    DOI: 10.1627/jpi1958.40.179

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  • 8-5. Synthesis Gas Production from Methane over Iridium-supported Catalysts

    NAKAGAWA Kiyoharu, IKENAGA Naoki, SUZUKI Toshimitsu, KOBAYASHI Tetsuhiko, HARUTA Masatake

    Proceedings of the Annual Conference of The Japan Institute of Energy   6   239 - 242   1997

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    DOI: 10.20550/jietaikaiyoushi.6.0_239

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  • Ni-Mo/Al2O3およびCo-Mo/Al2O3触媒による置換フェノール類の水素化脱酸素反応 Reviewed

    池永 直樹, 奥田晴彦, 新井太, 水田晋, 鈴木俊光

    石油学会誌   40巻192頁   1997

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    置換フェノール類の水素化脱酸素反応(HDO)を市販のNi-Mo/Al2O3触媒およびCo-Mo/Al2O3触媒を用いて流通式反応装置で検討した。Ni-Mo/Al2O3触媒での主生成物は芳香環水素化の後に脱酸素されることによって得られる置換シクロヘキサン類であったが、Co-Mo/Al2O3触媒での主生成物は芳香環からの直接脱酸素によるベンゼン類であった。3,4または5位にメチル置換されたフェノール類の反応性はメチル基の電子供与性効果によりOH基と触媒表面とのより強い相互作用が生じるため置換基が存在しないフェノールの反応性より増大する傾向が認められたが、メチル基の電子供与性による促進効果はCo-Mo/Al2O3触媒の方がNi-Mo/Al2O3触媒より顕著に認められた。 2,6位にメチル置換されたフェノール類の反応性は置換基の立体障害により触媒への吸着が阻害され、著しく低下した。この傾向もまた、Co-Mo/Al2O3触媒の方がNi-Mo/Al2O3触媒より明確に現れ、Ni-Mo/Al2O3触媒では芳香環の水素化後に脱水反応により脱酸素反応が起こるため、2,6位の置換基の影響を受けにくかったものと考えると、両触媒の作用機構の差異が説明される。

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  • CO2 GASIFICATICON OF IRON-LOADED CARBONS - ACTIVATION OF THE IRON CATALYST WITH CO

    S TANAKA, T UEMURA, K ISHIZAKI, K NAGAYOSHI, N IKENAGA, H OHME, T SUZUKI

    ENERGY & FUELS   9 ( 1 )   45 - 52   1995.1

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    Carbon dioxide gasification of various iron-loaded carbon species such as Yallourn coal char, carbon black, and activated carbon were investigated. Catalytic effect of iron was pronouncedly observed when less reactive carbons such as carbon black or activated carbon was gasified at 800 degrees C. Cyclic gasification in which a gasification agent and a product CO were fed alternately was carried out in order to enhance activities of iron catalyst. When appropriate intervals in the feeding of CO2 and CO was selected (CO2 75 s and CO 120 s), gasification rate increased considerably, even with the shorter effective gasification time. Moreover, instantaneous gasification of iron-loaded carbons occurred, if the iron-loaded carbons were treated with CO at 780 to 800 degrees C for 120 s before introducing CO2. Such phenomenon is called rapid gasification and is only observed when highly dispersed alpha-iron (elucidated by EXAFS) was produced on the carbon surface. The most significant rapid gasification was observed and about 70% of original carbon was gasified within 4 min at 800 degrees C, when 1.8 mmol of iron was loaded on 1 g of carbon black (surface area 101 m(2)/g).

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  • Hydrogen transfer mechanism in the cracking of C-C bond in coal model compounds Reviewed

    N Ikenaga, T Sakoda, T Matsui, K Ohno, T Suzuki

    COAL SCIENCE, VOLS I AND II   24   1423 - 1426   1995

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  • 高分散触媒を用いた石炭液化反応における水素移動機構 Reviewed

    池永 直樹, 鈴木俊光, 河南宗作, 佐古田隆仁

    日本エネルギー学会誌   74巻280頁   1995

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    科研費特定領域研究

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  • Oxidative dehydrogenation of ethylbenzene with carbon dioxide. Reviewed

    IKENAGA Naoki, M.Sugino, H.Shimada, T.Tsuruda, H.Miura, T.Suzuki

    Applied Catalysis   121巻125頁   1995

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    An attempt to use carbon dioxide as a diluent and oxidant in the dehydrogenation of ethylbenzene to styrene was carried out over an activated carbon-supported iron catalyst (Fe 17 wt.-%) at 773-973 K, CO2/ethylbenzene = 50-70 mol/mol and W/F = 30-120 g h/mol. An addition of 20-30 mol-% lithium nitrate to iron resulted in a significant increase in the catalytic activity. The highest yield of styrene (40-45%) with more than 90% selectivity was obtained at a ratio of lithium to iron of 0.1-0.2 (mol/mol). In addition to styrene, carbon monoxide and water were formed as products. This indicated that the reaction proceeds via an oxidative dehydrogenation mechanism. Added lithium nitrate was converted into lithium ferrite during the treatment of an iron-lithium co-loaded activated carbon catalyst under carbon dioxide at 973 K. Lithium ferrite thus formed would be an active center of the reaction.

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  • 1-6. Role of Highly Dispersed Catalyst in Coal Liquefaction with Tetralin

    SUZUKI Toshimitsu, IKENAGA Naoki

    Proceedings of the Annual Conference of The Japan Institute of Energy   4   21 - 24   1995

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    Language:Japanese   Publisher:The Japan Institute of Energy  

    DOI: 10.20550/jietaikaiyoushi.4.0_21

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  • COAL HYDROLIQUEFACTION WITH IRON-LOADED COAL AS CATALYST

    S OKAMOTO, A KITAJIMA, H TANIGUCHI, N IKENAGA, T SUZUKI

    ENERGY & FUELS   8 ( 5 )   1077 - 1082   1994.9

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    In order to enhance dispersion of catalyst for coal hydroliquefaction, an iron-loaded Blind Canyon coal (Fe-BC(K)) was prepared by reducing iron ion with potassium borohydride (KBH4) in the presence of Blind Canyon coal. Hydroliquefaction of Blind Canyon coal (low pyrite content in coal) was carried out with an iron-loaded coal as catalyst in l-methylnaphthalene at 420 degrees C for 60 min under a hydrogen atmosphere (5.0 MPa cold). Iron-loaded coal Fe-BC(K) showed the highest coal conversion and oil yield amounting to 92.0 and 43.9%, respectively, among the catalysts employed in this study. Dispersed iron species on Fe-BC(K) was assigned as alpha-Fe by the X-ray diffraction analysis. Iron dispersed coal, Fe-BC(K) afforded higher coal conversion and oil yield than metallic iron powder prepared by the same method in the absence of coal. The catalytic activity could only be enhanced when the reduction of iron ion was performed in the presence of coal to give highly dispersed iron species. This was proved by X-ray diffraction analyses of line broadening. Effects of catalyst level of iron and reaction time on the product distribution, on the amount of hydrogen transferred, and on the composition of the solvent were examined.

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  • HYDROGEN-TRANSFER REACTION OF COAL MODEL COMPOUNDS IN TETRALIN WITH DISPERSED CATALYSTS

    N IKENAGA, Y KOBAYASHI, S SAEKI, T SAKOTA, Y WATANABE, H YAMADA, T SUZUKI

    ENERGY & FUELS   8 ( 4 )   947 - 952   1994.7

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    In order to discuss quantitative hydrogen-transfer process, cracking of benzyl phenyl ether (BPE) and dibenzyl ether (DBE) in tetralin using highly dispersed catalyst precursors such, as Fe(CO)5, MO(CO)6, and Ru(acac)3 was carried out at 648 K under a hydrogen atmosphere. Identified products from cracking of BPE were benzene, toluene, phenol, diphenylmethane, 1,2-diphenylethane, isomeric (hydroxyphenyl)phenylmethanes, benzyltetralins, and benzylnaphthalenes, and identified products from DBE were benzaldehyde and benzyl alcohol in addition to the above substances except phenol. The required amount of hydrogen to stabilize free radicals from BPE was in good agreedment with the amount of hydrogen transferred from tetralin and gas phase. In the absence of a catalyst, more than 90 mol % of hydrogen was transferred from tetralin. In the presence of Mo(CO)6-S, the amount of hydrogen transferred from tetralin decreased to around 15 mol % of hydrogen and the amount of hydrogen transferred from the gas phase increased to around 85 mol % of hydrogen required for stabilizing free radicals. Similar observation was obtained in the reaction with DBE without or with added catalysts. In the reaction of BPE or DBE in tetralin, hydrogenation of naphthalene to tetralin did not occur or occurred slightly even with active catalysts. The direct hydrogen transfer from molecular hydrogen to radicals occurred in the cracking of BPE and DBE with active catalysts such as dispersed Ru or Mo.

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  • 石炭液化用触媒に関する研究-モデル物質の水素化分解反応に対する各種触媒の接触作用の比較(テトラリンの効果)- Reviewed

    池永 直樹, 小田廣和, 櫻井敦, 横川親雄

    燃料協会誌   70巻978頁   1991

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  • 石炭液化用触媒に関する研究-モデル物質の水素化分解反応に対する各種触媒の接触作用の比較(反応温度の影響)- Reviewed

    池永 直樹, 小田廣和, 横川親雄

    燃料協会誌   69, 1061-1067   1990.11

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  • 石炭液化用触媒に関する研究-モデル物質の水素化分解反応に対する各種触媒の接触作用の比較(反応温度の影響)- Reviewed

    池永 直樹, 小田廣和, 横川親雄

    燃料協会誌   69, 1061-1067   1990.11

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Books

  • 触媒調製ハンドブック Reviewed

    池永直樹, 鈴木俊光( Role: Joint author)

    (株)エヌ・ティー・エス  2011 

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  • メタン高度化学変換技術集成

    池永 直樹, 鈴木 俊光( Role: Joint author)

    シーエムシー出版  2007 

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  • ナノ材料に利用するスペクトロスコピー 固体表面キャラクタリゼーションの実際

    田中 庸裕, 山下 弘巳, 池永 直樹, 他

    講談社サイエンティフィク  2005 

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MISC

  • ナノ材料にもとづいた高度環境化学技術の開発プロジェクト

    岡田 芳樹, 鈴木 俊光, 室山 勝彦, 三宅 義和, 小田 廣和, 三宅 孝典, 越智 光一, 幸塚 広光, 田實 佳郎, 池永 直樹, 春名 匠

    関大ORDIST技苑   pp.38-53   2009.3

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  • CO2 gasification behavior of various biomass chars-Effect of mineral matter in biomass char-

    Ikenaga, N., Nakajima, H., Oda, H., Suzuki, T.

    Science and Technology Reports of Kansai University   51, 61-74   2009

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  • Promoting effect of CO2 on the degradation of polyethylene to ethylene and propylene over HZSM-5 catalyst

    N. Ikenaga, Y.Miyamura, T. Suzuki

    Technology Reports of Kansai University   48, 53-62   2006

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  • The role of chemisorbed oxygen on diamond surfaces for the dehydrogenation of ethane in the presence of carbon dioxide

    NAKAGAWA K, KAJITA C, IKENAGA N, SUZUKI T, KOBAYASHI T, NISHITANI(GAMO) M, ANDO T

    JOURNAL OF PHYSICAL CHEMISTRY B   107 ( 17 )   4048 - 4056   2003

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  • H2S absorption behavior of ferrites prepared in the presence of coal.

    Y Ohgaito, H Matsushima, N Ikenaga, T Suzuki

    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY   224   U539 - U539   2002.8

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  • 担持Ga触媒を用いるエタンの脱水素反応に対する二酸化炭素の促進効果

    中川 清晴, 梶田 千晶, 奥村 公人, 池永 直樹, 小林 哲彦, 鈴木 俊光

    触媒   43 ( 2 )   134 - 136   2001.3

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  • Oxidized diamond: A novel support for catalytic dehydrogenation

    K Nakagawa, C Kajita, N Ikenaga, T Kobayashi, M Nishitani-Gamo, T Ando, T Suzuki

    CHEMISTRY LETTERS   ( 9 )   1100 - 1101   2000.9

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    We found that oxidized diamond played a significant role to improve catalyst performance of Cr2O3 catalyst during the dehydrogenation of C2H6 to C2H4 in the presence of CO2.

    DOI: 10.1246/cl.2000.1100

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  • Partial oxidation of methane to synthesis gas over supported iridium catalysts

    K Nakagawa, N Ikenaga, T Suzuki, T Kobayashi, M Haruta

    APPLIED CATALYSIS A-GENERAL   169 ( 2 )   281 - 290   1998.5

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    Partial oxidation of methane to synthesis gas was carried out using supported iridium catalysts. The performance of supported iridium catalysts in synthesis gas formation depended strongly on the support materials. Ir(5 wt%)/TiO2 afforded 25% conversion of methane (CH4/O-2=5) to give CO and H-2 With the selectivity of above 80% at 600 degrees C. Ir/TiO2 catalyst gave a CO-to-H-2 ratio of 2.0, as expected from the stoichiometric reaction. No carbon deposition was observed with the supported TiO2, and a constant activity was exhibited for at least 15 h, The synthesis gas yield with Ir/TiO2 catalyst was the same as supported Ph catalyst, which is reported to be the best catalyst for this reaction. The active species of Ir/TiO2 catalyst was found to be metallic iridium by XPS analyses. (C) 1998 Elsevier Science B.V.

    DOI: 10.1016/S0926-860X(98)00020-9

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  • Effect of support on the conversion of methane to synthesis gas over supported iridium catalysts (vol 51, pg 163, 1998)

    K Nakagawa, K Anzai, N Matsui, N Ikenaga, T Suzuki, Y Teng, T Kobayashi, M Haruta

    CATALYSIS LETTERS   53 ( 3-4 )   231 - 231   1998

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  • ROLES OF MOLECULAR-HYDROGEN AND A HYDROGEN DONOR SOLVENT IN THE CRACKING OF COAL MODEL COMPOUNDS WITH DISPERSED CATALYSTS

    T SUZUKI, N IKENAGA, T SAKOTA, T MATSUI

    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY   208   33 - FUEL   1994.8

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Presentations

  • 層状複水酸化物由来NiCuAl複合酸化物を用いたメタノールの水蒸気改質による水素製造

    赤木 太政, 福 康二郎, 池永 直樹

    日本エネルギー学会 関西支部 第63回研究発表会  2108.12 

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    Venue:大阪  

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  • 水と酸素を原料とした光触媒的な過酸化水素生成の高効率化

    岩村 一志, 福 康二郎, 池永 直樹

    日本エネルギー学会 関西支部 第63回研究発表会  2108.12 

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  • Application to Heterogeneous Fenton Reaction of Fe-typed Layered Double Hydroxide

    FUKU, K., TODOROKI, M., KANAI, H., NISHIGUCHI, T., ICHIKAWA, K., IKENAGA, N.

    2020.3 

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  • プルシアンブルー類似体を用いたフェントン反応による有機化合物の酸化分解

    辻本隼也, 福康二郎, 池永直樹

    2020.3 

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  • 酸素を原料とする過酸化水素合成の高効率化を目指したカソード電極の設計

    櫻井志保, 古閑拓海, 福康二郎, 佐山和弘, 池永直樹

    2020.3 

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  • Searching for Layered Double Hydroxide as Catalysts capable of effectively degrading Organic Pollutants

    TODOROKI, M., IWAMURA, K., FUKU, K., NISHIGUCHI, T., ICHIKAWA, K., IKENAGA, N.

    2020.3 

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  • バナジン酸ビスマス光触媒を用いた過酸化水素製造に及ぼす助触媒の影響

    瀧岡稜介, 岩村一志, 福康二郎, 佐山和弘, 池永直樹

    2020.3 

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  • 銅フェライト触媒による1-ブテンの酸化脱水素に及ぼす金属および金属酸化物の添加効果

    星田和輝, 福康二郎, 池永直樹

    2019.12 

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  • カソード電極上での酸素を原料とする過酸化水素合成の高効率化

    櫻井志保, 古閑拓海, 福康二郎, 池永直樹

    2019.12 

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  • 層状複水酸化物を用いたFenton反応による有機汚染物質の分解無害化

    轟真誠, 福康二郎, 池永直樹

    2019.12 

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  • 金属助触媒担持バナジン酸ビスマス光触媒を用いる過酸化水素製造

    瀧岡稜介, 岩村一志, 福康二郎, 池永直樹

    2019.12 

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  • Effect of metal and metal oxide addition on oxidative dehydrogenation of but-1-ene over copper ferrite catalyst

    HOSHITA, K., FUKU, K., IKENAGA, N.

    2019.10 

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  • Metal-introduced NiCuAl-LDH with chelating agent for hydrogen production from steam reforming of methanol

    AKAGI, T., FUKU, K., IKENAGA, N.

    2019.10 

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  • Efficient Production of Hydrogen Peroxide from Water on BiVO4 Photoanode

    KOGA, T., FUKU, K., IKENAGA, N.

    2019.10 

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  • Catalytic synthesis of propylene from ethanol using gallium oxide-containing silica catalyst

    IKENAGA,N., OKUMURA, Y., FUKU, K.

    2019.9 

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  • 水からのH2O2合成の高効率化を目指したBiVO4光アノード電極へのアルカリ土類金属酸化物の導入

    古閑拓海, 藤本大樹, 福康二郎, 佐山和弘, 池永直樹

    2019.7 

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  • Development of Pd-introduced WO3 Photocatalyst for Efficient Hydrogen Peroxide Production

    FUJIMOTO, D., FUKU, K., IKENAGA, N.

    2019.7 

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  • Synthesis of buta-1,3-diene from ethanol with mixed catalyst of magnesium oxide and sulfonated graphite

    IKENAGA, N., HIROTA, Y., FUKU, K.

    2019.7 

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  • Efficient H2O2 Generation from Water and Oxygen using BiVO4 Photocatalyst under Visible Light

    IWAMURA, K., FUKU, K., SAYAMA, K., IKENAGA, N.

    2019.7 

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  • 金属酸化物触媒を用いるブテン類の酸化的脱水素反応によるブタ−1,3−ジエン製造

    池永 直樹

    2019.6 

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  • 有機汚染物質の効果的な分解無害化を可能にする鉄系層状複水酸化物の開発

    轟 真誠, 金井 穂波, 岩村 一志, 福 康二郎, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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    Venue:神戸  

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  • 酸素からの高効率な過酸化水素生成を実現するPd担持WO3光触媒の設計

    藤本 大輝, 福 康二郎, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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    Venue:神戸  

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  • 新規酸化鉄系触媒を用いるn-ブテンの酸化的脱水素反応

    清川 貴康, 福 康二郎, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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  • BiVO4アノード電極上での過酸化水素合成の高効率化、日本化学会 第99春季年会2019

    古閑 拓海, 藤本 大輝, 福 康二郎, 佐山 和弘, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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  • BiVO4を用いた水と酸素からのH2O2生成の高効率化

    岩村 一志, 福 康二郎, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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    Venue:神戸  

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  • Ga2O3系触媒を用いるエタノールからのプロピレン合成

    奥村 裕輝, 福 康二郎, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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  • BiVO4光触媒と過酸化水素を利用したオレフィン酸化反応の高効率化

    小田切 大知, 福 康二郎, 池永 直樹

    日本化学会 第99春季年会2019  2019.3 

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    Venue:神戸  

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  • 水と酸素を原料とした光触媒的な過酸化水素生成の高効率化

    岩村 一志, 福 康二郎, 池永 直樹

    日本エネルギー学会 関西支部 第63回研究発表会  2018.12 

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    Venue:大阪  

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  • 層状複水酸化物由来NiCuAl複合酸化物を用いたメタノールの水蒸気改質による水素製造

    赤木 太政, 福 康二郎, 池永 直樹

    日本エネルギー学会 関西支部 第63回研究発表会  2018.12 

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    Venue:大阪  

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  • NiCuAl complex oxide catalysts derived from layered double hydroxide for hydrogen production from steam reforming of methanol

    AKAGI, Taisei, FUKU, Kojiro, IKENAGA,Naoki

    OKCAT2018  2018.10 

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    Venue:Osaka  

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  • Synthesis of propylene from ethanol over gallium oxide based-catalyst

    OKUMURA, Yuki, FUKU, Kojiro, IKENAGA,Naoki

    OKCAT2018  2018.10 

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    Venue:Osaka  

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  • Hydrogen peroxide production from water and oxygen using Au-supported BiVO4 photocatalyst

    IWAMURA, Kazushi, FUKU, Kojiro, IKENAGA,Naoki

    OKCAT2018  2018.10 

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    Venue:Osaka  

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  • Reductive hydrogen peroxide production on metallic co-catalyst supported WO3

    FUJIMOTO, Daiki, FUKU, Kojiro, IKENAGA,Naoki

    OKCAT  2018.10 

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    Venue:Osaka  

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  • Styrene oxidation on core-shell typed Au-BiVO4@SiO2 using hydrogen peroxide

    ODAGIRI, Daichi, FUKU, Kojiro, IKENAGA,Naoki

    OKCAT2018  2018.10 

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    Venue:Osaka  

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  • Design of Fe-typed Layered Double Hydroxide for Degradation of Organic Pollutants by Fenton Process

    FUKU, Kojiro, KANAI, Honami, IKENAGA,Naoki

    OKCAT2018  2018.10 

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    Venue:Osaka  

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  • Oxidative dehydrogenation of but-1-ene with CuO-loaded catalyst

    KIYOKAWA, Takayasu, FUKU, KOojiro, IKENAGA,Naoki

    Chemeca2018  2018.9 

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    Venue:Queenstown (New Zealand)  

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  • Fe系層状複水酸化物を用いた有機汚染物質の酸化分解に及ぼすアニオン種の影響

    福 康二郎, 金井 穂波, 池永 直樹

    第122回触媒討論会  2018.9 

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    Venue:盛岡  

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  • Effect of Au-supporting Method on BiVO4 Photocatalyst on Efficient Hydrogen Peroxide Production

    IWAMURA, Kazushi, FUKU, Kojiro, IKENAGA,Naoki

    Chemeca2018  2018.9 

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    Venue:Queenstown (New Zealand)  

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  • Synthesis of propylene from ethanol with NiO-based catalyst

    OKUMURA, Yuki, FUKU, Kojiro, IKENAGA,Naoki

    Chemeca2018  2018.9 

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    Venue:Queenstown (New Zealand)  

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  • Hydrogen production by steam reforming of methanol with NiCuAl complex oxide catalysts derived from layered double hydroxide

    AKAGI, Taisei, FUKU, Kojiro, IKENAGA,Naoki

    Chemeca2018  2018.9 

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    Venue:Queenstown (New Zealand)  

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  • Preparation of Core-Shell typed Au-BiVO4@SiO2 for Styrene Oxidation Using Hydrogen Peroxide

    ODAGIRI, Daichi, FUKU, Kojiro, IKENAGA,Naoki

    ISEAS2018  2018.8 

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    Venue:Guam (USA)  

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  • Effects of Metallic Co-Catalysts on WO3 Photocatalyst for Efficient Proenviroduction of Hydrogen Peroxide by Oxygen Reduction

    FUJIMOTO, Daiki, FUKU, Kojiro, IKENAGA,Naoki

    ISEAS2018  2018.8 

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    Venue:Guam (USA)  

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  • Degradation of Organic Pollutants on Fe-Typed Layered Double Hydroxide by Fenton Process Using Hydrogen Peroxide

    FUKU, Kojiro, KANAI, Honami, IKENAGA, Naoki

    2018.8 

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    Venue:Guam (USA)  

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  • 助触媒担持酸化タングステン光触媒上での酸素からの過酸化水素製造

    藤本 大輝, 福 康二郎, 池永 直樹

    第37回光がかかわる触媒化学シンポジウム  2018.7 

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    Venue:大阪  

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  • 効率的なH2O2生成を目指したAu助触媒担持BiVO4光触媒の設計

    岩村 一志, 福 康二郎, 池永 直樹

    第37回光がかかわる触媒化学シンポジウム  2018.7 

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    Venue:大阪  

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  • 過酸化水素による水中有機汚染物質の効率的分解を目指したFeAl-LDHの設計

    福 康二郎, 金井 穂波, 池永 直樹

    第7回JACI/GSCシンポジウム  2018.6 

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    Venue:神戸  

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  • CuO担持SiO2触媒上での1-ブテンの酸化的脱水素反応による高選択的1,3-ブタジエン生成

    清川 貴康, 池永 直樹

    第7回JACI/GSCシンポジウム  2018.6 

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    Venue:神戸  

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  • 過酸化水素を用いたスチレン酸化反応のためのコアシェル型Au-BiVO4@SiO2触媒の調製

    小田切 大知, 福 康二郎, 池永 直樹

    第7回JACI/GSCシンポジウム  2018.6 

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    Venue:神戸  

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  • NiO含有SiO2-Al2O3触媒を用いるエタノールからのプロピレン合成

    奥村 裕輝, 池永 直樹

    石油学会第67回研究発表会  2018.5 

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    Venue:東京  

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  • 酸素還元による光触媒的な過酸化水素製造の高効率化を目指した金属助触媒の探索

    池永 直樹, 藤本 大輝, 福 康二郎

    2018.3 

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  • 有機汚染物質の効果的な分解を目指したFe系層状複水酸化物の設計

    池永 直樹, 福 康二郎, 金井 穂波, 奥薗 若奈

    日本化学会 第98春季年会  2018.3 

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  • Au-BiVO4光触媒を用いる過酸化水素生成に及ぼすAu担持条件の影響

    池永 直樹, 岩村 一志, 福 康二郎

    日本化学会 第98春季年会  2018.3 

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  • NiO系触媒を用いるエタノールからのプロピレン合成

    池永 直樹, 奥村 裕輝, 福 康二郎

    日本エネルギー学会 関西支部 第62回研究発表会  2017.12 

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  • Steam reforming of methane with Pt nanoparticles supported on Ti-containing silica prepared by photo-assisted deposition method

    N. Ikenaga, H. Ishikawa, T. Kiyokawa

    第10回触媒表面化学研究発表会  2017.10 

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  • Effect of various copper oxides catalyst on oxidative dehydrogenation of but-1-ene

    N. Ikenaga, T. Kiyokawa

    第10回触媒表面化学研究発表会  2017.10 

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  • 銅酸化物系触媒を用いる1-ブテンの酸化的脱水素反応

    池永 直樹, 清川 貴康

    第120回触媒討論会  2017.9 

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  • Design of composite catalysts introduced tungstate and inorganic anions on calcined LDH for controlling oxidative reaction property using hydrogen peroxide

    N. Ikenaga, K. Fuku, S. Fujimoto

    254th ACS National Meeting  2017.8 

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  • Oxidative dehydrogenation of but-1-ene with copper oxide catalyst

    N. Ikenaga, T. Kiyokawa, K. Fuku

    254th ACS National Meeting  2017.8 

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  • Steam reforming of methane with Pt nanoparticles supported on composite oxide of TiO2 and SiO2 prepared by photo-assisted deposition method

    N. Ikenaga, H. Ishikawa

    254th ACS National Meeting  2017.8 

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  • Ptナノ粒子担持Ti含有メソポーラスシリカを用いるメタンの水蒸気改質

    池永 直樹, 石川 北斗, 福 康二郎

    石油学会 第66回研究発表会  2017.5 

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  • 層状複水酸化物を用いる工業廃水からのフッ素およびホウ素の吸着除去

    池永 直樹, 清川 貴康, 前田 雄亮

    日本化学会 第97春季年会  2017.3 

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  • Nd-Ni系複合金属酸化物触媒を用いる酢酸の水蒸気改質による水素製造

    池永 直樹, 牧 智仁, 福 康二郎

    日本化学会 第97春季年会  2017.3 

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  • MgO+酸化ダイヤモンド混合触媒を用いるエタノールからの1,3-ブタジエン合成

    池永 直樹, 藤林 龍矢, 福 康二郎

    日本化学会 第97春季年会  2017.3 

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  • 酸化的な有機変換反応の高効率化を目指したアニオン含有触媒の設計

    池永 直樹, 福 康二郎, 藤本 駿平

    日本化学会 第97春季年会  2017.3 

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  • V-Co複合酸化物触媒を用いる1-ブテンの酸化的脱水素反応に及ぼすMgの添加効果

    池永 直樹, 畑山 順介, 福 康二郎

    日本化学会 第97春季年会  2017.3 

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  • Ru/CaO-ZrO2を用いるアンモニア分解による水素製造に及ぼすKの添加効果

    池永 直樹, 小川 涼平, 福 康二郎

    日本化学会 第97春季年会  2017.3 

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  • Ru系触媒を用いるグアイアコールの水素化脱酸素反応

    池永 直樹, 岩城 百音

    第46回石油・石油化学討論会  2016.11 

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  • 銅フェライト触媒を用いる1-ブテンの酸化的脱水素反応に及ぼす調製法の影響

    池永 直樹, 清川 貴康

    第9回触媒表面化学研究発表会  2016.10 

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  • Ru担持活性炭触媒を用いるグアイアコールの水素化脱酸素反応

    池永 直樹, 岩城 百音

    第9回触媒表面化学研究発表会  2016.10 

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  • Oxidative dehydrogenation of 1-butene with copper ferrite catalysts prepared by various preparation methods

    N. Ikenaga, T. Kiyokawa

    Chemeca 2016  2016.9 

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  • Hydrodeoxygenation of guaiacol over Ru-loaded activated carbon catalyst

    N. Ikenaga, M. Iwaki

    Chemeca 2016  2016.9 

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  • Oxidative dehydrogenation of 1-butene with copper ferrite catalysts prepared by various preparation methods

    N. Ikenaga, T. Kiyokawa

    第5回JACI/GSCシンポジウム  2016.5 

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  • Synthesis of 1,3-butadiene from ethanol with MgO-loaded Al2O3-ZrO2 catalyst

    N Ikenaga, R. Fujibayashi

    2015 International Chemical Congress of Pacific Basin Societies  2015.12 

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  • Effect of basic property of Co-loaded catalysts on hydrodeoxygenation of guiacol

    N. Ikenaga, M. Iwaki

    2015 International Chemical Congress of Pacific Basin Societies  2015.12 

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  • 白金内包中空シリカ触媒の調製および活性評価

    池永 直樹, 森 拓人

    日本エネルギー学会関西支部第60回研究発表会  2015.12 

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  • Co 担持触媒を用いるグアイアコールの水素化脱酸素反応における担体塩基性質の影響

    池永 直樹, 岩城 百音

    日本エネルギー学会関西支部第60回研究発表会  2015.12 

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  • Effect of preparation method on 1,2-dichloropropane combustion with Fe2O3/WOx-ZrO2

    N. Ikenaga, Y. Shinada

    2015 International Chemical Congress of Pacific Basin Societies  2015.12 

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  • Fe2O3/WOx-ZrO2を用いる1,2- ジクロロプロパンの燃焼活性に及ぼす酸性質の影響

    池永 直樹, 品田 雄治

    日本エネルギー学会関西支部第60回研究発表会  2015.12 

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  • Oxidative dehydrogenation of 1-butene using copper ferrite catalyst prepared with activated carbon

    N. Ikenaga, T. Kiyokawa

    2015 International Chemical Congress of Pacific Basin Societies  2015.12 

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  • Preparation of Pt-included hollow silica and its activity for CO oxidation

    N. Ikenaga, T. Mori

    2015 International Chemical Congress of Pacific Basin Societies  2015.12 

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  • Effect of iron addition on oxidative dehydrogenation of 1-butene using V-Mg complex oxide

    N. Ikenaga, J. Hatayama

    2015 International Chemical Congress of Pacific Basin Societies  2015.12 

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  • エタノールからの1,3-ブタジエン合成におけるMgO担持触媒の酸・塩基性質の影響

    池永 直樹, 藤林 龍矢

    第8回触媒表面化学研究発表会  2015.11 

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  • 銅フェライト触媒を用いる1-ブテンの酸化的脱水素反応―アンモニア処理の影響―

    池永 直樹, 清川 貴康

    第45回石油・石油化学討論会  2015.10 

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  • V-Mg複合酸化物触媒を用いる1-ブテンの酸化的脱水素反応―鉄の添加効果―

    池永 直樹, 畑山 順介, 萩原 孝志

    第45回石油・石油化学討論会  2015.10 

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  • 銅フェライト触媒を用いる1-ブテンの酸化的脱水素反応

    池永 直樹, 清川 貴康

    石油学会第64回研究発表会  2015.5 

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  • MgO担持触媒を用いるエタノールからの1,3-ブタジエン合成

    池永 直樹, 藤林 龍矢

    石油学会第64回研究発表会  2015.5 

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  • Fe2O3/WOx-ZrO2を用いる1,2-ジクロロプロパンの燃焼活性に及ぼす担体調製法の影響

    池永 直樹, 品田 雄治

    日本化学会第95春季年会講演予稿集  2015.3 

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  • Pt担持内包中空シリカの調製およびCO酸化反応による活性評価

    池永 直樹, 森 拓人

    日本化学会第95春季年会講演予稿集  2015.3 

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  • チタン複合酸化物を用いた 1,2-ジクロロプロパンの燃焼に及ぼす酸性質の影響

    池永 直樹, 山森 正也

    日本エネルギー学会関西支部第59回研究発表会  2014.12 

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  • スルホ基導入中空シリカ触媒の調製およびベンゼンのベンジル化反応に対する活性評価

    池永 直樹, 大塚 哲

    第44回石油・石油化学討論会  2014.10 

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  • Effect of Iron Addition on Oxidative Dehydrogenation of 1-Butene Using Lattice Oxygen of V-Mg Complex Oxide

    N. Ikenaga, T. Hagihara

    Chemeca2014  2014.9 

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  • Effect of Base Property of Support on Selective Oxidation of Alcohol Using Ru Supported Catalysts

    N. Ikenaga, J. Fujito

    Chemeca2014  2014.9 

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  • Direct Synthesis and Characterization of Sulfonic Acid Functionalized Hollow Silica

    N. Ikenaga, T. Otsuka

    Chemeca2014  2014.9 

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  • Oxidative Dehydrogenation of 1-Butene Using Lattice Oxygen of Ferrite Catalyst

    N. Ikenaga, T. Kiyokawa

    Chemeca2014  2014.9 

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  • 酸化鉄系触媒の格子酸素を用いる 1-ブテンの酸化的脱水素反応、第113回触媒討論会、2P14

    清川貴康, 池永直樹

    第113回触媒討論会  2014.3 

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  • V-Mg複合酸化物の格子酸素を用いる1-ブテンの酸化的脱水素反応に及ぼす鉄の添加効果

    萩原孝志, 池永直樹

    日本化学会第94春季年会講演予稿集  2014.3 

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  • Ru担持触媒を用いるアルコール選択酸化反応に及ぼす担体の塩基性質の影響

    藤戸淳, 池永直樹

    日本化学会第94春季年会講演予稿集  2014.3 

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  • カーボン系固体酸触媒を用いたセルロースからのグルコース生成、日本エネルギー学会関西支部第58回研究発表会, O7

    宇野健太郎, 池永直樹

    日本エネルギー学会関西支部第58回研究発表会  2013.12 

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  • Co-V系複合酸化物の格子酸素を用いる1-ブテンの酸化的脱水素反応、第43回石油・石油化学討論会, 2D06

    静間貴哉, 池永直樹

    第43回石油・石油化学討論会  2013.11 

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  • Oxidative dehydrogenation of 1-butene with lattice oxygen of V-Mg-Al complex oxide

    N. Ikenaga, S. Ohnishi

    Chemeca2013  2013.9 

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  • Pt担持中空シリカ触媒を用いる芳香族および脂肪族化合物の液相水素化反応, 日本エネルギー学会関西支部第57回研究発表会, O7

    西岡弘樹, 池永直樹

    ,日本エネルギー学会関西支部第57回研究発表会  2012.12 

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  • ポリエチレングリコール存在下で調製したVOx系触媒を用いるアルカンの酸化的脱水素反応

    福留健太, 池永直樹, 鈴木俊光, 三宅孝典

    第42回石油・石油化学討論会  2012.10 

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  • 金属酸化物の格子酸素を利用した低級炭化水素の部分酸化反応および酸化的脱水素反応

    池永直樹

    第110回触媒討論会  2012.9 

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  • 金属酸化物の格子酸素を利用した低級炭化水素の部分酸化反応および酸化的脱水素反応

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    第110回触媒討論会  2012.9 

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  • 金属アルコキシドとポリエチレングリコールのアルコキシ 交換反応によるVOx-SiO2触媒の調製と脱水素反応への適用

    福留健太, 池永直樹, 鈴木俊光, 三宅孝典

    第109回触媒討論会予稿集  2012.3 

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  • V-Mg-Al複合酸化物の格子酸素を用いる1-ブテンの酸化的脱水素反応

    大西 翔, 池永直樹

    日本化学会第92春季年会講演予稿集  2012.3 

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  • Cr-Ce/SiO2触媒を用いたCO2気流下での1-ブテンの酸化的脱水素反応

    大西 翔, 崎谷一貴, 三宅孝典, 池永直樹

    第41回石油・石油化学討論会講演要旨  2011.11 

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  • ポリエチレングリコール存在下で調製したVOx-SiO2触媒を用いるアルカンの酸化的脱水素反応

    福留健太, 池永直樹, 鈴木俊光, 三宅孝典

    第41回石油・石油化学討論会講演要旨  2011.11 

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  • Oxidative dehydrogenation of ethane over NiO-loaded high surface area ZrO2 catalysts

    Ikenaga, N., Sakitani, K., Nakamura, K., Miyake, T., Suzuki, T.

    Chemeca2011  2011.9 

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  • Oxidative dehydrogenation of propane with lattice oxygen of V2O5/SiO2

    Fukudome, K., Ikenaga, N., Miyake, T., Suzuki, T.

    2010 International Chemical Congress of Pacific Basin Societies  2010.12 

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  • Preferential CO oxidation in hydrogen-rich stream over Ru/carbon catalysts

    Horiuchi, N., Miyake, T., Suzuki, T., Ikenaga, N.

    2010 International Chemical Congress of Pacific Basin Societies  2010.12 

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  • Role of lattice oxygen of metal oxides in the dehydrogenation of ethylbenzene under carbon dioxide atmosphere

    Ikenaga, N., Saito, K., Okuda, K., Miyake, T., Suzuki, T.

    2010 International Chemical Congress of Pacific Basin Societies  2010.12 

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  • Co/MgO触媒を用いるCNT合成における炭素/酸素のCNTの結晶性に与える影響

    川嶋 優, 池永直樹, 三宅孝典, 鈴木俊光

    日本化学会第90春季年会講演予稿集  2010 

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  • 種々のリン酸塩を触媒担体に用いるエタンの酸化的脱水素反応

    辻 邦啓, 徳重 信, 池永直樹, 三宅孝典, 鈴木俊光

    日本エネルギー学会関西支部第55回研究発表会要旨集  2010 

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  • V2O5/SiO2を用いるプロパンの酸化的脱水素反応に及ぼすバナジウム前駆体の影響

    福留健太, 池永直樹, 鈴木俊光, 三宅孝典

    第106回触媒討論会A予稿集  2010 

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  • Fe-Cr複合酸化物の格子酸素を用いるCH4からの合成ガス製造

    岡本直也, 池永直樹, 三宅孝典, 鈴木俊光

    日本化学会第90春季年会講演予稿集  2010 

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  • 担持Fe触媒を用いたFischer-Tropsch合成におけるFeカーバイド種の生成

    仁科喬優, 池永直樹, 三宅孝典, 鈴木俊光

    日本化学会第90春季年会講演予稿集  2010 

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  • Production of syngas or hydrogen from CH4 using lattice oxygen of Fe-Cr complex oxide

    Okamoto, N., Nakayama, O., Ikenaga, N., Miyake, T., Suzuki, T.

    EuropaCatIX  2009 

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  • Ru担持CaO-ZrO2 触媒によるアルコール類の選択的酸素酸化反応

    安枝 隆, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第89春季年会  2009 

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  • Fe-Cr 複合酸化物の格子酸素を用いるCH4からの合成ガス・水素製造

    岡本 直也, 池永 直樹, 三宅 孝典

    日本化学会第89春季年会  2009 

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  • 担持Fe触媒を用いたFT合成におけるMnの添加効果

    仁科喬優, 三宅孝典, 池永直樹, 鈴木俊光

    石油学会第58回研究発表会講演要旨  2009 

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  • V2O5の格子酸素を用いるプロパンの酸化的脱水素反応

    福留健太, 池永直樹, 三宅孝典, 鈴木俊光

    第104回触媒討論会A予稿集  2009 

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  • バナジウム触媒を用いるCO2気流下での1-ブテンの酸化的脱水素反応

    崎谷一貴, 池永直樹, 三宅孝典, 鈴木俊光

    日本エネルギー学会関西支部第54回研究発表会要旨集  2009 

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  • Ru/cabon aerogel触媒を用いるH2雰囲気下でのCOの選択酸化反応第

    堀内伸彦, 石野陽介, 三宅孝典, 鈴木俊光, 池永直樹

    第39回石油・石油化学討論会講演要旨  2009 

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  • Oxidative dehydrogenation of propane with lattice oxygen of vanadium oxide

    Fukudome, K., Ikenaga, N., Miyake, T., Suzuki, T.

    EuropaCatIX  2009 

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  • 内外両管壁を触媒反応場とするメタノールの水蒸気改質反応-メタノール燃焼熱の高効率利用法-

    中尾 文彦, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第101回触媒討論会  2008 

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  • 種々のバイオマスチャーのCO2ガス化に及ぼす灰分中の無機物の影響

    池永 直樹, 中嶋 浩志, 鈴木 俊光

    第45回石炭科学会議  2008 

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  • Co触媒を用いたカーボンナノチューブの生成における炭素源の影響

    川嶋 優, 宇田川 匠, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本エネルギー学会関西支部第53回研究発表会  2008 

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  • 酸化ダイヤモンド担持パラジウム触媒を用いるH2とO2 からのH2O2直接合成

    山根 良介, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第38回石油・石油化学討論会  2008 

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  • 酸化ダイヤモンド担持Pd触媒を用いるH2とO2からのH2O2直接合成

    山根 良介, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第88春季年会  2008 

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  • CeO2担持Ru触媒を用いたNH3合成に対する種々の金属塩の添加効果

    横井 優, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第88春季年会  2008 

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  • POx/NiO/ZrO2触媒を用いるエタンの酸化的脱水素反応

    崎谷 一貴, 中村 健一, 池永 直樹, 三宅 孝典, 鈴木 俊光

    石油学会第57回研究発表会  2008 

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  • 種々のバイオマスチャーのCO2 ガス化に及ぼす灰分中の無機物の影響

    池永 直樹, 中嶋 浩志, 鈴木 俊光

    第45回石炭科学会議発表論文集  2008 

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  • エチルベンゼン脱水素反応─CO2の反応促進機構の解明─

    斉藤 一博, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第102回触媒討論会  2008 

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  • Ni/CaO-ZrO2 触媒を用いたグリセリンの水蒸気改質による水素製造

    北村 丞, 末永 卓哉, 平井 寿英, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第38回石油・石油化学討論会  2008 

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  • 酸化ダイヤモンド担持パラジウム触媒を用いるH 2とO2 からのH 2O2 直接合成

    山根 良介, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第38回石油・石油化学討論会講演要旨  2008 

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  • Direct synthesis of H2O2 from H2 and O2 over Pd-loaded powdered diamond catalyst

    R. Yamane, N. Ikenaga, T. Miyake, T. Suzuki

    5th International Conference on Environmental Catalysis  2008 

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    Venue:Belfast (Ireland)  

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  • Co 触媒を用いたカーボンナノチューブの生成における炭素源の影響

    川嶋 優, 宇田川 匠, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本エネルギー学会関西支部第53回研究発表会要旨集  2008 

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  • 担持パラジウム触媒によるヨードベンゼンとオレフィンの一酸化炭素挿入を伴うカップリング反応

    清家 涼, 安枝 隆, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第88春季年会  2008 

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  • Co担持MgO触媒によるカーボンナノチューブの生成機構

    宇田川 匠, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第88春季年会  2008 

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  • 共沈法により調製したNi-Bi-ZrO2触媒を用いるプロパンの酸化的脱水素反応

    福留 建太, 観野 亜紀, 池永 直樹, 三宅 孝典, 鈴木 俊光

    石油学会第57回研究発表会  2008 

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  • Partial oxidation of CH4 to produce pure hydrogen with air

    O. Nakayama, N. Ikenaga, T. Miyake, E. Yagasaki, T. Suzuki

    Europacat VIII  2007 

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    Venue:Turku (Finland)  

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  • 酸化ダイヤモンド担持パラジウム触媒を用いる炭素-炭素結合生成反応-塩基性酸化物の添加効果-

    清家 涼, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第99回触媒討論会  2007 

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  • Ni系複合酸化物上での空気を用いたCH4の部分酸化反応による純水素の製造法

    中山 修美, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第100回触媒討論会  2007 

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  • Ni-Sb/ZrO2触媒を用いるエタンの酸化的脱水素反応

    崎谷 一貴, 中村 健一, 池永 直樹, 三宅 孝典, 鈴木 俊光

    石油学会第56回研究発表会  2007 

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  • Pd-金属酸化物担持酸化ダイヤモンド触媒によるアルコール類の選択的酸化反応

    安枝 隆, 清家 涼, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第37回石油・石油化学討論会  2007 

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  • エチルベンゼン脱水素反応におけるCO2促進効果のパルス反応による検討

    斉藤 一博, 奥田 和美, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第100回触媒討論会  2007 

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  • 酸化ダイヤモンド担持パラジウム触媒による分子状酸素を酸化剤としたアルコール類の選択的酸化反応

    安枝 隆, 清家 涼, 三宅 孝典, 池永 直樹, 鈴木 俊光

    日本化学会第87春季年会  2007 

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  • トリクルベット反応器による酸化ダイヤモンド担持Co-Mn 触媒を用いたFischer-Tropsch 合成

    西澤 淳夫, 北野 哲史, 三宅 孝典, 池永 直樹, 鈴木 俊光

    日本化学会第87春季年会  2007 

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  • 酸化剤に空気を用いるCH4の部分酸化反応による純水素の製造法

    中山 修美, 三宅 孝典, 池永 直樹, 鈴木 俊光

    日本化学会第87春季年会  2007 

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  • Steam reforming of methanol with CuO-ZnO loaded alumina wall tube reactor

    F. Naka-o, N. Ikenaga, T. Miyake, T. Suzuki

    Europacat VIII  2007 

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    Venue:Turku (Finland)  

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  • Carbon nanofiber synthesis over Co-Mn catalyst

    T. Udagawa, Y. Yamada, N. Ikenaga, T. Miyake, T. Suzuki

    Europacat VIII  2007 

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    Venue:Turku (Finland)  

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  • Ir-Co系バイメタリック触媒を用いたメタンの部分酸化による合成ガス生成

    中村 紀章, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本エネルギー学会関西支部第52回研究発表会  2007 

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  • Selective oxidation of alcohols with molecular oxygen over Pd-loaded oxidized diamond catalyst

    T. Yasu-eda, R. Se-ike, N. Ikenaga, T. Miyake, T. Suzuki

    Europacat VIII  2007 

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    Venue:Turku (Finland)  

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  • C-C bond formation over Pd-loaded oxidized diamond catalyst

    R. Se-ike, T. Yasu-eda, N. Ikenaga, T. Miyake, T. Suzuki

    Europacat VIII  2007 

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    Venue:Turku (Finland)  

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  • Oxidative dehydrogenation of propane over Ni-MO/ZrO2

    A. Kanno, K. Nakamura, N. Ikenaga, T. Miyake, T. Suzuki

    TOCAT 5  2006 

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    Venue:Tokyo(Japan)  

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  • Co-Mn/O-Diaを用いたFischer-Tropsch反応

    北野 哲史, 田戸 励, 本庄 孝夫, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第97回触媒討論会  2006 

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  • 鉄族金属を坦持したシリカ上でのカーボンナノファイバーの生成条件

    山田 康純, 細野 勇樹, 村越 暢之, 市岡 宏章, 三宅 孝典, 池永 直樹, 鈴木 俊光

    日本化学会第86春季年会  2006 

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  • 陽極酸化アルミナを担体とした管型反応器によるメタノールの水蒸気改質

    中尾 文彦, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第98回触媒討論会  2006 

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  • Ni担持触媒を用いたグリセリンの水蒸気改質による水素製造

    末永 卓哉, 平井 寿英, 池永 直樹, 三宅 孝典, 鈴木 俊光

    石油学会第55回研究発表会  2006 

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  • Ni/CeO2/γ-Al2O3触媒を用いたエタンの部分酸化による合成ガス生成反応

    岩崎 尚喜, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第86春季年会  2006 

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  • 種々のバイオマスチャーのCO2 ガス化特性

    中嶋 浩志, 池永 直樹, 鈴木 俊光

    日本エネルギー学会関西支部第51回研究発表会  2006 

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  • 酸化ダイヤモンド担持パラジウム触媒を用いる炭素-炭素結合生成反応

    清家 涼, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第36回石油・石油化学討論会  2006 

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  • カーボンナノチューブ生成に対する触媒媒金属形状の影響

    市岡 宏章, 山田 康純, 三宅 孝典, 池永 直樹, 鈴木 俊光

    第96回触媒討論会  2005 

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  • Ammonia synthesis over alkali metal promoted Ru/O-Dia catalyst

    H. Matsumoto, N. Ikenaga, T. Miyake, T. Suzuki

    7th European Congress on Catalysis  2005 

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    Venue:Sofia (Bulgaria)  

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  • CNT formation with 8-10 group metalloaded MgO catalysts

    H. Ichi-oka, N. Higashi, N. Ikenaga, T. Miyake, T. Suzuki

    7th European Congress on Catalysis  2005 

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    Venue:Sofia (Bulgaria)  

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  • Carbon nanofiber formation on iron group metal-loaded SiO2

    Y. Hosono, N. Murakoshi, Y. Yamada, N. Higashi, A. Ichi-oka, N. Ikenaga, T. Suzuki

    16th European Conference on Diamond, Diamond-Like Materials, Carbon Nanotubes, Nitrides&Silicon Carbide  2005 

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    Venue:Toulouse (France)  

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  • Dispersion of supported metal catalyst on oxidized diamond

    T. Kitano, T. Hirai, N. Ikenaga, T. Miyake, T. Suzuki

    7th European Congress on Catalysis  2005 

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    Venue:Sofia (Bulgaria)  

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  • SO2 Desulfurization Behavior of Ca- Based Absorbents Prepared with Oyster Shell and Organic Substances

    N. Ikenaga, H. Nakajima, S. Yamamizu, T. Suzuki

    2005 Int. Conf. on Coal Sci.&Technol.  2005 

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    Venue:Okinawa (Japan)  

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  • H2S Absorption Mechanism of Fe-Based Absorbents

    N. Ikenaga, M. Hamana, T. Suzuki

    2005 Int. Conf. on Coal Sci.&Technol.  2005 

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    Venue:Okinawa (Japan)  

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  • Pd担持酸化ダイヤモンド触媒によるエチレンからの酢酸ビニル気相合成

    植松 良有, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本エネルギー学会関西支部第49回研究発表会  2005 

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  • Oxidative dehydrogenation of ethane over Ni-loaded catalyst

    K. Nakamura, H. Matsumura, N. Ikenaga, T. Miyake, T. Suzuki

    7th European Congress on Catalysis  2005 

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    Venue:Sofia (Bulgaria)  

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  • Partial oxidation of ethylene to synthesis gas over Coloaded catalysts

    N. Iwasaki, N. Ikenaga, T. Miyake, T. Suzuki

    10th Japan-Korea Symposium on Catalysis  2005 

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    Venue:Matsue(Japan)  

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  • 酸化ダイヤモンド担持Ru―アルカリ金属触媒によるアンモニア合成反応

    松本 ひとみ, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第85春季年会  2005 

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  • コバルト触媒を用いたエタンの部分酸化反応による合成ガス生成

    岩崎 尚喜, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第85春季年会  2005 

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  • MgO担時金属触媒を用いたカーボンナノチューブの接触合成

    市岡 宏章, 東 直樹, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本化学会第85春季年会  2005 

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  • NiO/ZrO2触媒を用いたエタンの酸化的脱水素反応

    中村 健一, 観野 亜紀, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第96回触媒討論会  2005 

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  • 酸化ダイヤモンド担持金属触媒の金属分散度の評価

    北野 哲史, 平井 寿英, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第95回触媒討論会  2005 

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  • カキ殻担持石炭チャーを用いた炉内脱硫条件における脱硫活性評価

    中嶋 浩史, 山水 宣仁, 池永 直樹, 鈴木 俊光

    第42回石炭科学会議  2005 

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  • Development of Calcium Ferrite Prepared from Oyster Shell for H2S Absorption

    M. Hamana, N. Ikenaga, T. Suzuki

    21st Pittsburgh Coal Conference  2004 

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    Venue:Osaka(Japan)  

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  • CARBON NANOTUBE FORMATION ON Ni OR Pd-LOADED DIAMOND CATALYSTS

    N. Higashi, N. Ikenaga, T. Miyake, T. Suzuki

    15th European Conference on Diamond, Diamond-Like Materials, Carbon Nanotubes, Nitrides&Silicon Carbide  2004 

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    Venue:Riva Del Garda(Italy)  

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  • Oxidized Diamond as a Novel Support Material for Various Heterogeneous Catalytic Reactions

    T. Suzuki, K. Takeda, T. Honsho, N. Ikenaga

    13th International Congress on Catalysis  2004 

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    Venue:Paris(France)  

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  • 酸化ダイヤモンド担持触媒を用いたFischer-Tropsch合成におけるMnの添加効果

    北野 哲史, 田戸 励, 本庄 孝夫, 池永 直樹, 鈴木 俊光

    第35回石油・石油化学討論会  2004 

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  • Ni/MgO触媒を用いたエタンの酸化的脱水素反応

    中村 健一, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第94回触媒討論会  2004 

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  • Fischer-Tropsch合成におけるCo/酸化ダイヤモンド触媒のコバルト種の影響

    池永 直樹, 本庄 孝夫, 中川 清晴, 三宅 孝典, 鈴木 俊光

    石油学会第53回研究発表会  2004 

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  • カキ殻を利用した高性能H2S吸収剤の開発―CaSO4のH2S吸収速度増加に及ぼす影響―

    濱名 通隆, 池永 直樹, 鈴木 俊光

    第41回石炭科学会議  2004 

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  • グリセリン水蒸気改質反応用触媒の開発

    平井 寿英, 池永 直樹, 三宅 孝典, 鈴木 俊光

    第34回石油・石油化学討論会  2004 

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  • バナジウムアルコキシドより調製した活性炭担持触媒を用いるエチルベンゼンの脱水素反応

    奥田 和美, 武田 和剛, 池永 直樹, 三宅 孝典, 鈴木 俊光

    石油学会第54回研究発表会  2004 

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  • NiおよびPd/酸化ダイヤモンド触媒を用いたカーボンナノチューブの生成

    東 直樹, 池永 直樹, 三宅 孝典, 鈴木 俊光

    日本エネルギー学会関西支部第48回研究発表会  2004 

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Industrial property rights

  • ブテンの脱水素に用いるフェライト系触媒の製造方法

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    Patent/Registration no:特許第6195246号  Date registered:2017  Date issued:2017

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Awards

  • 日本エネルギー学会進歩賞(学術部門)

    2002.2   社団法人 日本エネルギー学会  

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    Country:Japan

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Research Projects

  • Production of Nitrogen Free Hydrogen or Synthesis Gas from Methane Using Lattice Oxygen of Complex Oxide and Air

    Grant number:20560722  2008 - 2010

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (C)

    SUZUKI Toshimitsu, MIYAKE TAkanori, IKENAGA NaーOki

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    Grant amount:\4680000 ( Direct Cost: \3600000 、 Indirect Cost:\1080000 )

    Partial oxidation of methane to give hydrogen or synthesis gas is a superior route in view of an energy saving process. However, pure oxygen is required as an oxidant and this limits the process to a large scale production on account of a costly oxygen plant. The objective of this research is to overcome such drawbacks, and we employed lattice oxygen of metal oxides as soul oxygen sources. Using nickel oxide or iron oxide combined with chromium oxide and magnesium oxide, we could obtain synthesis gas with a high methane conversion and a high selectivity. After the reaction of mixed oxides with methane, oxidation state of nickel or iron decreased to lower valence oxides. Reduced oxides could be oxidized to their original state by oxidation with air. The reaction of methane and oxides and oxidation of reduced oxides with air could successfully be repeated. Thus, we could obtain synthesis gas continuously free from nitrogen.

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  • Development and activity evaluation of new catalyst prepared by using carbon aerogel

    Grant number:18560745  2006 - 2008

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (C)

    IKENAGA Naoki, SUZUKI Toshimitsu, HORIKAWA Toshihide

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    Grant amount:\4030000 ( Direct Cost: \3400000 、 Indirect Cost:\630000 )

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  • Oxidative Dehydrogenation of Ethane and Propane using Ni-Loaded Catalysts

    Grant number:18360382  2006 - 2007

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (B)

    SUZUKI Toshimitsu, IKENAGA Nao ki

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    Grant amount:\16720000 ( Direct Cost: \15400000 、 Indirect Cost:\1320000 )

    Most important basic organic chemicals ethylene and propylene are commercially produced by energy consuming and less selective steam cracking of light hydrocarbons. In order to develop more energy saving and selective processes, catalytic oxidative dehydrogenation was investigated.
    As an active species of the catalyst, NiO was selected, and support material of NiO was exploited. MgO having high surface area was found to be an appropriate support and with 5 wt% loading of NiO on MgO, ethane conversion of 53% and ethylene selectivity of 62% were obtained at the reaction temperature of 600℃.
    Further studies on exploiting the support material of NiO, ZrO_2 was found to reduce the reaction temperature to 450℃. Additives of NiO-ZrO_2 catalyst were examined and SbOx and P_2O_5 were found to promote the catalytic activity and to increase selectivity to ethylene at 550℃ Ethane conversion of 35% and ethylene selectivity of 64% were obtained with the addition of 0.7 wt% SbOx.
    Addition of 0.52 wt% of P to Ni0-Zr02 catalyst, afforded ethane conversion of 33% and ethylene selectivity of 62% at 450℃, and an increase in the ratio of ethane/oxygen increased the ethane conversion to 41% with the selectivity to ethylene of 65%. The results are one of the highest selectivity to ethylene from ethane without dilution of the feed.
    Application of this catalyst system to the oxidative dehydrogenation to propane was not successful. Catalyst preparation was changed to the co-precipitation method using an aqueous solution of Ni(NO_3)_2 and ZrOCl_2 by adding aqueous ammonia. The catalyst exhibited moderate activity in the dehydrogenation of propane to propylene at 400℃.
    Transient response technique was developed to understand dehydrogenation mechanism using ethylbenzene as a substrate.

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  • PREPARATION OF FERRITE WITH BIMODAL PORE STRUCTURE

    Grant number:15560670  2003 - 2005

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (C)

    IKENAGA Naoki, SUZUKI Toshimitsu

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    Grant amount:\3600000 ( Direct Cost: \3600000 )

    We have already reported that ZnFe_2O_4 and CaFe_2O_4 prepared with coal exhibited a high reactivity in the desulfurization process at 500-800℃, and could efficiently remove 4000ppm of H_2S to less than a few ppm. ZnFe_2O_4 could be regenerated after the H_2S absorption by air oxidation. When CaFe_2O_4 absorbent was regenerated after the absorption, Fe_2O_3 and CaSO_4 produced (CaS+2FeS+11/2O_2→CaSO_4+Fe_2O_3+2SO_2). Although CaFe_2O_4 could not reproduced after the regeneration, when the regenerated absorbent was used for the H_2S absorption, H_2S concentrations in the effluent gas (4-6ppm) were smaller than that (15-20ppm) of Fe_2O_3, indicating that CaSO_4 in the regenerated absorbent seems to contribute to high absorption rate of H_2S.
    In order to elucidate a role of CaSO_4,CaSO_4-loaded Fe_2O_3 (Fe_2O_3/CaSO_4) was prepared by impregnation method. The temperature programed reaction (TPR) under argon atmosphere was carried and the decomposition behavior of CaSO_4 was obtained. In Fe_2O_3/CaSO_4, the release of SO_2 was observed from 450 to 500℃. In contrast, for Fe_2O_3,SO_2 was not observed. From these results, in order that metal sulfate have the H_2S absorption capability, it is necessary to be decomposed CaSO_4 into SO_2 and CaO under argon atmosphere until absorption temperature (500℃). CaO and Fe_2O_3 existed in the absorbent contribute in H_2S absorption. When CaO and Fe_2O_3 are simultaneously used, Fe_2O_3 seems to contribute to decrease the high concentration of H_2S to less than 20ppm, and then CaO seems to contribute to decrease 20ppm of H_2S to a few ppm.

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  • 酸化物系ナノ・マイクロチューブの創製とその機能に関する研究

    Grant number:15656206  2003 - 2004

    日本学術振興会  科学研究費助成事業  萌芽研究

    三宅 孝典, 小田 廣和, 池永 直樹

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    Grant amount:\3000000 ( Direct Cost: \3000000 )

    酸化物系ナノ・マイクロチューブを合成する基礎検討を、昨年に引き続きキャピラリーチューブリアクターを用いた無機塩の熱分解で行った。
    昨年度に硝酸鉄をホルムアミド溶媒に溶解して調製した酸化鉄が目的のチューブ状になっているかどうかについて、透過型電子顕微鏡で形態観察を行ったが、チューブを示すトンネルは見えなかった。なお、硝酸鉄を電気炉を用いて熱処理した場合には、キャピラリーチューブでの熱分解に比べ150℃以上の高温でないと同じ結晶構造の酸化鉄が得られないことが明らかとなり、やはりマイクロチューブリアクターの特徴があることを確認できた。
    同じ方法論を用い、光学材料として興味ある性質を有する酸化亜鉛の調製を検討した。硝酸塩あるいはアセチルアセトナートを原料とし、それらの純物質の熱分解温度より低温の200℃での調製を検討した。亜鉛塩の場合、溶媒の選択により、生成物の結晶構造が異なること、また、酸化亜鉛となっていればないはずの重量減少が熱重量分析で認められた。更に赤外分光測定の結果、溶媒に由来する吸収が見られたことから、亜鉛塩がキャピラリーチューブ中で分解していく過程で溶媒和が起こり、これにより亜鉛塩の熱安定性が増し、結果的に十分な熱分解が起こらなかったと考えられた。
    これらの結果を総括すると、マイクロチューブリアクターを用いた塩の熱分解で、現状では目的とした酸化物系のナノ・マイクロチューブは得られていない。目的物を得るためには、チューブを開けるための添加物等の検討が必要と考えられる。マイクロチューブリアクターを用いることで、得られる酸化物の二次粒子の形態を制御できるという新しい知見が得られたので、更に基礎研究を続ける価値があると示唆された。

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  • Development of Diamond-Carbon Nanotube Hybrid Materials

    Grant number:14350429  2002 - 2004

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (B)

    SUZUKI Toshimitsu, IKENAGA Naoki, ANODO Toshihiro

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    Grant amount:\14900000 ( Direct Cost: \14900000 )

    Diamond has unique physical properties and recent progress in CVD diamond process provided semi-conductor diamond thin films. We have first discovered that several metals or metal oxide loaded on powdered diamonds surface exhibited very high catalytic activities in several reactions involving methane and lower hydrocarbons. This research is extent ion of diamond catalyzed reactions of hydrocarbons on metal loaded oxidized diamond to give diamond and carbon nanotube hybrid materials. Diamond is composed of sp3 carbons whereas carbon nanotube is composed of sp2 carbons. If diamond and carbon nanotube hybrid materials could be synthesized, unique physical properties would be expected. From these perspectives, this research was planned and synthesis of diamond-carbon nanotube hybrid material was successfully achieved.
    Several iron group metal loaded diamond powder was hydrogen reduced and reacted with methane and ethane at an elevated temperature of 400 to 800 ℃. Ni and Pd loaded diamond afforded a large amount of carbon nanofibers. On Ni-loaded case the maximum rate of carbon was obtained at 500 ℃ with methane and 600 ℃ with ethane, and from both hydrocarbons no nanofiber formation was observed at 650 ℃. Very small amount of carbon nanofibers were obtained on Co and Fe loaded diamond irrespective of the reaction temperature. On Fe-loaded diamond at 1000 ℃, very small amount of single wall carbon nanotube directly bonded to diamond surface was obtained by TEM observation.
    On the contrary, with Pd-loaded case carbon nanofibers were produced at higher temperature of 500 to 800 ℃, and even at 800 ℃ a large amount of carbon nanofibers were produced both from methane and ethane. In addition, at 800 ℃ with ethane as a carbon source over Pd-loaded diamond catalyst, very thick carbon fibers were produced by the combinations of initially produced thin carbon fibers.
    Metal catalyzed carbon nanofiber growth mechanism by the decomposition of hydrocarbon was clarified and this shed light to the design of the catalyst and growth conditions.

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  • 二酸化炭素を酸化剤に用いるメタン、エタンからの含酸素化合物合成触媒の開発

    Grant number:14655301  2002 - 2003

    日本学術振興会  科学研究費助成事業  萌芽研究

    鈴木 俊光, 池永 直樹

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    Grant amount:\3300000 ( Direct Cost: \3300000 )

    メタンの酸化により直接メタノールやホルムアルデヒドを生成させることは触媒化学の究極の目標であるが、メタンより、生成物の含酸素化合物の方が酸素との反応性は高いため、二酸化炭素への酸化の方が進行しやすく、目的生成物の選択性は低いのがこれまでの結果である。
    本研究では、二酸化炭素が、穏和な酸化剤として、炭化水素の脱水素に効果的な触媒となることを参考にして、以下の反応式によるメタン、エタンの二酸化炭素による酸化反応を用いるアルデヒド合成の可能性について研究した。
    CH_4 + CO_2→HCHO+CO+H_2O
    種々の触媒について検討した結果V_2O_5をシリカに担持したときに、ホルムアルデヒドを生成することを見いだした。反応は高温でのみ進行し、550℃以上の温度が必要であった。触媒の担体として様々な酸化物について検討したところ、我々が新規触媒担体として系統的な研究を展開しているダイヤモンド粉末を水素化し、空気酸化したものがシリカについで高い活性を示した。
    この反応では生成物のアルデヒドが触媒表面からの脱離がキー反応となり、接触時間を大きくすると、ホルムアルデヒドの収率および選択率が向上した。副反応としては生成物の分解によるCOが生成した。
    CO_2の働きについて、詳細に検討した。CO_2はメタンの酸化によってV_2O_5の格子酸素が奪われ、バナジウムが低原子価に還元されるのを、再酸化し高原子価を保つ働きをすることを、IR、UV-Vis、XEANSなどの分光学的手法ならびに、触媒のCO_2による酸化の可能性を昇温還元によって明らかにした。

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  • Development of High Performance Desulfurization Sorbent in the Coal Combustion and Gasification

    Grant number:11218212  1999 - 2002

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research on Priority Areas

    SUZUKI Toshimitsu, ISHIMORI Michihiro, IKENAGA Na-oki, ODA Hirokazu

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    Grant amount:\38400000 ( Direct Cost: \38400000 )

    In order to mitigate carbon dioxide emission in the utilization of coal, increase in the thermal efficiency is indispensable. For this purpose, Integrated Coal Gasification Combined Cycle (IGCC) has been proposed. Further increase in the thermal efficiency of IGCC, high temperature gas cleaning is indispensable. This project is aimed at development of efficient absorbent of H_2S in the coal gasification gas from an entrained bed coal gasifier. Ferrites were reported to be a good absorbent of H_2S at an elevated temperature. However, a ferrite produced by dry method exhibited very low surface area and only the surface of the ferrite was utilized as an absorbent. To overcome this, we have developed a new process preparing ferrite at a low temperature in a wet method using an activated carbon as ferrite carrier. The zinc ferrite produced in the presence of an activated carbon exhibited a high surface area. H_2S absorption behavior of this sorbent exhibited excellent performance, where almost all of Fe and Zn in the ferrite was sulfided at 400 to 600℃. Moreover, effluent gas after absorption by using a fixed bed flow reactor, contained very low H_2S concentration of less than 1 ppm. Such high performance has never been observed with zinc ferrite prepared other methods. Ferrites prepared in the presence of low sulfur coal exhibited similar behavior as that prepared in the presence of activated carbon. Cost of the absorbent with coal would be reduced considerably as compared to the ferrite prepared with activated carbon. Calcium ferrite prepared in the presence of coal also exhibited excellent performance for the absorption of H_2S. Detailed studies on the performance of ferrites were done in order to understand performance of the ferrites. Characteristic feature of the ferrite was elucidated.
    In addition to H_2S absorbent, SO_2 absorbent in coal combustion was developed with CaO and oyster shell. Oyster shell treated with Yallourn coal at 850℃. Improved SO_2 absorption capacity compared to raw oyster shell was achieved.

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  • Development of catalyst for the synthesis of styrene from ethane and benzene

    Grant number:11650811  1999 - 2000

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (C)

    SUZUKI Toshimitsu, IKENAGA Naoki

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    Grant amount:\3700000 ( Direct Cost: \3700000 )

    A large quantity of styrene monomer was produced in the world from ethylene and benzene to give ethylbenzene followed by dehydrogenation. 3 step processes were required in the current technology. This project was planned to develop a simple and energy saving chemical process. For this, ethane was used for the alkylation of benzene using various acid catalysts such as zeolite. However, yield of ethylbenzene was very small. Considering that formation of ethyl cation from ethane is difficult, loading of several metal species which are capable of dehydrogenation of alkane was examined.
    Alkylation of benzene with ethane was carried out using various zeolite catalyst at temperature ranges of 400 to 550℃. Loading of platinum onto zeolite enhanced yield of ethylbenzene greatly. Among zeolite tested, H-ZSM5, H-AlMCM41, and H-MCM22 showed catalytic activities. However, mordenite did not give ethylbenzene. Moderate acid strength distribution is the key factor of zeolite catalyst. Optimum catalyst and conditions for this reaction is as follows :
    Platinum-loaded H-ZSM5 catalyst containing 6.8 wt % Pt, at the reaction temperature of 500℃, afforded ethylbenzene and styrene formation rates of 14.2 and 0.8 mmol h^<-1>・g^<-1> of catalyst, respectively (benzene-based yields 7.3 and 0.4 %). In the alkylation of benzene with ethane over platinum-loaded H-ZSM5, ethene would be initially formed from ethane over the metallic platinum. Then the alkylation would proceed over the acid sites of H-ZSM5.
    Dehydrogenation of ethylbenzene was investigated, and found that magnesium oxide-loaded vanadium oxide exhibited very high activity in the presence of carbon dioxide. Carbon dioxide promoted redox cycle of vanadium oxide during dehydrogenation reaction. Where lattice oxygen of vanadium oxide was gradually lost during dehydrogenation, then carbon dioxide reoxidized low valent vanadium oxide to higher valency state.

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  • Development of new dehydrogenation catalyst using powdered or thin film diamond as support

    Grant number:10555283  1998 - 2000

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (B)

    SUZUKI Toshimitsu, YASU E, IIKENAGA Naoki

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    Grant amount:\12000000 ( Direct Cost: \12000000 )

    Activated carbon composed of sp2 carbon atoms were often used as support material for catalytic reactions. However, up to now diamond composed of sp3 carbon atoms have never been used as support material for catalytic reactions. This work focused on the catalyiic activities of various metal or metal oxides loaded on oxidized diamond catalyst for several reactions, and have first elucidated in the world that oxidized powdered diamond exhibited excellent behavior
    1. Several metal oxides loaded oxidized diamond catalyzed dehydrogenation of ethane was carried out, and found that chromium oxide loaded oxidized diamond exhibited high activity in the dehydrogenation of ethane to ethene. In this reaction, when carbon dioxide was used as a diluent for ethane, at 650 ℃ 23 % ethene yield was obtained. This value is three times higher than that observed in the run under Ar atmosphere
    2. Partial oxidation of methane was carried out over nickel loaded oxidized diamond catalyst. At 650 ℃ synthesis gas was obtained in a high yield. Increasing a reaction temperature to 700 ℃, carbon deposition over catalyst was greatly decreased, indicating that oxidized diamond can be used even in oxidizing conditions. Cobalt loaded oxidized diamond exhibited similar catalytic activity as that of nickel loaded catalyst. Carbon deposition did not occur even lower
    temperature of 60Q ℃
    3. Methanol decomposition over nickel loaded oxidized diamond catalyst was carried out. Catalyiic activity was observed at 250 ℃ and increased greatly at 300 ℃. However, at a higher temperature methane formation increased to give lower yield of hydrogen. Addition of water to methanol decreased methane formation to give CO to H_2 ratio of 1. Detailed studies on these reactions by spectroscopic analyses of the catalysts and non steady state reactions to elucidate mechanisms of the reaction path ways were carried out. High performance of oxidized diamond support seemed to be weak but significant interaction of loaded metal or metal oxide to diamond surface

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  • 鉄担持炭素質を触媒とする石炭液化反応

    Grant number:09750860  1997 - 1998

    日本学術振興会  科学研究費助成事業  奨励研究(A)

    池永 直樹

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    Grant amount:\1900000 ( Direct Cost: \1900000 )

    本研究では、触媒前駆体の微結晶化を目的とし、鉄系触媒の中では比較的高い活性を持つオキシ水酸化鉄を新しい方法で炭素質に担持し、石炭液化反応を行った。また、反応後の触媒の再利用を検討した。
    担持オキシ水酸化鉄触媒は、数種の活性炭をFeSO_4、NaOHおよびNa_2HPO_1のメタノール+水混合溶液に浸し、空気を吹き込みながら40℃で24時間攪拌し、蒸留水で洗浄した後空気中100℃で乾燥して調製した。このようにして調製した前駆体をXRDおよびXPS分析したところ、微結晶あるいは非晶質なオキシ水酸化鉄が生成していることが確認された。
    活性炭(表面積:950m^2/g)を用いて調製した前駆体は高い転化率(91.1%)およびオイル収率(43.9%)を与え、液化反応に対して高い活性が知られている鉄ペンタカルボニルよりもわずかに高い活性を示した。このとき生成した活性種であるピロタイトの結晶子径をScherrer式より求めたところ18nmとなり、活性種の結晶子径が小さいほど高い転化率およびオイル収率を与えた。従来より指摘されているように、高活性を得るためには触媒結晶の成長を抑制することが重要であると考えられる。また、オイル収率より転化率の方が結晶子径により大きく依存していることから、ある程度低分子化されたアスファルテンやプレアスファルテンのような生成物からオイルを生成するためにも結晶子径が小さいことは重要であるが、巨大分子である石炭の分解ラジカルの水素化には触媒の微結晶化がより重要であると考えられる。
    触媒の再利用を目的として、活性の高かった活性炭担持オキシ水酸化鉄触媒を用いた反応の残渣を触媒とし、過剰の硫黄を添加して反応を行った。触媒を再使用しても、転化率およびオイル収率はほとんど低下しなかった。そのとき、活性種であるピロタイトの結晶子径は23nmとなり、ほとんど成長していなかった。

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  • Development of New Catalyst for the Dehydrogenation of iso-Butane to iso-Butene

    Grant number:09650864  1997 - 1998

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (C)

    SUZUKI Toshimitsu, IKENAGA Na-oki

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    Grant amount:\3300000 ( Direct Cost: \3300000 )

    An additive for gasoline, methyl t-butyl ether(MTB) is known to improve emission from exhaust gas from motor vehicles. However, the amount of iso-butene a principal feed for MTB production is limited. This research is aimed to exploit new catalysts for the dehydrogenation of iso-butane to iso-butene.
    Iron-loaded activated carbon was proposed as an active catalyst for the dehydrogenation of isobutane. In addition, the activity of the iron-loaded activated carbon catalyst was promoted in the co-feeding of iso-butanme with carbon dioxide. The enhanced activity of carbon dioxide was attributed to the oxidation of reduced iron species to the higher oxidation state by carbon dioxide.
    Chromia and vanadium oxide loaded activated carbon catalyst exhibited similar catalytic activity in the dehydrogenation of iso-butane. Promoting effect of carbon dioxide was significant on the vanadium oxide loaded activated catalyst. However, catalytic activities of vanadium oxide loaded SiO_2 or Al_2O_3 catalysts decreased in the presence of carbon dioxide.
    Catalytic activity of vanadium oxide loaded activated carbon catalyst was promoted with co-loading a small amount of strontium, barium, and calcium carbonates. The amounts of alkaline-earth metal was optimum when it was co-loaded with 10 mol% of vanadium oxide. Further increase in the loading level decreased catalytic activity.

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  • メタンの部分酸化による合成ガス製造のための高活性触媒の開発

    Grant number:09218255  1997

    日本学術振興会  科学研究費助成事業  重点領域研究

    鈴木 俊光, 池永 直樹

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    Grant amount:\1800000 ( Direct Cost: \1800000 )

    メタンの部分酸化による合成ガスの製造は、水蒸気改質反応より、省エネルギー、高効率プロセスとなる。本研究では、高活性・高選択性メタン部分酸化触媒を開発し、今後大気汚染防止のためガソリンへの添加剤として需要の著しく増すメタノールや、FT法炭化水素合成の原料供給に道を開くために、新触媒の開発を行いイリジウム金属の担体に酸化チタンを用いると活性選択性とも高いことを見いだした。Niと微量のIrを複合化するとNi単独では活性を示さない低温でメタンから合成ガスが得られることを見いだした。これらの触媒では用いる担体によって触媒の活性が著しく影響されることが明らかになり、メタンの部分酸化の触媒反応機構が金属や担体によって異なることが推察された。
    平成7年度の補助金で購入した4重極マススペクトロメーターを用いて、パルス反応を検討し、触媒層の温度変化(完全燃焼が起これば著しい発熱とそれに続く改質による吸熱が観測される)を追跡したところ、金属・担体によりメタンと酸素の混合ガスをアルゴンをキャリアーガスとして通じた中へパルス状に導入すると、触媒層の前縁で激しい発熱が起こるケース(Ir/TiO_2やPt/TiO_2)と吸熱が起こるRh/TiO_2が認められた。いずれの場合にも生成物は、水素、CO、CO_2であり、発熱が起こる触媒ではメタンの完全燃焼がまず起こり、ついでメタンの水蒸気および二酸化炭素による改質反応が進行することが明らかとなり、吸熱が起こるケースではまず触媒金属上でメタンの水素への解離が起こり、ついで酸素と触媒上の炭素質との反応によりCOが生成するものと推察された。

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  • メタンの酸化カップリング反応による高選択的エチレン合成触媒の開発

    Grant number:08650931  1996

    日本学術振興会  科学研究費助成事業  基盤研究(C)

    鈴木 俊光, 池永 直樹

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    Grant amount:\1900000 ( Direct Cost: \1900000 )

    メタンの酸化カップリング反応について、より活性の高いエチレン選択性の高い触媒の探索を行った。酸化ランタンにアルカリ金属のハロゲン化物を添加した触媒を用いると、メタンの2量化生成物中のエチレンとエタンの比が大きくなることを見いだし、触媒の形態をX-線回折により検討したところ、LaOBrのような酸化臭化物に変化していた。LaBr_3とLa_2O_3の反応により酸化臭化物を用いてメタンの酸化カップリングを行ったところ、高いエチレン選択性が得られたことより、メタンの2量化に続く脱水素過程に酸化臭化物が活性を示すことが分かった。しかし、この触媒を用いて長時間反応を行うと、次第にエチレンの選択性が低下し、酸化ランタンのみを用いたときと同じ選択性になった。これは、臭素が次第に系外へ揮散していくためと反応後の触媒が酸化ランタンに再び変化していることから推察された。
    酸化ランタン触媒を臭化ナトリウムの水溶液で処理したときにメタンの転化率が増大するのが認められた。このときLa_2O_3はLaOH_3に変化していたので、LaOH_3を触媒に用いて反応を行ったところ、メタンの転化率が増大し、これは酸化ランタンの表面積が5倍程度増加したためと考えられた。反応中に水酸化ランタンは反応中に酸化ランタンに再び戻るので、反応中に系内に水蒸気を導入したところ、700℃の反応では転化率が増大し、エタン、エチレン収率は増加したが、C2の選択性は変わらなかった。

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  • メタンの部分酸化による合成ガス製造のための高活性触媒の開発

    Grant number:08232275  1996

    日本学術振興会  科学研究費助成事業  重点領域研究

    鈴木 俊光, 池永 直樹

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    Grant amount:\2200000 ( Direct Cost: \2200000 )

    メタンの部分酸化反応にイリジウムを酸化チタンに担持した触媒を用いることにより高いメタン転化率と合成ガスへの選択性を得ることができることを明らかにした。このときイリジウムの担持率が比較的たかいときに高い活性が発揮されたので、第一周期の遷移金属とイリジウムを複合化し低いイリジウム担持率で活性を発現させる可能性を検討した。ニッケルをTiO_2に担持した触媒を用いると,600℃ではほとんど活性を示さず、水素還元した時にメタンの部分酸化に活性を示した。この触媒に0.5wt%のイリジウムを添加すると水素還元を行わなくても活性を示し、このときメタンの転化率はそれぞれの金属を単独で用いるた時より高くなり、相乗効果が認められた。担体としては、イリジウム単独触媒の時最大の活性、選択性を示したTiO_2よりLa_2O_3を用いたときの方が活性、選択性が高くなった。
    この触媒はNi単独の触媒と同様に炭素析出が起こり、SEM観察によれば繊維状炭素が生成していた。実使用条件を考慮しSV=30,000と高流速で反応を行っているが、さらに流速をSV=120,000まで上げてもメタンの転化率は低下せずに反応が進行した。本触媒の極めて高い活性があきらかになった。このとき、炭素析出量はメタンの反応量に対して相対的に低下した。
    Ni-Ir複合触媒はIrの触媒作用によってメタンからの合成ガス生成反応が起こり、生成したCO,H_2によってニッケルの還元が起り、相乗作用が発揮されたものと考えられた。

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  • High Performance Thin-Layr Ruthenium Catalyst for Next Generation Coal Liquefaction

    Grant number:07555556  1995 - 1996

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for Scientific Research (A)

    SUZUKI Toshimitsu, KANEKO Takao, IKENAGA Naoki

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    Grant amount:\2900000 ( Direct Cost: \2900000 )

    In order to reduce the cost of coal liquefaction process currently under developing, improvement of cost reduction in variety of fundamental technologies involved in the complex coal liquefaction process. We have previously proposed that ruthenium based dispersed catalyst exhibited 20 to 50 times as active as those catalysts used in the current process. However, ruthenium is a precious metal and consequently very expensive. To overcome this undesirable problem, reduction of the amount of catalyst, long term service, and recycle use are the key requirement of rethenium catalyst development.
    We have developed ruthenium loaded-thin layred alumina by electrode oxidation of aluminum plate. Liquefaction of Indonesian lignite was carried out with the catalyst, and shape and loading level of ruthenium on thin layred alumina were examined. The best catalyst achieved conversion of 82% at 420 oC,under hydrogen partial pressure of 5 MPa (cold), affording light oil fraction of 50%. Since the evaluation was conducted in a batch autoclave, and the catalyst is expected to use in a flow reactor system, the results obtained could not describe flow reaction. This result exhibits possibility of the usage of such thin layred rethenium catalyst, in flow system.
    Use of alumina wire was examined but the strength of alumina wire is not sufficient for the liquefaction reaction.
    For a large scale reactions, further improvement in the strength of alumina thin layr is required.

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  • メタンの部分酸化による合成ガス製造のための高活性触媒の開発

    Grant number:07242268  1995

    日本学術振興会  科学研究費助成事業  重点領域研究

    鈴木 俊光, 池永 直樹

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    Grant amount:\2200000 ( Direct Cost: \2200000 )

    メタンから合成ガスや水素をより高効率で製造する目的で,新規なメタンの部分酸化に高活性,高選択性触媒の開発を行った。
    白金族金属とイオン交換したゼオライトを用いて種々の反応条件(温度500-650℃,メタン/O_2=1-0.2,SV=3,000-30,0000)で反応を行ったところ,イリジウムに高い触媒活性を見いだした。イオン交換ゼオライトとの比較対照のために種々の担体に担持した白金族触媒の本反応に対する活性・選択性を検討し,酸化チタンが優れた担体であることを見いだし,従来知られているロジウム触媒をしのぐ活性とCO,H_2への高い選択性を示すことを見いだした。イリジウム-酸化チタン触媒は400-500℃程度の低温では酸化活性を全く示さず,550℃以上の高温で活性を示した。しかし,600℃で活性を示すようになった触媒を不活性ガス雰囲気下で400℃まで冷却し,再びメタンの部分酸化を行ったところ,400℃でも完全酸化が起こった。
    イリジウム-酸化チタン触媒を用いて,メタンと二酸化炭素の反応を行ったところ,600℃でCO,H_2が生成したことから,メタンの部分酸化のみならず,メタンのCO_2改質反応に活性を示すことが明らかになった。
    酸化チタン上に担持したイリジウムは担持後焼成したときに酸化物になり,これは活性を示さず,反応中に還元されて,メタンの完全酸化が起こり,それに引き続くCO,H_2への改質反応が進行することが明らかとなった。

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  • OXIDATIVE DEHYDROGENATION OF HYDROCARBONS USING CARBON DIOXIDE AS AN OXIDANT

    Grant number:06453104  1994 - 1995

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for General Scientific Research (B)

    SUZUKI Toshimitsu, IKENAGA Naoki

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    Grant amount:\6600000 ( Direct Cost: \6600000 )

    An attempt to use carbon dioxide as a diluent and oxidant in the dehydrogenation of ethylbenzene to stirene was carried out over an activated carbon supported iron catalysts (Fe 17 wt %) at 773-973 K,CO2/ ethylbenzene=50-70mol/mol and W/F=30-120 g h/mol. An addition of 20-30 mol % lithium nitrate to iron resulted in a significant increase in the catalytic activity. The highest yield stirene (40-45 %) with more than 90 % selectivity was obtained at a ratio of lithium to iron of 0.1-0.2 (mol/mol). In addition to stirene, carbon monoxide and water were formed as products. This indicated that the reaction proceeds via an oxidative dehydrogenaiton mechanism. Added lithium nitrate was converted into lithium ferrite during treatment of an iron -lithium co-loaded activated carbon catalyst under carbon dioxide at 973 K.
    The same catalyst was employed in the dehydrogenation of isobutane to isobutene. At 823 K and W/F= 8 g h/mol, conversion of isobutane was 24 % in the 80 % selectivity to isobutene. With increasing the W/F to 14, conversion of isobutane increased to 30 % with an increase in the selectivity to 85 %. Again deactivation of the catalyst during the reaction occurred. Slight recovery of the catalytic activity was achieved by regeneration of the catalyst with carbon dioxide flow without feeding isobutane. Additives such as lithium nitrate did neither improve catalytic activity and activity decay.
    In both reactions iron and iron oxide redox cycle was a key catalytic cycle.
    Catalytic activity of chromia loaded activated carbon was comparable to the iron loaded activated carbon in the dehydrogenation of ethylbenzene to stirene. However, in this case, no redox cycle of the catalyst was observed.

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  • Developing Advanced Coal Utilization Processes to Minimize Environmental Impact

    Grant number:04044086  1992 - 1994

    Japan Society for the Promotion of Science  Grants-in-Aid for Scientific Research  Grant-in-Aid for international Scientific Research

    HASHIMOTO Kenji, MUKAI Shin, IKENAGA Naoki, HAYASHI Junichi, ASAMI Kenji, FUNAZUKURI Toshitaka, NINOMIYA Yoshihiko, SILVESTON P.l., WATKINSON P.a., PRICE J.t., MACPHEE J.a., FURIMSKY E., CHAMBERS A., KOVACIK G., TOLLEFSON E.l., CHORNET E., SCOTT D.s., MAE Kazuhiro, MASUDA Takao, UEMURA Yoshimitsu, KORAI Yozo, SASAOKA Eiji, OHTSUKA Yasuo, OGUMI Zenpachi, ISHIDA Masaru, MIURA Kouichi, TOMITA Akira, HAYASHI Jun-ichiro, ADSCHIRI Tadahumi, DE LASA H., NG Flora T.t.

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    Grant amount:\20600000 ( Direct Cost: \20600000 )

    This joint research program was undertaken to build intimate and friendly relationship between Japan and Canada as well as to develop advanced coal utilization processes which minimize the emission of environmentally malign substances. The types of cooperation consisted of the exchange of researchers to perform researches, mutual visits to research institutes in both countries, presentation of research activities at review meetings, and the publication of the results in scientific journals.
    In 1992 nine junior researchers were sent to Canadian universities and governmental research institutes for 2 to 3 months in summer season to perform joint researches with Canadian hosts. A review meeting was held on July 31 at the University of British Columbia. The report for this year was prepared in Japanese.
    In 1993 three Canadian investigators were invited to Japan. Six Japanese researchers also visited Canada for two months in summer time to perform joint researches with their hosts. On Sep.10 all the members met together at CANMET,where the review meeting was held. The report for this year was also prepared in Japanese.
    In 1994 two junior researchers were sent to the University of Waterloo and CANMET in summer to perform joint researches. In October four professors, K.Hashimoto (Kyoto University), M.Ishida (Tokyo Institute of Technology), Z.Ogumi (Kyoto University), and K.Miura (Kyoto University) visited Canada and the United States to discuss the prospect of the joint research and to investigate research activities in coal chemistry and coal conversion in the two countries. A final report was prepared in English, and was distributed to the researchers in both countries.

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  • 新規接触部分酸化反応による天然ガスの化学原料への転換プロセスの開発

    Grant number:04650745  1992

    日本学術振興会  科学研究費助成事業  一般研究(C)

    鈴木 俊光, 池永 直樹

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    Grant amount:\1900000 ( Direct Cost: \1900000 )

    メタンとエタンの酸化的交差2量化について希土類酸化物を触媒成分として用い,固定床流通反応系により検討した。
    反応は反応性の低いメタンを過剰に用いて,メタン/エタン/酸素=45:7.5:4.5の割合の混合ガスをヘリウムで希釈して800-1000Kの温度範囲で行なった。用いた14種類の希土類酸化物のなかでは,La_2O_3,Sm_23_3,Eu_2O_3等が酸化的交差2量かに活性を示した。 Eu_2O_3が最大で4.5%の収率でプロパンおよびプロペンを生成した。次いでSm_2O_3,La_2O_3の順に活性は低下した。副反応としてはエタンの脱水素によるエチレンの生成とエタンの完全酸化によるCO,CO_2の生成であった。エタンの脱水素は酸化的2量化の活性の高いSm,Eu触媒で著しく起こり,完全酸化は希土類全てで起こり,希土類間で差異は認められなかった。
    反応の諸条件を詳細に検討した。反応温度について検討したところSm,Euの酸化物では,900K付近で交差2量化によるプロパンおよびプロペンの生成量は最大となったが,La_2O_3触媒ではより高温で高い収率が得られた。トルエンとメタンの交差2量化において,触媒効果を向上させたアルカリ金属の臭化物を添加したが,促進効果はトルエンとメタンの反応の場合のように顕著な効果は認められなかった。メタンとエタンの供給比をさらに高く18:1として反応を行なうと,プロパンおよびプロペンの収率は7。7%までに向上した。
    メタン,エタンの光化学的酸化についても検討し,MoO_3-SiO_2触媒系を用いて,触媒層を420-470Kに加熱すると,高選択的にホルムアルデヒドが生成することを見いだした。またこのとき,触媒層に効果的に光を照射するため触媒層を反応ガスにより流動化させることが,光の利用効率を高め,生成物の収率を向上させることを明かにした。

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  • 新規高分散石炭液化触媒の開発

    Grant number:03203254  1991

    日本学術振興会  科学研究費助成事業  重点領域研究

    鈴木 俊光, 池永 直樹

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    Grant amount:\2400000 ( Direct Cost: \2400000 )

    有機金属錯体を石炭直接液化反応の触媒前駆物質に用いることにより従来の石炭液化に用いられる触媒より高い活性を発揮できることを明らかにしてきた。特にルテニウム化合物を用いることにより著しく隠和な条件で石炭液化が行なわれることを明かにした。豪洲褐炭については375℃,3MPaで石炭の転化率90%以上を達成することに成功した。
    さらに本年度は水素供与性溶剤の存在下に高性能な高分散触媒のを用いより隠和な条件で液化が行なえるか否かの検討を褐炭から瀝青炭まで4種の石炭化度のことなる石炭を用いて行なった。水素供与性溶剤としてテトラリンを用いて反応を行ったところ,褐炭ではあまり大きな変化が見られなかったが,瀝青炭では軽質分の収量が増加することがわかった。このとき褐炭では水素は触媒が存在するときはガス中の水素が主に石炭へ移行するが,瀝青炭では水素供与性溶剤からの水素の移行が大きな比重を占めることが示された。このことから,瀝青炭の液化においては良好な水素供与性溶剤の調製が極めて重要になることを明かにした。用いた触媒のうちではFeは多量に用いると高い活性を示し,Mo,Ruなどは少量で良好な活性を示した。モデル物質を用いた化学量論的な研究を行ない,炭化水素ラジカルへは水素供与性溶剤からの水素移行が主として起こり,含酸素ラジカルへは触媒上で活性化された水素からラジカルへの水素移行が起こることが推察された。Ru触媒は特に気相の水素の活性化に高い触媒作用をすることを明かにした。
    水素供与性溶剤を調製するために必要な触媒に関する試み,石油精製用のCoーMo/Al_2O_3およびNiーMo_2O_3触媒より芳香環の水素化に対するより選択的な触媒の開発が必要なことを見いだした。

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Devising educational methods

  • オフィスアワーは当然設けているが、個人的に授業内容に関して質問されても、その学生にしか回答できないので、できるだけ授業中(授業の途中でも)に質問するように指導している。この指導が行き届いてきたのか、今年の春学期の授業では自ら手を上げ、質問をしてくれる学生が多くなってきた。  授業評価アンケートの実施後に複数回の授業が残っており、その授業は授業評価アンケートで指摘された事項を改善して行った。

Teaching materials

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Teaching method presentations

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Special notes on other educational activities

  • Kan-DaiネックレスセミナーおよびKan-Dai1セミナーの講師を務めた。