研究者詳細 - 菊地　英一

写真a

キクチ　エイイチ

菊地　英一

所属

理工学術院

職名

名誉教授

学位

博士(工学) ( 早稲田大学 )

ホームページ

http://www.appchem.waseda.ac.jp/fm-jp/kikuch-j.htm

経歴

1980年

-

　

- 早稲田大学教授
1980年

-

　

- Professor, Waseda University
1975年

-

1980年

早稲田大学助教授
1975年

-

1980年

Associate Professor, Waseda University
1969年

-

1975年

早稲田大学助手
1969年

-

1975年

Research Assistant, Waseda University
1972年

-

1973年

研究員(カナダアルバータ大学)
1972年

-

1973年

Postdoctoral fellow, University of Alberta

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学歴

　

-

1969年

早稲田大学理工学研究科応用化学
　

-

1969年

早稲田大学
　

-

1964年

早稲田大学理工学術院応用化学科
　

-

1964年

Waseda Univrsity Faculty of Science and Engineering Department of Applied Chemistry

委員歴

2006年

-

　

石油学会会長
2002年

-

2003年

解媒学会会長
2000年

-

2001年

ゼオライト学会会長
1999年

　

　

北海道大学大学院地球環境科学研究科外部評価委員会評価委員 1999 － 1999
1997年

-

1998年

日本化学会理事
1985年

-

1996年

日本エネルギー学会(旧称燃料協会) 理事

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所属学協会

　

　

　

日本表面科学会
　

　

　

American Chemical Society(アメリカ化学会)
　

　

　

ゼオライト学会
　

　

　

化学工学会
　

　

　

日本エネルギー学会(旧称燃料協会)
　

　

　

解媒学会
　

　

　

石油学会
　

　

　

日本化学会

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研究キーワード

有機工業化学
反応・分離工学
触媒・化学プロセス
Catalysis and chemical processes

受賞

石油学会賞

1999年
ICＣ Distinguished Lectureship Award

1998年
触媒学会賞

1996年
触媒調製化学賞

1993年
燃料協会進歩賞

1981年
石油学会論文賞

1978年

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書籍等出版物

脱硝触媒－自動車「二元機能触媒」

触媒活用大事典 2004年
ゼオライトを利用した機能複合化による触媒設計

環境触媒ハンドブック（第5章3節）／エヌ・ティー・エス 2001年
石油化学プロセス（石油学会編）

2001年
Modification of Mordenite Catalyst for Selective Synthesis of 2,6-Diisopropylnaphthalene by Alkylation

ACS Symposium Series／American Chemical Society 2000年
Modification of Mordenite Catalyst for Selective Synthesis of 2,6-Diisopropylnaphthalene by Alkylation

ACS Symposium Series／American Chemical Society 2000年
触媒機能の複合化による触媒設計

季刊化学総説／日本化学会 1999年
環境触媒の今後の展望「環境触媒実際と展望」

共立出版 1997年
環境触媒の今後の展望

環境触媒ー実際と展望／共立出版 1997年
新しい触媒化学

三共出版 1988年

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Works(作品等)

日本・サウジアラビア国際研究交流事業「高機能触媒技術研究」

1991年

-

1994年
Japan-Saudi Arabia International Exchange Program of Research on High Performance Catalysts

1991年

-

1994年
エネルギー重点領域研究(多様なエネルギーの利用)

1987年

-

1989年
エネルギー特別研究

1981年

-

1986年
米国におけるCI化学研究開発状況に関する調査

1980年

-

共同研究・競争的資金等の研究課題

メンブレンリアクター
無機分離膜
環境触媒化学
エネルギー変換化学
不均一系触媒化学
一酸化窒素の選択還元触媒
水素透過型メンブレン触媒リアクター
選択的水素透過膜
membrane reactors
Inorganic membranes
environmental catalysis
chemistry of energy transformation
Heterogeneous catalysis
Selective catalysts for reduction of nitric oxide
Hydrogen-permselective catalytic membrane reactor
Hydrogen-permselective membrane

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Misc

エタノール水蒸気改質反応用CoおよびNi触媒担体へのペロブスカイト型酸化物の適用

浦崎浩平, 石川清宏, 関根泰, 菊地英一, 松方正彦

触媒 48 ( 2 ) 65 - 67 2006年

CiNii
Hydrogen production via steam-iron reaction using iron oxide modified with very small amounts of palladium and zirconia

K Urasaki, N Tanimoto, T Hayashi, Y Sekine, E Kikuchi, M Matsukata

APPLIED CATALYSIS A-GENERAL 288 ( 1-2 ) 143 - 148 2005年07月

　概要を見る

We investigated hydrogen production by the steam-iron reaction using iron oxide modified with very small amounts of palladium and/or zirconia at a temperature of 723 K and under atmospheric pressure. Reduction of iron oxide with hydrogen and oxidation of partially reduced iron oxide with steam (Fe3O4 + 4H(2) <-> 3Fe + 4H(2)O) were repeated in the range of reduction degree of 30-50 mol%. Changes in the weight of the samples were monitored using a tapered element oscillating microbalance (TEOM) to control the degree of reduction. Unmodified iron oxide caused significant deactivation due to sintering with increasing number of redox cycles. The addition of a very small amount (0.23 mol%) of palladium or zirconia onto the surface of the iron oxide enhanced the reduction and/or oxidation of the partially reduced iron oxide, which suppressed sintering. Palladium accelerated both the reduction and oxidation rates of partially reduced iron oxide, while zirconia increased only the oxidation rate. Addition of both palladium and zirconia together to the iron oxide resulted in marked enhancement of both reduction and oxidation. (c) 2005 Elsevier B.V. All rights reserved.

DOI CiNii
Hydrogen production via steam-iron reaction using iron oxide modified with very small amounts of palladium and zirconia

K Urasaki, N Tanimoto, T Hayashi, Y Sekine, E Kikuchi, M Matsukata

APPLIED CATALYSIS A-GENERAL 288 ( 1-2 ) 143 - 148 2005年07月

　概要を見る

We investigated hydrogen production by the steam-iron reaction using iron oxide modified with very small amounts of palladium and/or zirconia at a temperature of 723 K and under atmospheric pressure. Reduction of iron oxide with hydrogen and oxidation of partially reduced iron oxide with steam (Fe3O4 + 4H(2) <-> 3Fe + 4H(2)O) were repeated in the range of reduction degree of 30-50 mol%. Changes in the weight of the samples were monitored using a tapered element oscillating microbalance (TEOM) to control the degree of reduction. Unmodified iron oxide caused significant deactivation due to sintering with increasing number of redox cycles. The addition of a very small amount (0.23 mol%) of palladium or zirconia onto the surface of the iron oxide enhanced the reduction and/or oxidation of the partially reduced iron oxide, which suppressed sintering. Palladium accelerated both the reduction and oxidation rates of partially reduced iron oxide, while zirconia increased only the oxidation rate. Addition of both palladium and zirconia together to the iron oxide resulted in marked enhancement of both reduction and oxidation. (c) 2005 Elsevier B.V. All rights reserved.

DOI CiNii
Improving Oxygen Permeability in SrFeCo0.5Ox Asymmetric Membranes by Modifying Support-layer Ｐorous Structure

IKEGUCHI Masayuki, ISHII Kentaro, SEKINE Yasushi, KIKUCHI Eiichi, MATSUKATA Masahiko

Mater. Lett. 59 ( 11 ) 1356 - 1360 2005年05月

DOI CiNii
Catalytic activities and coking resistance of Ni/perovskites in steam reforming of methane

K Urasaki, Y Sekine, S Kawabe, E Kikuchi, M Matsukata

APPLIED CATALYSIS A-GENERAL 286 ( 1 ) 23 - 29 2005年05月

　概要を見る

Steam reforming of methane for the purpose of hydrogen production was performed using nickel catalysts supported on a variety of perovskites, including LaAlO3, LaFeO3, SrTiO3, BaTiO3, La0.4Ba0.6Co0.2Fe0.8O3-delta, to compare the catalytic activity and resistance to coking of these catalysts to those of the conventional Ni/alpha-Al2O3 catalyst. Ni/LaAlO3 and Ni/SrTiO3 showed high catalytic activities among the Ni/perovskites and longer-term stabilities than the conventional catalyst. Temperature programmed oxidation of carbon deposited on used catalysts revealed that inactive carbon species detected on Ni/alpha-Al2O3 were not formed in the case of Ni/LaAlO3. The results of temperature programmed reduction confirmed that consumption and recovery of the lattice oxygen in perovskites occurred during the reaction, and that the reducibility of perovskites had a great impact on the steam reforming activity. The lattice oxygen in perovskites is considered to play important roles in promoting the oxidation of CH, fragments adsorbed on metallic nickel. (c) 2005 Published by Elsevier B.V.

DOI CiNii
Improving oxygen permeability in SrFeCo0.5Ox asymmetric membranes by modifying support-layer porous structure

M Ikeguchi, K Ishii, Y Sekine, E Kikuchi, M Matsukata

MATERIALS LETTERS 59 ( 11 ) 1356 - 1360 2005年05月

　概要を見る

Disk-type SrFeCo0.50Ox, asymmetric membranes were prepared for high-temperature oxygen separation using both a previously reported solid state technique in which ethyl cellulose is introduced and then removed by calcination to produce a porous support layer and a modified technique in which carbon fiber is added to the ethyl cellulose. The oxygen permeabilities of the resulting SrFeCo0.50Ox asymmetric membranes were measured at 973-1173 K. The addition of carbon fiber to ethyl cellulose resulted in the improvement of gas diffusivity in the porous support layer, which increased the flux of oxygen through the modified asymmetric membrane. (c) 2005 Elsevier B.V. All rights reserved.

DOI CiNii
Catalytic activities and coking resistance of Ni/perovskites in steam reforming of methane

K Urasaki, Y Sekine, S Kawabe, E Kikuchi, M Matsukata

APPLIED CATALYSIS A-GENERAL 286 ( 1 ) 23 - 29 2005年05月

　概要を見る

Steam reforming of methane for the purpose of hydrogen production was performed using nickel catalysts supported on a variety of perovskites, including LaAlO3, LaFeO3, SrTiO3, BaTiO3, La0.4Ba0.6Co0.2Fe0.8O3-delta, to compare the catalytic activity and resistance to coking of these catalysts to those of the conventional Ni/alpha-Al2O3 catalyst. Ni/LaAlO3 and Ni/SrTiO3 showed high catalytic activities among the Ni/perovskites and longer-term stabilities than the conventional catalyst. Temperature programmed oxidation of carbon deposited on used catalysts revealed that inactive carbon species detected on Ni/alpha-Al2O3 were not formed in the case of Ni/LaAlO3. The results of temperature programmed reduction confirmed that consumption and recovery of the lattice oxygen in perovskites occurred during the reaction, and that the reducibility of perovskites had a great impact on the steam reforming activity. The lattice oxygen in perovskites is considered to play important roles in promoting the oxidation of CH, fragments adsorbed on metallic nickel. (c) 2005 Published by Elsevier B.V.

DOI CiNii
Ｓtandarization of Catalyst Preparation Using Reference Catalyst. Ion Exchange of Mordenite Type Zeolite 2: Origin of Dealumination and Recommended Standard Conditions

Appl. Catal. A: General 283 ( 1-2 ) 75 - 84 2005年04月

DOI
Standardization of catalyst preparation using reference catalyst: ion exchange of mordenite type zeolite - 1. Remarkable dealumination accompanying ion exchange

N Katada, T Takeguchi, T Suzuki, T Fukushima, K Inagaki, S Tokunaga, H Shimada, K Sato, Y Oumi, T Sano, K Segawa, K Nakai, H Shoji, P Wu, T Tatsumi, T Komatsu, T Masuda, K Domen, E Yoda, JN Kondo, T Okuhara, Y Kageyama, M Niwa, M Ogura, M Matsukata, E Kikuchi, N Okazaki, M Takahashi, A Tada, S Tawada, Y Kubota, Y Sugi, Y Higashio, M Kamada, Y Kioka, K Yamamoto, T Shouji, Y Arima, Y Okamoto, H Matsumoto

APPLIED CATALYSIS A-GENERAL 283 ( 1-2 ) 63 - 74 2005年04月

　概要を見る

A joint study was organized to establish a standard set of conditions for the ion exchange of zeolite from sodium into proton-form. The sodium-form mordenite with Si/Al-2 = ca. 15 was ion exchanged into an NH4-form, followed by calcination according to various recipes. Then various advanced techniques for characterization (ICP, TG, XPS, SEM, XRD, N-2 adsorption Si-29 and Al-27 NMR, benzene diffusion, IR of OH and adsorbed pyridine and CO, ammonia TPD) were applied. and some test reactions (cracking of cumene, isopropylation of biphenyl, oligomerization of propene and chichibabin condensation of acetaldehyde and ammonia into picoline) were conducted. The ion exchange (removal of sodium) proceeded as expected, but remarkable differences were observed in physicochemical and catalytic properties of the thus-prepared proton-form samples. Exceptionally high temperature (383 K) for the ion exchange resulted in the structural degradation, while most samples exchanged at 333-353 K maintained the crystallinity and pore volume. The use of NH4Cl slightly changed the crystal morphology. Extra-framework aluminum species was formed on most samples after calcination above 773 K. In contrast, calcination at 673 K maintained the framework aluminum. Therefore, the dealumination is considered to proceed after complete removal of ammonia from the ammonium-form zeolite. However, the proton-form zeolite was stable under dry conditions, so it is speculated that the dealumination was induced by the contact of the proton-form zeolite to atmosphere with humidity. The total and Bronsted acidity decreased with the dealumination, while Lewis acidity increased. On the other hand, rapid heating of the ammonium type zeolite caused narrowing of the micropores. These structural changes seriously affected the catalytic activities for various reactions. (c) 2005 Elsevier B.V. All rights reserved.

DOI
Standardization of catalyst preparation using reference catalyst: ion exchange of mordenite type zeolite - 2. Origin of dealumination and recommended standard conditions

N Katada, T Takeguchi, T Suzuki, T Fukushima, K Inagaki, S Tokunaga, H Shimada, K Sato, Y Oumi, T Sano, K Segawa, K Nakai, H Shoji, P Wu, T Tatsumi, T Komatsu, T Masuda, K Domen, E Yoda, JN Kondo, T Okuhara, T Kanai, M Niwa, M Ogura, M Matsukata, E Kikuchi, N Okazaki, M Takahashi, A Tada, S Tawada, Y Kubota, Y Sugi, Y Higashio, M Kamada, Y Kioka, K Yamamoto, T Shouji, S Satokawa, Y Arima, Y Okamoto, H Matsumoto

APPLIED CATALYSIS A-GENERAL 283 ( 1-2 ) 75 - 84 2005年04月

　概要を見る

The undesired structural change of mordenite with Si/Al-2 = 15 during the ion exchange and during calcination from the sodium form into proton form, especially the dealumination after the calcination, was studied. The Si-29 NMR results clarified that calcination of the NH4-form mordenite with Si/Al-2 = 15 at > ca. 800 K, followed by the contact of proton-form sample with the atmosphere containing humidity, induced the dealumination. However, the samples carefully kept free from humidity after the heat treatment showed no dealumination or only a low degree of it. The Al-27 NMR and ammonia TPD results agreed with these findings. The origin of dealumination is thus considered to be the contact of the proton-form sample with humidity after the calcination. On the other hand, the dealumination was not observed after calcination at < 673 K. The H-1 NMR indicated that the ca. 1/3 of the ion-exchange sites were blocked by the ammonium cations after calcination at 673 K, suggesting that the dealumination was prevented by the ammonium cations. On the basis of these findings, a standard set of conditions in which one can safely prepare the proton-form zeolite with high quality is proposed. The recommended temperature for the ion exchange is room temperature, because it is high enough to exchange the ions in this case. The most important variable is the calcination temperature; it should be lower than 673 K in order to avoid the dealumination. These conditions were confirmed to yield zeolites with a high framework aluminum content and ordinary catalytic performance. (c) 2005 Elsevier B.V. All rights reserved.

DOI
Standardization of catalyst preparation using reference catalyst: ion exchange of mordenite type zeolite - 1. Remarkable dealumination accompanying ion exchange

N Katada, T Takeguchi, T Suzuki, T Fukushima, K Inagaki, S Tokunaga, H Shimada, K Sato, Y Oumi, T Sano, K Segawa, K Nakai, H Shoji, P Wu, T Tatsumi, T Komatsu, T Masuda, K Domen, E Yoda, JN Kondo, T Okuhara, Y Kageyama, M Niwa, M Ogura, M Matsukata, E Kikuchi, N Okazaki, M Takahashi, A Tada, S Tawada, Y Kubota, Y Sugi, Y Higashio, M Kamada, Y Kioka, K Yamamoto, T Shouji, Y Arima, Y Okamoto, H Matsumoto

APPLIED CATALYSIS A-GENERAL 283 ( 1-2 ) 63 - 74 2005年04月

　概要を見る

A joint study was organized to establish a standard set of conditions for the ion exchange of zeolite from sodium into proton-form. The sodium-form mordenite with Si/Al-2 = ca. 15 was ion exchanged into an NH4-form, followed by calcination according to various recipes. Then various advanced techniques for characterization (ICP, TG, XPS, SEM, XRD, N-2 adsorption Si-29 and Al-27 NMR, benzene diffusion, IR of OH and adsorbed pyridine and CO, ammonia TPD) were applied. and some test reactions (cracking of cumene, isopropylation of biphenyl, oligomerization of propene and chichibabin condensation of acetaldehyde and ammonia into picoline) were conducted. The ion exchange (removal of sodium) proceeded as expected, but remarkable differences were observed in physicochemical and catalytic properties of the thus-prepared proton-form samples. Exceptionally high temperature (383 K) for the ion exchange resulted in the structural degradation, while most samples exchanged at 333-353 K maintained the crystallinity and pore volume. The use of NH4Cl slightly changed the crystal morphology. Extra-framework aluminum species was formed on most samples after calcination above 773 K. In contrast, calcination at 673 K maintained the framework aluminum. Therefore, the dealumination is considered to proceed after complete removal of ammonia from the ammonium-form zeolite. However, the proton-form zeolite was stable under dry conditions, so it is speculated that the dealumination was induced by the contact of the proton-form zeolite to atmosphere with humidity. The total and Bronsted acidity decreased with the dealumination, while Lewis acidity increased. On the other hand, rapid heating of the ammonium type zeolite caused narrowing of the micropores. These structural changes seriously affected the catalytic activities for various reactions. (c) 2005 Elsevier B.V. All rights reserved.

DOI
Hydrogen Production from Biomass Ethanol at Ａmbient Ｔemperature with Ｎovel ＤｉａｐｈｒａｇｍＲｅａｃｔｏｒ

SEKINE Yasushi, ASAI Shinjiro, URASAKI Kouhei, MATSUKATA Masahiko, KIKUCHI Eiichi, KADO Shigeru, HAGA Fumihiro

Chem. Lett. 34 ( 5 ) 658 - 659 2005年

DOI CiNii
New evaluation method of carbonaceous structure on coal steam gasification

Y Sekine, K Ishikawa, E Kikuchi, M Matsukata

ENERGY & FUELS 19 ( 1 ) 326 - 327 2005年01月

DOI CiNii
A novel method for hydrogen production from liquid ethanol/water at room temperature

Y Sekine, K Urasaki, S Asai, M Matsukata, E Kikuchi, S Kado

CHEMICAL COMMUNICATIONS ( 1 ) 78 - 79 2005年

　概要を見る

We demonstrated that non-catalytic ethanol steam reforming proceeds efficiently and selectively without coking at the conditions of room temperature and atmospheric pressure using low-energy pulsed (LEP) discharge in combination with carbon fiber electrodes.

DOI PubMed CiNii
Effect of a Small Amount of Zirconia Additive on the Activity and Stability of Iron Oxide during Repeated Redox Cycles

Chem. Lett. 34 ( 2 ) 230 - 231 2005年

DOI CiNii
石炭外表面の親水・疎水度がカラム浮選成績に及ぼす影響

日本エネルギー学会誌 84 918 - 923 2005年
メタン水蒸気改質反応用Ni/perovskite触媒担体の還元性が反応に及ぼす影響

触媒 47 409 - 411 2005年
Hydrogen Production from Biomass Ethanol at Ａmbient Ｔemperature with Ｎovel ＤｉａｐｈｒａｇｍＲｅａｃｔｏｒ

Chem. Lett. 34 ( 5 ) 658 - 659 2005年

DOI CiNii
New evaluation method of carbonaceous structure on coal steam gasification

Y Sekine, K Ishikawa, E Kikuchi, M Matsukata

ENERGY & FUELS 19 ( 1 ) 326 - 327 2005年01月

DOI CiNii
A novel method for hydrogen production from liquid ethanol/water at room temperature

Y Sekine, K Urasaki, S Asai, M Matsukata, E Kikuchi, S Kado

CHEMICAL COMMUNICATIONS ( 1 ) 78 - 79 2005年

　概要を見る

We demonstrated that non-catalytic ethanol steam reforming proceeds efficiently and selectively without coking at the conditions of room temperature and atmospheric pressure using low-energy pulsed (LEP) discharge in combination with carbon fiber electrodes.

DOI PubMed CiNii
Effect of a Small Amount of Zirconia Additive on the Activity and Stability of Iron Oxide during Repeated Redox Cycles

Kohei Urasaki, Yasushi Sekine, Naoshi Tanimoto, Eri Tamura, Eiichi Kikuchi, Masahiko Matsukata

Chem. Lett. 34 ( 2 ) 230 - 231 2005年

DOI CiNii
Ｓｙｎｔｈｅｓｉｓ of MCM-41-type Mesoporous Materials using Filtrate of alkaline dissolution of ＺSM-5 Ｚeolite

INAGAKI S, OGURA M, INAMI T, SASAKIC Y, KIKUCHI E, MATSUKATA M

Microporous Mesoporous Mater. 74 ( 1-3 ) 163 - 170 2004年09月

DOI CiNii
Synthesis of MCM-41-type mesoporous materials using filtrate of alkaline dissolution of ZSM-5 zeolite

S Inagaki, M Ogura, T Inami, Y Sasaki, E Kikuchi, M Matsukata

MICROPOROUS AND MESOPOROUS MATERIALS 74 ( 1-3 ) 163 - 170 2004年09月

　概要を見る

MCM-41-type mesoporous materials possessing strong Bronsted acidity originated from ZSM-5 zeolite were synthesized by using soluble aluminosilicate species containing the fragments of the structure of ZSM-5 zeolite. The thermal stability of the mesoporous structure of the obtained mesoporous material was enhanced by the post-treatment with an ammonium aqueous solution. These results suggest an important role of alkalinity of slurries on the following two processes; (1) alkaline dissolution of ZSM-5 zeolite and (2) formation of mesoporous structure. These successive processes were efficiently improved by use of a continuous-flow reactor. The mesoporous material synthesized in the continuous-flow reactor catalyzed the cracking of cumene at 523 K, while a conventional Al-MCM-41 hardly catalyzed. The mesoporous material synthesized by using the filtrate of alkaline dissolution of ZSM-5 possessed a stronger Bronsted acidity than a conventional Al-MCM-41. (C) 2004 Elsevier Inc. All rights reserved.

DOI CiNii
Textural and catalytic properties of MCM-22 zeolite crystallized by the vapor-phase transport method

S Inagaki, K Kamino, M Hoshino, E Kikuchi, M Matsukata

BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN 77 ( 6 ) 1249 - 1254 2004年06月

　概要を見る

MCM-22 zeolite crystallized by the vapor-phase transport (VPT) method showed a higher shape-selectivity to p-xylene in the alkylation of toluene with methanol, compared with MCM-22 crystallized by the hydrothermally synthetic (HTS) method, because VPT-MCM-22 has a smaller external surface area and a smaller number of acid sites thereon than HTS-MCM-22. Such textural properties of VPT-MCM-22 are caused by the fact that the spherical particles of VPT-MCM-22 are composed of hexagonal plates as thin as 55 nm; they are larger than those of HTS-MCM-22, which are 30 nm thick. The acidic properties, characterized by NH3-TPD and FT-IR using a pyridine adsorption technique, showed no significant difference between VPT- and HTS-MCM-22, except for the acidity on the external surface.

DOI CiNii
Textural and catalytic properties of MCM-22 zeolite crystallized by the vapor-phase transport method

S Inagaki, K Kamino, M Hoshino, E Kikuchi, M Matsukata

BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN 77 ( 6 ) 1249 - 1254 2004年06月

　概要を見る

MCM-22 zeolite crystallized by the vapor-phase transport (VPT) method showed a higher shape-selectivity to p-xylene in the alkylation of toluene with methanol, compared with MCM-22 crystallized by the hydrothermally synthetic (HTS) method, because VPT-MCM-22 has a smaller external surface area and a smaller number of acid sites thereon than HTS-MCM-22. Such textural properties of VPT-MCM-22 are caused by the fact that the spherical particles of VPT-MCM-22 are composed of hexagonal plates as thin as 55 nm; they are larger than those of HTS-MCM-22, which are 30 nm thick. The acidic properties, characterized by NH3-TPD and FT-IR using a pyridine adsorption technique, showed no significant difference between VPT- and HTS-MCM-22, except for the acidity on the external surface.

DOI CiNii
Non-equilibrium Pulsed Discharge: the Difinitive Technology for PEMFC-copatible Hydrogen Generators Based on Steam Reforming Reactions

Energy and Fuels 18 455 - 459 2004年

DOI
Hydrovapothermal Conversion of Tetraethoxysilane Vapor to Polycrystalline Zeolite Layer by in situ Gelation

Chem. Commun. 899 - 900 2004年
Non-equilibrium Pulsed Discharge: the Difinitive Technology for PEMFC-copatible Hydrogen Generators Based on Steam Reforming Reactions

Energy and Fuels 18 455 - 459 2004年

DOI
Hydrovapothermal Conversion of Tetraethoxysilane Vapor to Polycrystalline Zeolite Layer by in situ Gelation

Chem. Commun. 899 - 900 2004年
The control of phase and orientation in zeolite membranes by the secondary growth method

G Li, E Kikuchi, M Matsukata

MICROPOROUS AND MESOPOROUS MATERIALS 62 ( 3 ) 211 - 220 2003年08月

　概要を見る

Mordenite and ZSM-5 seeds could grow on the surface of an asymmetric alpha-Al2O3 support using an identical organic-free aluminosilicate solution under the same hydrothermal conditions. It suggests that the phase of zeolite can be controlled by varying the type of seed. Continuous mordenite and ZSM-5 membranes were prepared by the secondary growth method using corresponding seeds under appropriate conditions. The water content in the secondary growth mixture strongly influenced the growth of zeolite crystals. ZSM-5 seeds grew at a smaller rate and showed a habit of thin hexagonal plate in a concentrated mixture, while the crystals with a habit of rectangular parallelepiped were formed from a diluted secondary growth mixture. ZSM-5 crystals had poor intergrowth in the former case, whereas the crystals were highly intergrown in the latter case. ZSM-5 crystals in either membrane have a random orientation. In contrast to ZSM-5 zeolite, the crystal orientation in the secondary grown mordenite membranes strongly depended on the water content in the secondary growth mixture. The crystals in the mordenite membrane developed in a diluted secondary growth mixture were oriented with the (1 5 0) face parallel to the support surface, whereas the crystals in the membrane grown in a concentrated mixture were oriented with the (0 0 2) face parallel to the support surface. These results suggest that the crystal orientation in mordenite membranes can be manipulated only by changing the water content in a secondary growth mixture. The formation of the preferred crystal orientation in the secondary grown mordenite membrane is discussed in terms of an "evolutionary selection" process. (C) 2003 Elsevier Inc. All rights reserved.

DOI CiNii
The control of phase and orientation in zeolite membranes by the secondary growth method

G Li, E Kikuchi, M Matsukata

MICROPOROUS AND MESOPOROUS MATERIALS 62 ( 3 ) 211 - 220 2003年08月

　概要を見る

Mordenite and ZSM-5 seeds could grow on the surface of an asymmetric alpha-Al2O3 support using an identical organic-free aluminosilicate solution under the same hydrothermal conditions. It suggests that the phase of zeolite can be controlled by varying the type of seed. Continuous mordenite and ZSM-5 membranes were prepared by the secondary growth method using corresponding seeds under appropriate conditions. The water content in the secondary growth mixture strongly influenced the growth of zeolite crystals. ZSM-5 seeds grew at a smaller rate and showed a habit of thin hexagonal plate in a concentrated mixture, while the crystals with a habit of rectangular parallelepiped were formed from a diluted secondary growth mixture. ZSM-5 crystals had poor intergrowth in the former case, whereas the crystals were highly intergrown in the latter case. ZSM-5 crystals in either membrane have a random orientation. In contrast to ZSM-5 zeolite, the crystal orientation in the secondary grown mordenite membranes strongly depended on the water content in the secondary growth mixture. The crystals in the mordenite membrane developed in a diluted secondary growth mixture were oriented with the (1 5 0) face parallel to the support surface, whereas the crystals in the membrane grown in a concentrated mixture were oriented with the (0 0 2) face parallel to the support surface. These results suggest that the crystal orientation in mordenite membranes can be manipulated only by changing the water content in a secondary growth mixture. The formation of the preferred crystal orientation in the secondary grown mordenite membrane is discussed in terms of an "evolutionary selection" process. (C) 2003 Elsevier Inc. All rights reserved.

DOI CiNii
Effects of preparation method on oxygen permeation properties of SrFeCo0.5Ox membrane

M Ikeguchi, Y Yoshino, K Kanie, M Nomura, E Kikuchi, M Matsukata

SEPARATION AND PURIFICATION TECHNOLOGY 32 ( 1-3 ) 313 - 318 2003年07月

　概要を見る

It was investigated that the effects of preparation methods and conditions for SrFeCo0.5Ox dense membrane on their oxygen permeability. Three different methods, a solid-state reaction method, an evaporation-to-dryness method, and a combined citrate and EDTA complexing method, were applied for the preparation of parent powder. The oxygen flux through membrane at 900 degreesC was increased in the order listed above. The oxygen flux could be greatly improved by repeated calcination and grinding of parent powder. The membrane sintered at a temperature as high as 1200 degreesC showed a higher oxygen flux (0.22 cm(3) (STP)/cm(2) min). (C) 2003 Elsevier Science B.V. All rights reserved.

DOI
Separation of water-acetic acid mixtures by pervaporation using a thin mordenite membrane

G Li, E Kikuchi, M Matsukata

SEPARATION AND PURIFICATION TECHNOLOGY 32 ( 1-3 ) 199 - 206 2003年07月

　概要を見る

Mordenite membranes have been prepared on the outer surface of a porous a-alumina tube by seed-assisted crystallization. The kind of silica source was found to have significant influence on the microstructure of the membrane grown on the seeded support. Highly water-selective mordenite membranes were prepared with crystallization time as short as 2-4 h at 180 degreesC. The dehydration of acetic acid by pervaporation was investigated using these thin membranes as functions of temperature and feed concentration. The separation mechanism is discussed. (C) 2003 Published by Elsevier Science B.V.

DOI
A study on the pervaporation of water-acetic acid mixtures through ZSM-5 zeolite membranes

G Li, E Kikuchi, M Matsukata

JOURNAL OF MEMBRANE SCIENCE 218 ( 1-2 ) 185 - 194 2003年07月

　概要を見る

A study was carried out on the pervaporation of water from water-acetic acid mixtures through tubular ZSM-5 zeolite membranes. ZSM-5 zeolite membranes were prepared on the outer surface of a porous a-alumina tube by the seed-assisted crystallization method in the absence of organic templates. It was observed that water preferentially permeated with selectivities higher than the selectivity based on the vapor-liquid equilibrium in the entire range of acetic acid concentration. The separation mechanism of water through ZSM-5 zeolite membranes was discussed and compared with that through mordenite membranes. It was found that the permeability coefficients of both water and acetic acid decreased with increasing temperature, although the pervaporation fluxes of both water and acetic acid increased. As a result, it was concluded that the increase in the pervaporation flux with temperature was due to the increase in the driving force in terms of transmembrane partial vapor pressure difference with temperature. According to the mechanism proposed herein, a study was also directed to modify as-synthesized membranes for the improvement in their pervaporation performance. It was observed that both the water flux and the separation factor were increased through a membrane treated in alkaline solution under appropriate conditions. (C) 2003 Elsevier Science B.V. All rights reserved.

DOI CiNii
Effects of preparation method on oxygen permeation properties of SrFeCo0.5Ox membrane

M Ikeguchi, Y Yoshino, K Kanie, M Nomura, E Kikuchi, M Matsukata

SEPARATION AND PURIFICATION TECHNOLOGY 32 ( 1-3 ) 313 - 318 2003年07月

　概要を見る

It was investigated that the effects of preparation methods and conditions for SrFeCo0.5Ox dense membrane on their oxygen permeability. Three different methods, a solid-state reaction method, an evaporation-to-dryness method, and a combined citrate and EDTA complexing method, were applied for the preparation of parent powder. The oxygen flux through membrane at 900 degreesC was increased in the order listed above. The oxygen flux could be greatly improved by repeated calcination and grinding of parent powder. The membrane sintered at a temperature as high as 1200 degreesC showed a higher oxygen flux (0.22 cm(3) (STP)/cm(2) min). (C) 2003 Elsevier Science B.V. All rights reserved.

DOI
Separation of water-acetic acid mixtures by pervaporation using a thin mordenite membrane

G Li, E Kikuchi, M Matsukata

SEPARATION AND PURIFICATION TECHNOLOGY 32 ( 1-3 ) 199 - 206 2003年07月

　概要を見る

Mordenite membranes have been prepared on the outer surface of a porous a-alumina tube by seed-assisted crystallization. The kind of silica source was found to have significant influence on the microstructure of the membrane grown on the seeded support. Highly water-selective mordenite membranes were prepared with crystallization time as short as 2-4 h at 180 degreesC. The dehydration of acetic acid by pervaporation was investigated using these thin membranes as functions of temperature and feed concentration. The separation mechanism is discussed. (C) 2003 Published by Elsevier Science B.V.

DOI
ZSM-5 zeolite membranes prepared from a clear template-free solution

G Li, E Kikuchi, M Matsukata

MICROPOROUS AND MESOPOROUS MATERIALS 60 ( 1-3 ) 225 - 235 2003年06月

　概要を見る

Template-free nanosized ZSM-5 seeds were prepared from commercially available ZSM-5 powder. By use of these seeds, thin and hydrophilic ZSM-5 zeolite membranes were prepared on the outer surface of a porous a-alumina tube in a clear solution free from organic template. The membranes showed high thermal stability to withstand pretreatment at 400 degreesC, At 270 degreesC, the ideal selectivities for H-2/i-butane and N-2/SF6 were 61 and 20, respectively. The membrane was effective to separate butane isomers at high temperatures. The maximum of the n/i-butane ideal selectivity was 36 at 300 degreesC. The separation factors for a 50/50 n/i-butane mixture were as high as 13 in the temperature range from 300 to 400 degreesC. (C) 2003 Elsevier Science Inc. All rights reserved.

DOI CiNii
ZSM-5 zeolite membranes prepared from a clear template-free solution

G Li, E Kikuchi, M Matsukata

MICROPOROUS AND MESOPOROUS MATERIALS 60 ( 1-3 ) 225 - 235 2003年06月

　概要を見る

Template-free nanosized ZSM-5 seeds were prepared from commercially available ZSM-5 powder. By use of these seeds, thin and hydrophilic ZSM-5 zeolite membranes were prepared on the outer surface of a porous a-alumina tube in a clear solution free from organic template. The membranes showed high thermal stability to withstand pretreatment at 400 degreesC, At 270 degreesC, the ideal selectivities for H-2/i-butane and N-2/SF6 were 61 and 20, respectively. The membrane was effective to separate butane isomers at high temperatures. The maximum of the n/i-butane ideal selectivity was 36 at 300 degreesC. The separation factors for a 50/50 n/i-butane mixture were as high as 13 in the temperature range from 300 to 400 degreesC. (C) 2003 Elsevier Science Inc. All rights reserved.

DOI CiNii
Selective Deposition of Pd on Porous Alumina Support Using Supercritical CO2

Mat. Res. Soc. Symp. Proc. 752 265 - 270 2003年
Steam Reforming of Methanol on Ni/Al2O3 Catalyst in a Pd-membrane Reactor

菊地英一, 河部正, 松方正彦

J. Jpn Petrol. Inst. 46 ( 2 ) 93 - 98 2003年

DOI CiNii
Hydroisomerization of Tetralin on Zeolite Beta: Influence of Crystal Size

Stud. Surf. Sci. Catal. 145 219 - 222 2003年
Trace element behavior on coal combustion

12th ICCS 2003年
The behavior of trace Elements from High Temperature Coal Combustion Process

ACS 225th 2003年
Steam Reforming of Hydrocarbons and Alcohols Using Non-equilibrium Pulsed Discharge

ISPC 16 2003年
Selective Oxidation of Ethylene-Glycol by Active Carbon Catalyst

GSCTOKYO2003 2003年
Preparation of asymmetric ceramic membranes for oxygen permeation with slurries

NAMS 2003 2003年
Non-equilibrium Pulsed Discharge; Definitive Technology for PEMFC-compatibleH2 Generators

GSCTOKYO2003 2003年
Hydrogen-Butane Separation Through MFI-type Zeolite Membrane Grown by a Secondary Growth Method

ACS 225th 2003年
Effect of Water Adsorption on Permeation Properties of MFI-type Zeolite Membrane Produced by in-situ Crystallization

ACS 225th 2003年
Effect of Pd on the activity of Fe-K mixed oxide catalyst for dehydrogenation of ethylbenzene

APCAT3 2003年
Development of Liquid Fuel Reformer Using Low Energy Pulsed Discharge at Room Temperature

ISPC 16 2003年
Characterization of gas phase reaction with pulsed discharge under atmospheric pressure

FLTPD-V 2003年
Behavior of coal minerals on steam gasification of coal char

The 8th Japan China Symposium on Coal and C1 Chemistry 2003年
Ash Rejection Behavior on Continuous Column Flotation Process

ACS 225th 2003年
触媒研究の現状と将来動向：水素透過膜による触媒反応の高効率化と夢の難反応の実現

触媒技術の動向と展望／触媒学会 p.4-13 2003年
低エネルギーパルス放電を用いた水素製造プロセス

ケミカルエンジニアリング 12, 25-33 2003年
Selective Deposition of Pd on Porous Alumina Support Using Supercritical CO2

Mat. Res. Soc. Symp. Proc. 752 265 - 270 2003年
パラジウムメンブレンリアクターにおけるNi/Al2O3触媒上でのメタノール水蒸気改質

菊地英一, 河部正, 松方正彦

Journal of the Japan Petroleum Institute 46 ( 2 ) 93 - 98 2003年

DOI CiNii
A Study on the Pervaporation of Water-Acetic Acid Mixtures through ZSM-5 Zeolite Membranes

J. Membrane Sci. 218 ( 1/2 ) 185 - 194 2003年

DOI CiNii
Hydroisomerization of Tetralin on Zeolite Beta: Influence of Crystal Size

Stud. Surf. Sci. Catal. 145 219 - 222 2003年
Trace element behavior on coal combustion

12th ICCS 2003年
The behavior of trace Elements from High Temperature Coal Combustion Process

ACS 225th 2003年
Steam Reforming of Hydrocarbons and Alcohols Using Non-equilibrium Pulsed Discharge

ISPC 16 2003年
Selective Oxidation of Ethylene-Glycol by Active Carbon Catalyst

GSCTOKYO2003 2003年
Preparation of asymmetric ceramic membranes for oxygen permeation with slurries

NAMS 2003 2003年
Non-equilibrium Pulsed Discharge; Definitive Technology for PEMFC-compatibleH2 Generators

GSCTOKYO2003 2003年
Hydrogen-Butane Separation Through MFI-type Zeolite Membrane Grown by a Secondary Growth Method

ACS 225th 2003年
Effect of Water Adsorption on Permeation Properties of MFI-type Zeolite Membrane Produced by in-situ Crystallization

ACS 225th 2003年
Effect of Pd on the activity of Fe-K mixed oxide catalyst for dehydrogenation of ethylbenzene

APCAT3 2003年
Development of Liquid Fuel Reformer Using Low Energy Pulsed Discharge at Room Temperature

ISPC 16 2003年
Characterization of gas phase reaction with pulsed discharge under atmospheric pressure

FLTPD-V 2003年
Behavior of coal minerals on steam gasification of coal char

The 8th Japan China Symposium on Coal and C1 Chemistry 2003年
Ash Rejection Behavior on Continuous Column Flotation Process

ACS 225th 2003年
Crystallization behavior of zeolite beta during steam-assisted crystallization of dry gel

M Matsukata, T Osaki, M Ogura, E Kikuchi

MICROPOROUS AND MESOPOROUS MATERIALS 56 ( 1 ) 1 - 10 2002年10月

　概要を見る

Zeolite beta with SiO2/Al2O3 ratios from 30 to 730 was synthesized by a steam-assisted crystallization method, and the crystallized products obtained within 24 h were characterized by means of chemical analyses, XRD, FE-SEM, Si-29- MAS NMR, N-2 adsorption, and temperature-programmed decomposition of tetraethylammonium cation occluded in the micropores of zeolite beta. Based on these results, the crystallization mechanism is discussed herein. It was found that agglomerates of nano-particles were formed from a dry gel before the development of a periodical structure in a long-range order, which can be detected by XRD. After several hours of crystallization, morphological changes in nano-particle agglomerates proceeded to give highly crystalline zeolite beta. (C) 2002 Elsevier Science Inc. All rights reserved.

DOI
Crystallization behavior of zeolite beta during steam-assited crystallization of dry gel

M. Matsukata, T. Osaki, M. Ogura, E. Kikuchi

Microporous and Mesoporous Materials 56 ( 1 ) 1 - 10 2002年10月

　概要を見る

Zeolite beta with SiO2/Al2O3 ratios from 30 to 730 was synthesized by a steam-assisted crystallization method, and the crystallized products obtained within 24 h were characterized by means of chemical analyses, XRD, FE-SEM, 29Si-MAS NMR, N2 adsorption, and temperature-programmed decomposition of tetraethylammonium cation occluded in the micropores of zeolite beta. Based on these results, the crystallization mechanism is discussed herein. It was found that agglomerates of nano-particles were formed from a dry gel before the development of a periodical structure in a long-range order, which can be detected by XRD. After several hours of crystallization, morphological changes in nano-particle agglomerates proceeded to give highly crystalline zeolite beta. © 2002 Elsevier Science Inc. All rights reserved.

DOI
Co Cation Effects on Activity and Stability of Isolated Pd(II) Cations in Zeolite Matrices for Selective Catalytic Reduction of Nitric Oxide with Methane

OGURA M, KAGE S, SHIMOJO T, OBA J, HAYASHI M, MATSUKATA M, KIKUCHI E

J. Catal. 211 ( 1 ) 75 - 84 2002年

DOI CiNii
Synthesis of MCM-22 Zeolite by the Vapor-phase Transport Method

Stud. Surf. Sci. Catal. 142 53 - 60 2002年
Co Cation Effects on Activity and Stability of Isolated Pd(II) Cations in Zeolite Matrices for Selective Catalytic Reduction of Nitric Oxide with Methane

J. Catal. 211 ( 1 ) 75 - 84 2002年

DOI CiNii
Synthesis of MCM-22 Zeolite by the Vapor-phase Transport Method

Stud. Surf. Sci. Catal. 142 53 - 60 2002年
Quantitative analyses for TEA(+) and Na+ contents in zeolite beta with a wide range of Si/2Al ratio

M Matsukata, M Ogura, T Osaki, E Kikuchi, A Mitra

MICROPOROUS AND MESOPOROUS MATERIALS 48 ( 1-3 ) 23 - 29 2001年11月

　概要を見る

Beta zeolites with a wide range of Si/2Al ratios from 7 to infinity were synthesized by steam-assisted crystallization method. X-ray diffraction, FE-SEM, and MASNMR studies confirmed the formation of highly crystalline zeolite beta and Al incorporation in the framework under various conditions by the SAC method at temperatures ranging from 373 to 438 K. Na+ and TEA(+) contents occluded in micropores of beta zeolite were determined. Quantitative knowledge on such occluded cations gave great insight on understanding crystallization mechanism of beta. (C) 2001 Published by Elsevier Science B.V.

DOI CiNii
Synthesis of EMT zeolite by a steam-assisted crystallization method using crown ether as a structure-directing agent

M Matsukata, K Kizu, M Ogura, E Kikuchi

CRYSTAL GROWTH & DESIGN 1 ( 6 ) 509 - 516 2001年11月

　概要を見る

A high-silica hexagonal faujasite EMT was crystallized by a steam-assisted crystallization (SAC) method using a crown ether of 1,4,7,10,13,16-hexaoxacyclooctadecane, 18-crown-6, as a structure-directing agent. The growth mechanism of EMT by SAC is quite different from that of EMT by the conventional hydrothermal synthetic method, in which layer-by-layer growth occurs. Another characteristic of SAC is that nanoparticles fuse and the surface of the dry gel is rearranged, resulting in a distinct hexagonal shape for the EMT crystals. Sodium content must be strictly defined when the SAC method is used, and the crystallization temperature must be kept below 408 K to keep the crown ether in the dry gel to obtain a pure phase of EMT.

DOI
Quantitative analyses for TEA(+) and Na+ contents in zeolite beta with a wide range of Si/2Al ratio

M Matsukata, M Ogura, T Osaki, E Kikuchi, A Mitra

MICROPOROUS AND MESOPOROUS MATERIALS 48 ( 1-3 ) 23 - 29 2001年11月

　概要を見る

Beta zeolites with a wide range of Si/2Al ratios from 7 to infinity were synthesized by steam-assisted crystallization method. X-ray diffraction, FE-SEM, and MASNMR studies confirmed the formation of highly crystalline zeolite beta and Al incorporation in the framework under various conditions by the SAC method at temperatures ranging from 373 to 438 K. Na+ and TEA(+) contents occluded in micropores of beta zeolite were determined. Quantitative knowledge on such occluded cations gave great insight on understanding crystallization mechanism of beta. (C) 2001 Published by Elsevier Science B.V.

DOI CiNii
Effect of NH+ 4 Exchange on Hydrophobicity and Catalytic Properties of Al-Free Ti-Si-beta Zeolite

Masaru Ogura, Shin-Ichi Nakata, Eiichi Kikuchi, Masahiko Matsukata

Journal of Catalysis 199 ( 1 ) 41 - 47 2001年04月

　概要を見る

Al-free Ti-Si-beta was synthesized by a steam-assisted crystallization (SAC) method using tetraethylammonium hydroxide as a structure-directing agent. It was noted that Na in a parent gel was essential for synthesizing highly crystalline Ti-Si-beta by means of the SAC method. An absorption band at 225 nm, assigned to isolated Ti species, and another band at around 270 nm appeared in the UV spectra of the Ti-Si-beta. The latter absorption band decreased upon ion exchange of as-synthesized materials with 1 M aqueous NH4NO3 solution, and this treatment did not change the SiO2/TiO2 molar ratio in Ti-Si-beta. The Q3 signal in the 29Si-NMR spectrum almost disappeared and the amount of H2O adsorbed decreased due to the NH+ 4 exchange of Ti-Si-beta. The NH+ 4 exchange resulted in a higher catalytic activity of the zeolite for cyclohexene epoxidation with H2O2 and a high selectivity toward epoxide compared with the H2SO4-treated Ti-Si-beta and Al-containing Ti-beta samples prepared in this study. Summarizing these results, the NH+ 4 exchange of Ti-Si-beta zeolite is found to induce a hydrophobic environment around Ti sites without detitanation from the zeolite frame-work. © 2001 Academic Press.

DOI CiNii
Effect of NH4+ exchange on hydrophobicity and catalytic properties of Al-free Ti-Si-beta zeolite

M Ogura, S Nakata, E Kikuchi, M Matsukata

JOURNAL OF CATALYSIS 199 ( 1 ) 41 - 47 2001年04月

　概要を見る

Al-free Ti-Si-beta was synthesized by a steam-assisted crystallization (SAC) method using tetraethylammonium hydroxide as a structure-directing agent. It was noted that Na in a parent gel was essential for synthesizing highly crystalline Ti-Si-beta by means of the SAC method. An absorption band at 225 nm, assigned to isolated Ti species, and another band at around 270 nm appeared in the UV spectra of the Ti-Si-beta. The latter absorption band decreased upon ion exchange of as-synthesized materials with 1 M aqueous NH4NO3 solution, and this treatment did not change the SiO2/TiO2 molar ratio in Ti-Si-beta. The Q(3) signal in the Si-29-NMR spectrum almost disappeared and the amount of H2O adsorbed decreased due to the NH4+ exchange of Ti-Si-beta. The NH4+ exchange resulted in a higher catalytic activity of the zeolite far cyclohexene epoxidation with H2O2 and a high selectivity toward epoxide compared with the H2SO4-treated Ti-Si-beta and AI-containing Ti-beta samples prepared in this study. Summarizing these results, the NH4+ exchange of Ti-Si-beta zeolite is found to induce a hydrophobic environment around Ti sites without detitanation from the zeolite framework. (C) 2001 Academic Press.

DOI CiNii
Alkali treatment technique ? new method for modification of structural and acid-catalytic properties of ZSM-5 zeolites

Appl. Catal. A219, 33 2001年

DOI
Novel organic-vycor glass composite membrane having Si-C bonds

NOMURA M, MINETA Y, YAMAGUCHI N, KIKUCHI E, FUKUNAGA K, NISHIYAMA N, UEYAMA K, MATSUKATA M

J. Chem. Eng. Japan 34 ( 6 ) 731 - 736 2001年

DOI
Separation of Hydrogen from Gas Mixtures Using Supported Platinum-group Metal Membranes(共著)

UEMIYA S, KATO W, UYAMA A, KAJIWARA M, KOJIMA T, KIKUCHI E

Separation & Purification Technology 22/23 ( 1/3 ) 309 - 317 2001年

DOI CiNii
Influence of Nano-particle Agglomeration on the Catalytic Properties of MFI Zeolite

Stud. Surf. Sci. Catal. 135 566 - 572 2001年
Growth of Oriented Mordenite Membranes on Porous a-Al2O3 Support

Stud. Surf. Sci. Catal. 135 3151 - 3159 2001年
MFI Zeolite with Uniform Mesopores Created by Alkali Treatment

Stud. Surf. Sci. Catal. 135 1820 - 1827 2001年
Synthesis of Msoporous Materials Using Filtrate of Alkali Treatment of MFI Zeolite

Stud. Surf. Sci. Catal. 135 1290 - 1297 2001年
ゼオライトに担持された金属カチオンの触媒特性‐HC-SCRを反応例とした眺望

ゼオライト 18;89 2001年

DOI
21世紀のゼオライト学会への期待

ゼオライト 18(1);1 2001年
Alkali treatment technique ? new method for modification of structural and acid-catalytic properties of ZSM-5 zeolites

Appl. Catal. A219, 33 2001年

DOI
Novel organic-vycor glass composite membrane having Si-C bonds

J. Chem. Eng. Japan 34 ( 6 ) 731 - 736 2001年

DOI
Separation of Hydrogen from Gas Mixtures Using Supported Platinum-group Metal Membranes(共著)

Separation & Purification Technology 22/23 ( 1/3 ) 309 - 317 2001年

DOI CiNii
Synthesis of EMT Zeolite by a Steam-assisted Crystallization Method Using Crown Ether as a Structure-directing Agent

Crystal Growth & Design 2001 509 - 516 2001年

DOI
Influence of Nano-particle Agglomeration on the Catalytic Properties of MFI Zeolite

Stud. Surf. Sci. Catal. 135 566 - 572 2001年
Growth of Oriented Mordenite Membranes on Porous a-Al2O3 Support

Stud. Surf. Sci. Catal. 135 3151 - 3159 2001年
MFI Zeolite with Uniform Mesopores Created by Alkali Treatment

Stud. Surf. Sci. Catal. 135 1820 - 1827 2001年
Synthesis of Msoporous Materials Using Filtrate of Alkali Treatment of MFI Zeolite

Stud. Surf. Sci. Catal. 135 1290 - 1297 2001年
Membrane reactor application to hydrogen production

E. Kikuchi

Catalysis Today 56 ( 1-3 ) 97 - 101 2000年02月

　概要を見る

Selective removal of hydrogen in a membrane reactor enables the hydrogen production by steam reforming at lower reaction temperatures than conventional processes. We invented a composite membrane consisting of thin palladium layer deposited on the outer surface of porous ceramics by electroless-plating. The palladium layer could completely cover the surface, so that only hydrogen could permeate through the membrane with a 100% selectivity. By use of this kind of membrane, Tokyo Gas and Mitsubishi Heavy Industries have developed a membrane reformer applicable to the polymer electrolyte fuel cell system. Our current approach is the application of a CVD technique to deposit non-Pd metals, such as Pt, to overcome the limitations caused by Pd membranes, such as hydrogen embrittlement. The permeability and permeation selectivity of these metal-ceramic composite CVD membranes were investigated in a comparison with electroless-plating palladium membranes, as well as the performance in membrane reactors applied to steam reforming of methane. The permeation of hydrogen through the CVD membranes is not based on the solution-diffusion transport mechanism but on the surface diffusion mechanism. Although the CVD membranes gave higher conversion of methane than thermodynamic equilibrium, their performance became similar to electroless-plating membranes, only when the membranes showed high H2/N2 separation factors. © 2000 Elsevier Science B.V All rights reserved.

DOI
Membrane reactor application to hydrogen production

E Kikuchi

CATALYSIS TODAY 56 ( 1-3 ) 97 - 101 2000年02月

　概要を見る

Selective removal of hydrogen in a membrane reactor enables the hydrogen production by steam reforming at lower reaction temperatures than conventional processes. We invented a composite membrane consisting of thin palladium layer deposited on the outer surface of porous ceramics by electroless-plating. The palladium layer could completely cover the surface, so that only hydrogen could permeate through the membrane with a 100% selectivity. By use of this kind of membrane, Tokyo Gas and Mitsubishi Heavy Industries have developed a membrane reformer applicable to the polymer electrolyte fuel cell system. Our current approach is the application of a CVD technique to deposit non-Pd metals, such as Pt, to overcome the limitations caused by Pd membranes, such as hydrogen embrittlement. The permeability and permeation selectivity of these metal-ceramic composite CVD membranes were investigated in a comparison with electroless-plating palladium membranes, as well as the performance in membrane reactors applied to steam reforming of methane. The permeation of hydrogen through the CVD membranes is not based on the solution-diffusion transport mechanism but on the surface diffusion mechanism. Although the CVD membranes gave higher conversion of methane than thermodynamic equilibrium, their performance became similar to electroless-plating membranes, only when the membranes showed high H-2/N-2 separation factors. (C) 2000 Elsevier Science B.V. All rights reserved.

DOI
Remarkable Enhancement in Durability of Pd/H-ZSM-5 Zeolite Catalysts for CH₄-SCR(共著)

Appl. Catal. B27/,L213 2000年

DOI
Rhodium-and Iridium-dispersed Porous Alumina Membranes and Their Hydrogen Permeation Properties(共著)

KAJIWARA M, UEMIYA S, KOJIMA T, KIKUCHI E

Catal. Today 56 ( 1/3 ) 83 - 87 2000年

DOI CiNii
Steam Reforming of Methane in Membrane Reactors : Comparison of Electroless-plating and CVD Membranes and Catalyst Packing Modes(共著)

KIKUCHI E, NEMOTO Y, KAJIWARA M, UEMIYA S, KOJIMA T

Catal. Today 56 ( 1/3 ) 75 - 81 2000年

DOI CiNii
Hydrogen Permeation Properties through Composite Membranes of Platinum Supported on Porous Alumina(共著)

KAJIWARA M, UEMIYA S, KOJIMA T, KIKUCHI E

Catal. Today 56 ( 1/3 ) 65 - 73 2000年

DOI CiNii
Palladium Species in Pd/H-ZSM-5 Zeolite Catalysts for CH₄-SCR(共著)

KIKUCHI E, OGURA M

Res. Chem. Intermed. 26 ( 1 ) 55 - 60 2000年

DOI CiNii
Preparation of Mordenite Membranes on-Alumina Tubular Supports for Pervaporation of Water-isopropyl alcohol Mixtures(共著)

Chem. Comm. 2000/,957 2000年
Formation of Uniform Mesopores in ZSM-5 Zeolite through Treatment in Alkaline Solution(共著)

Chem. Lett. 2000/,882 2000年
Catalytic Activity of Ir for NO-CO Reaction in the Presence of SO2 and Excess Oxygen

Chem.Lett. 2000 2000年

DOI
Remarkable Enhancement in Durability of Pd/H-ZSM-5 Zeolite Catalysts for CH₄-SCR(共著)

Appl. Catal. B27/,L213 2000年

DOI
Rhodium-and Iridium-dispersed Porous Alumina Membranes and Their Hydrogen Permeation Properties(共著)

Catal. Today 56 ( 1/3 ) 83 - 87 2000年

DOI CiNii
Steam Reforming of Methane in Membrane Reactors : Comparison of Electroless-plating and CVD Membranes and Catalyst Packing Modes(共著)

Catal. Today 56 ( 1/3 ) 75 - 81 2000年

DOI CiNii
Hydrogen Permeation Properties through Composite Membranes of Platinum Supported on Porous Alumina(共著)

Catal. Today 56 ( 1/3 ) 65 - 73 2000年

DOI CiNii
Palladium Species in Pd/H-ZSM-5 Zeolite Catalysts for CH₄-SCR(共著)

Res. Chem. Intermed. 26 ( 1 ) 55 - 60 2000年

DOI CiNii
Preparation of Mordenite Membranes on-Alumina Tubular Supports for Pervaporation of Water-isopropyl alcohol Mixtures(共著)

Chem. Comm. 2000/,957 2000年
Formation of Uniform Mesopores in ZSM-5 Zeolite through Treatment in Alkaline Solution(共著)

Chem. Lett. 2000/,882 2000年
Catalytic Activity of Ir for NO-CO Reaction in the Presence of SO2 and Excess Oxygen

Chem.Lett. 2000 2000年

DOI
Selective Reduction of NO by CH4 on Pd- and Co/Pd-HZSM-5 Catalysts

The Fourth International Conference on Environmental Catalysis 1999年
Determination of Active Palladium Species in ZSM-5 Zeolite for Selective Reduction of Nitric Oxide with Methane

Appl.Catal. B23 1999年

DOI
Catalytic Performances of Cobalt-based Ultrafine Particles Prepared by Chemical Reducation in Slurry-phase Fischer-Tropsch Synthesis

KIKUCHI E, SORITA R, TAKAHASHI H, MATSUDA T

Appl. Catal. 186 ( 1/2 ) 121 - 128 1999年

DOI CiNii
Conversion of Dry Gel to Microporous Crystals in Gas Phase

Topics in Catal, 9, 77 (1999) 9 1999年
Palladium Species in Co/Pd/H-ZSM-5 Catalysts for CH4-SCR of NOx

Proceedings of the12th International Zeolite Conference 2833 1999年
Synthesis of OU-1, a Large-pore, High Silica Zeolite by Dry Gel Conversion

Proceedings of the12th International Zeolite Conference 2009 1999年
Synthesis of Pure Silica BEA and Al-free Ti-BEA using TEAOH and Their Characterization

Proc.of the 12th Intl.Zeolite Conf. 1515 1999年
Conversion of Dry Gels to Zeolites(共著)

Proc. Internal. Conf. On Solid-Solid Phase Transformation'99(JIMIC-3) /,1421 1999年
窒素酸化物の炭化水素-SCR反応活性点と反応機構

地球環境講演会 1999年
Selective Reduction of NO by CH4 on Pd- and Co/Pd-HZSM-5 Catalysts

The Fourth International Conference on Environmental Catalysis 1999年
Determination of Active Palladium Species in ZSM-5 Zeolite for Selective Reduction of Nitric Oxide with Methane

Appl.Catal. B23 1999年

DOI
Catalytic Performances of Cobalt-based Ultrafine Particles Prepared by Chemical Reducation in Slurry-phase Fischer-Tropsch Synthesis

Appl. Catal. 186 ( 1/2 ) 121 - 128 1999年

DOI CiNii
Conversion of Dry Gel to Microporous Crystals in Gas Phase

Topics in Catal, 9, 77 (1999) 9 1999年
Palladium Species in Co/Pd/H-ZSM-5 Catalysts for CH4-SCR of NOx

Proceedings of the12th International Zeolite Conference 2833 1999年
Synthesis of OU-1, a Large-pore, High Silica Zeolite by Dry Gel Conversion

Proceedings of the12th International Zeolite Conference 2009 1999年
Synthesis of Pure Silica BEA and Al-free Ti-BEA using TEAOH and Their Characterization

Proc.of the 12th Intl.Zeolite Conf. 1515 1999年
Conversion of Dry Gels to Zeolites(共著)

Proc. Internal. Conf. On Solid-Solid Phase Transformation'99(JIMIC-3) /,1421 1999年
Active Sites of HC-SCR Catalysts based on Pd/ZSM-5

17th International Conference on Catalysis - The Taniguchi Foundation-, 1998年
Membrane Reactor Application to Hydrogen Production(Plenary)

Third International Conference on Catalysis in Membrane Reactors(Copenhagen) 1998年
Heterogeneous Catalysis in Membrane Reactors

International Catalysis Symposium on “Frontier and Tasks of Catalysis towards Next Century”（文部省） 1998年
Hydrogen Permeation through Composite CVD Membranes of Group VIII Metals and Porous Alumina

Proceedings of the Fifth Intl. Conference on Inorganic Membranes p.250 1998年
Role of Zeolite Structure on Reduction of Nox with Methane over In-and Pd-based Catalysts

Catalysis Today/ Elsevier 45;p.139 1998年

DOI
Intrapore Catalysis in Reduction of Nitric Oxide with Methane

Catalysis Today/ Elsevier 42;p.159 1998年

DOI
The Effect of Zeolite Structures on the Creation of InO⁺ Active Sites for NOx

OGURA M, OHSAKI T, KIKUCHI E

Microporous and Mesoporous Materials/Elsevier 21 ( 4/6 ) 533 - 540 1998年

DOI CiNii
Phase Transformation of High Silica BEA to OU-1 and MTW

Chem. Lett., 日本化学会 1998巻,311頁 1998年
Phase Transformation of High Silica BEA to OU-1 and MTW

Chemistry Letters、日本化学会 1998;p.311 1998年
Syngas Formation by Partial Oxidation of Methane in Palladium Membrane Reactor

Studies in Surface Science and Catalysis/ Elsevier 119;p.441 1998年
無機膜の進歩とメンブレンリアクターへの応用 - 水素製造反応を適用例として -（展望講演）

化学工学会 1998年
ゼオライトでNOxを還元する

化学と教育/日本化学会 12;p.760 1998年
Active Sites of HC-SCR Catalysts based on Pd/ZSM-5

17th International Conference on Catalysis - The Taniguchi Foundation-, 1998年
Membrane Reactor Application to Hydrogen Production(Plenary)

Third International Conference on Catalysis in Membrane Reactors(Copenhagen) 1998年
Heterogeneous Catalysis in Membrane Reactors

International Catalysis Symposium on “Frontier and Tasks of Catalysis towards Next Century”（文部省） 1998年
Hydrogen Permeation through Composite CVD Membranes of Group VIII Metals and Porous Alumina

Proceedings of the Fifth Intl. Conference on Inorganic Membranes p.250 1998年
Role of Zeolite Structure on Reduction of Nox with Methane over In-and Pd-based Catalysts

Catalysis Today/ Elsevier 45;p.139 1998年

DOI
Intrapore Catalysis in Reduction of Nitric Oxide with Methane

Catalysis Today/ Elsevier 42;p.159 1998年

DOI
The Effect of Zeolite Structures on the Creation of InO⁺ Active Sites for NOx

Microporous and Mesoporous Materials/Elsevier 21 ( 4/6 ) 533 - 540 1998年

DOI CiNii
Phase Transformation of High Silica BEA to OU-1 and MTW

Chem. Lett., 日本化学会 1998巻,311頁 1998年
Phase Transformation of High Silica BEA to OU-1 and MTW

Chemistry Letters、日本化学会 1998;p.311 1998年
Syngas Formation by Partial Oxidation of Methane in Palladium Membrane Reactor

Studies in Surface Science and Catalysis/ Elsevier 119;p.441 1998年
Catalytic Properties of Pd/Al2O3 calcined at high temperatures for methane combustion(San Francisco)

ACS Symposium on Catalytic Combustion 1997年
Hydrogen-Permselective Membrane Reactors

CaTTech, Baltzer 第1巻, 67頁 1997年
Zeolitic Membranes: Synthesis, Properties and Prospects

Bull. Chem. Soc. Jpn.，日本化学会第70巻,2341頁 1997年

DOI
Selective Reduction of Nitric Oxide with Methane on In/H-ZSM-5-based Catalysts

Catal. Surveys from Jpn., Baltzer 第1巻,227頁 1997年
Synthesis of a zeolitic thin layer by a vapor-phase transport method: appearance of a preferential orientation of MFI zeolite

Microporous Materials, Elsevier 第11巻,107頁 1997年

DOI
Low-Temperature Syngas Formation by CO2 Reforming of Methane in a Hydrogen-Permselective Membrane Reactor.

Stud. Surf. Sci. and Catal. Elsevier 第107巻, 547頁 1997年
Low-Temperature Syngas Formation by CO₂ Reforming of Methane in a Hydrogen-Permselective Membrane Reactor

Stud. in Surface Science and Catalysis 107/,547 1997年
Hydrogen-Permselective Membrane Reactors

CaTTech. 1/,67 1997年
次世代リーンNOx触媒の開発

NGCフォーラム'97 1997年
メンブレンリアクター利用触媒反応プロセス

触媒学会 1997年
メタンによるNO選択還元反応における機能複合化効果

文部省重点領域研究公開シンポ 1997年
ゼオライトの細孔で起こる炭化水素-SCR反応

触媒学会 1997年
Catalytic Properties of Pd/Al2O3 calcined at high temperatures for methane combustion(San Francisco)

ACS Symposium on Catalytic Combustion 1997年
Hydrogen-Permselective Membrane Reactors

CaTTech, Baltzer 第1巻, 67頁 1997年
Zeolitic Membranes: Synthesis, Properties, and Prospects.

Matsukata Masahiko, Kikuchi Eiichi

Bulletin of the Chemical Society of Japan 第70巻,2341頁 ( 10 ) 2341 - 2356 1997年

　概要を見る

This article is intended to describe recent progress in the synthesis of zeolitic membranes and their permeation properties. While hydrothermal synthesis has been widely employed for zeolitic-membrane synthesis, the development of a new technique for zeolite synthesis, vapor-phase transport (VPT), has enabled us to prepare pinhole-free, zeolite-porous support composite membranes. This article consists of three sections that describe: a survey of the hydrothermal synthesis of zeolitic membranes, our synthesis results and the formation mechanism of zeolitic membranes by the VPT method as well as some permeation results to show the prospects of zeolitic membranes.

DOI CiNii
Selective Reduction of Nitric Oxide with Methane on In/H-ZSM-5-based Catalysts

Catal. Surveys from Jpn., Baltzer 第1巻,227頁 1997年
Synthesis of a zeolitic thin layer by a vapor-phase transport method: appearance of a preferential orientation of MFI zeolite

Microporous Materials, Elsevier 第11巻,107頁 1997年

DOI
Low-Temperature Syngas Formation by CO2 Reforming of Methane in a Hydrogen-Permselective Membrane Reactor.

Stud. Surf. Sci. and Catal. Elsevier 第107巻, 547頁 1997年
Low-Temperature Syngas Formation by CO₂ Reforming of Methane in a Hydrogen-Permselective Membrane Reactor

Stud. in Surface Science and Catalysis 107/,547 1997年
Hydrogen-Permselective Membrane Reactors

CaTTech. 1/,67 1997年
YBa2Cu3Ox as an electroconductive catalyst for combustion of carbon monoxide

E. Kikuchi, M. Hondo

Catalysis Today 29 ( 1-4 ) 409 - 414 1996年05月

　概要を見る

YBa2Cu3Ox, known as a high-Tc superconductor, was used as an electroconductive catalyst and its characteristics in CO oxidation were investigated. Charging 3 V, direct current, heated YBa2Cu3Ox up to about 500°C, at which it could catalyze CO oxidation. Thus, this oxide has proper features required for electrically temperature-controlled combustion catalysts: one is self-heating property caused by electric current (Joule's heat) and the other is catalytic activity for combustion. The catalytic activity of YBa2Cu3Ox was greatly affected by the oxygen deficiency in the solid which was directly related to the partial pressure of oxygen in the reaction system.

DOI
YBa2Cu3Ox as an electroconductive catalyst for combustion of carbon monoxide

E. Kikuchi, M. Hondo

Catalysis Today 29 ( 1-4 ) 409 - 414 1996年05月

　概要を見る

YBa2Cu3Ox, known as a high-Tc superconductor, was used as an electroconductive catalyst and its characteristics in CO oxidation were investigated. Charging 3 V, direct current, heated YBa2Cu3Ox up to about 500°C, at which it could catalyze CO oxidation. Thus, this oxide has proper features required for electrically temperature-controlled combustion catalysts: one is self-heating property caused by electric current (Joule's heat) and the other is catalytic activity for combustion. The catalytic activity of YBa2Cu3Ox was greatly affected by the oxygen deficiency in the solid which was directly related to the partial pressure of oxygen in the reaction system.

DOI
Shape Selective Alkylation of Biphenyl with Propene on SAPO-11 Catalysts

Appl.Catal. A136/,19 1996年

DOI
Shape Selective Alkylation of Biphenyl with Propene on SAPO-11 Catalysts

Appl.Catal. A136 1996年

DOI
Shape Selective Alkylation of Biphenyl with Propene on SAPO-11 Catalysts

Appl. Catal./Elsevier A136 1996年

DOI
"Reduction of Nitric Oxide with Methane on Pd/Co/H-ZSM-5 Catalysts : Cooperative effects of Pd and Co"

Catal. Lett. 42/,185 1996年
Reduction of Nitric Oxide with Methane on Pd/Co/H-ZSM-5 Catalysts: Cooperative Effects of Pd and Co

Catal. Lett. 42 1996年
Steam Reforming and Related Reactions in Hydrogen-permselective Membrane Reactor

Sekiyu Gakkaishi 39;5 1996年

DOI
YBa₂Cu₃Ox as an Electroconductive Catalyst for Combustion of Carbon Monoxide

Catal Today 29/,409-14 1996年

DOI
YBa2Cu3Ox as an Electroconductive Catalyst for Combustion of Carbon Monoxide

Catalysis Today/Elsevier 29 1996年

DOI
YBa2Cu3Ox as an Electroconductive Catalyst for Combustion of Carbon Monoxide

Catal. Today 29 1996年

DOI
Promotive Effect of Additives to In/H-ZSM-5 Catalyst Selectibe Reduction of Nitric Oxide with Methane in the Presence of Water Vapor

Catalysis today 27/,35 1996年

DOI
Promotive Effect of Additives to In/H-ZSM-5 Catalyst for Selective Reduction of Nitric Oxide with Methane in the Presence of Water Vapor

Catalysis Today /Elsevier 27 1996年

DOI
Promotive Effect of Additives to In/H-ZSM-5 Catalyst for Selective Red

Catalysis Today 27 1996年

DOI
Selective Reduction of Nitric Oxide with Methane on Gallium and Indium Containing H-ZSM-5 Catalysts : Formation of Active Sites by Solid State Ion Exchange

J.Catal. 161/,465-470 1996年

DOI
Selective Reduction of Nitric Oxide with Methane on H-ZSM-5 Catalysts

Containing Gallium or Indium: Formation of Active Sites by Solid State Ion Exchange,J. Catal. 161 1996年
Precious Metal Loaded In/H-ZSM-5 for Reduction of Nitric Oxide with Methane in the Presence of Water Vapor

Stud.in Surface Sci.and Catal 110/,671 1996年
Formation of Active Sites for Reduction of NO₂ with Methane by Solid State Exchange of In₂O₃ into H-Zeolites"

Stud. in Surface Science and Catalysis 105/,1593 1996年
Formation of Active Sites for Reduction of NO2 with Methane by Solid State Exchange of In2O3 into H-Zeolites

Stud. in Surface Science and Catalysi 105 1996年
Precious Metal Loaded In/H-ZSM-5 for Reduction of Nitric Oxide with Me thane in the Presence of Water Vapor

Stud. in Surface Science and Catalysis 101 1996年
Ir/In/H-ZSM-5触媒上でのメタンによるNO選択還元反応

触媒 *38;6 1996年
壮年期の学会への期待

ペトロテック 19;5 1996年
Shape Selective Alkylation of Biphenyl with Propene on SAPO-11 Catalysts

Appl.Catal. A136/,19 1996年

DOI
Shape Selective Alkylation of Biphenyl with Propene on SAPO-11 Catalysts

Appl.Catal. A136 1996年

DOI
Shape Selective Alkylation of Biphenyl with Propene on SAPO-11 Catalysts

Appl. Catal./Elsevier A136 1996年

DOI
"Reduction of Nitric Oxide with Methane on Pd/Co/H-ZSM-5 Catalysts : Cooperative effects of Pd and Co"

Catal. Lett. 42/,185 1996年
Reduction of Nitric Oxide with Methane on Pd/Co/H-ZSM-5 Catalysts: Cooperative Effects of Pd and Co

Catal. Lett. 42 1996年
Steam reforming and related reactions in hydrogen-permselective membrane reactor

Eiichi Kikuchi

Sekiyu Gakkaishi (Journal of the Japan Petroleum Institute) 39 ( 5 ) 301 - 313 1996年

　概要を見る

Selective and efficient permeation of H2 was accomplished by a thin Pd or Pd-Ag alloy membrane supported on porous alumina ceramics. Such membranes were prepared by deposition of Pd or Pd and Ag on the outer surface of the support cylinder by an electroless plating technique. It was found that either steam or CO2 reforming of CH4 was promoted beyond equilibrium by use of a membrane reactor with the Pd/ceramic composite membrane at temperatures as low as 773 K. In spite of a similar type of reforming, a quite different pattern of reaction products was obtained in the membrane reactor: H2 and CO2 from steam reforming, and H2 and CO (syngas) from CO2 reforming. Nickel catalyzed carbon-free steam reforming, and the level of CH4 conversion depended on the efficiency of the membrane for H2 permeation since the rate of H2 production was sufficiently higher than that of H2 permeation. On the contrary, carbon deposition extensively took place in CO2 reforming on Ni catalyst, while alumina-supported noble metals showed far less selectivities for carbon deposition than did Ni even in the membrane reactor. Differing from the activity sequence observed in the conventional reaction system, it was found in membrane reactor that it decreased in the order: Rh∼Pt&gt
Pd&gt
Ru&gt
Ir, due to contamination of the active surface. Among the noble metal catalysts tested, Pt supported on Al2O3-La2O3 and Al2O3-CeO2 was effective without significant carbon deposition to enable prolonged activity. The membrane reactor can provide a partial oxidation process with utilization of air instead of pure O2 to produce H2 or syngas.

DOI
YBa₂Cu₃Ox as an Electroconductive Catalyst for Combustion of Carbon Monoxide

Catal Today 29/,409-14 1996年

DOI
Promotive Effect of Additives to In/H-ZSM-5 Catalyst Selectibe Reduction of Nitric Oxide with Methane in the Presence of Water Vapor

Catalysis today 27/,35 1996年

DOI
Promotive Effect of Additives to In/H-ZSM-5 Catalyst for Selective Reduction of Nitric Oxide with Methane in the Presence of Water Vapor

Catalysis Today /Elsevier 27 1996年

DOI
Promotive Effect of Additives to In/H-ZSM-5 Catalyst for Selective Red

Catalysis Today 27 1996年

DOI
Selective Reduction of Nitric Oxide with Methane on Gallium and Indium Containing H-ZSM-5 Catalysts : Formation of Active Sites by Solid State Ion Exchange

J.Catal. 161/,465-470 1996年

DOI
Selective Reduction of Nitric Oxide with Methane on H-ZSM-5 Catalysts

Containing Gallium or Indium: Formation of Active Sites by Solid State Ion Exchange,J. Catal. 161 1996年
Precious Metal Loaded In/H-ZSM-5 for Reduction of Nitric Oxide with Methane in the Presence of Water Vapor

Stud.in Surface Sci.and Catal 110/,671 1996年
Formation of Active Sites for Reduction of NO₂ with Methane by Solid State Exchange of In₂O₃ into H-Zeolites"

Stud. in Surface Science and Catalysis 105/,1593 1996年
Formation of Active Sites for Reduction of NO2 with Methane by Solid State Exchange of In2O3 into H-Zeolites

Stud. in Surface Science and Catalysi 105 1996年
Precious Metal Loaded In/H-ZSM-5 for Reduction of Nitric Oxide with Me thane in the Presence of Water Vapor

Stud. in Surface Science and Catalysis 101 1996年
Palladium/ceramic membranes for selective hydrogen permeation and their application to membrane reactor

Eiichi Kikuchi

Catalysis Today 25 ( 3-4 ) 333 - 337 1995年08月

　概要を見る

Plating thin Pd or Pd-Ag alloy film on the outer surface of a porous alumina ceramic tube enables very rapid hydrogen permeation with an absolute selectivity based on the solution-diffusion transport mechanism. Effectiveness, such as displacement of thermodynamic equilibrium, selectivity enhancement, is brought forth by incorporating the metal/ceramic composite membrane in the catalytic reactor, as demonstrated in concrete examples of steam and CO2 reforming of methane and dehydrogenation of isobutane. It is also shown that the membrane reactor occasionally requires its own catalyst which is different from conventional ones. © 1995.

DOI
Liquid-phase methanol synthesis on Cu-based ultrafine particles prepared by chemical deposition in liquid phase

T. Matsuda, M. Shizuta, J. Yoshizawa, E. Kikuchi

Applied Catalysis A, General 125 ( 2 ) 293 - 302 1995年05月

　概要を見る

Liquid-phase methanol synthesis was investigated using copper-based ultrafine particle (UFP) catalysts. Cu{single bond}Zn UFP catalyst was active for methanol synthesis, although the activity decreased with time-on-stream. Cu{single bond}V UFP catalyst was stable against deactivation and showed the highest methanol productivity of the catalysts tested. The space time yield of methanol on this catalyst was about 3.5 times as large as that of a co-precipitated Cu{single bond}Zn catalyst. The selectivity of the Cu{single bond}V UFP catalyst for methanol was low, as compared to that of the co-precipitated Cu{single bond}Zn catalyst, due to the formation of methane. The addition of carbon dioxide in the feed gas was effective in suppressing the formation of methane. © 1995 Elsevier Science B.V. All rights reserved.

DOI
Liquid-phase methanol synthesis on Cu-based ultrafine particles prepared by chemical deposition in liquid phase

T. Matsuda, M. Shizuta, J. Yoshizawa, E. Kikuchi

Applied Catalysis A, General 125 ( 2 ) 293 - 302 1995年05月

　概要を見る

Liquid-phase methanol synthesis was investigated using copper-based ultrafine particle (UFP) catalysts. Cu{single bond}Zn UFP catalyst was active for methanol synthesis, although the activity decreased with time-on-stream. Cu{single bond}V UFP catalyst was stable against deactivation and showed the highest methanol productivity of the catalysts tested. The space time yield of methanol on this catalyst was about 3.5 times as large as that of a co-precipitated Cu{single bond}Zn catalyst. The selectivity of the Cu{single bond}V UFP catalyst for methanol was low, as compared to that of the co-precipitated Cu{single bond}Zn catalyst, due to the formation of methane. The addition of carbon dioxide in the feed gas was effective in suppressing the formation of methane. © 1995 Elsevier Science B.V. All rights reserved.

DOI
Effect of SiO₂/Al₂O₃ Ratio on the Catalytic Properties of Mordenite for Alkylation of Biphenyl with Propene

Appl.Catal. A131/,293 1995年

DOI
Effect of SiO2/Al2O3 Ratio on the Catalytic Properties of Mordenite for Alkylation of Biphenil with Propene

Appl. Catal. /Elsevier A131 1995年

DOI
Effect of SiO2/Al203 Ratio on the Catalytic Properties of Mordenite for Alkylation of Biphenil with Propene

Appl. Catal. A127/,293 1995年
Catalytic Properties of Copper-exchanged Clays for the Dehydrogenation of Methanol to Nethyl Formate

Appl.Catal. A126/,177 1995年

DOI
Catalytic Properties of Copper-exchanged Clays for the Dehydrogenation of Methanol to Methyl Formate

Appl. Catal. /Elsevier A126 1995年

DOI
Liquid-phase Methanol Synthesis on Cu-based Ultrafine Particles Prepared by Chemical Deposition in the Liquid Phase

Appl. Catal./Elsevier A125;2 1995年
Liquid-phase Methanol Synthesis on Cu-based Ultrafine Particles Prepared by Chemical Deposition in the Liquid Phase

Appl. Catal. A125/,293 1995年

DOI
Liquid-phase Methanol Synthesis on Cu-based Ultrafine Particles Perpared by Chemical Deposition in the Liquid Phase

Appl.Catal. A125/,293 1995年

DOI
Mechanism of Selective Catalytic Reduction of NO by Propene on Fe Silicate in Oxygen-rich atmosphere A Transient Response Study

ACS Symposium Series 587/,123 1995年
Mechanism of Selective Catalytic Reduction of NO by Propene on Fe Silicate in Oxygen-rich Atmosphere: A Transient Response Study

ACS Symposium Series/アメリカ化学会 587 1995年
Effects of Cr Addition on the Catalytic Properties of Ultrafine Particles of Co for Liquid Phase Fischer-Tropsch Synthesis

Sekiyu Gakkaishi /石油学会 38;5 1995年
Palladium/Ceramic Membranes for Selective Hydrogen Permeationand their Application to Membrane Reactor

Catalysis Today/Elsevier 25;3,4 1995年

DOI
palladium/Ceramic Membranes for Selectibe Hydrogen Permeation and their Application to Membrane Reactor

Catalysis Today 25/,333 1995年

DOI
Precious Metal Load In/H-ZSM-5 for Low Concentration No Reduction with Methane in the Presence of Water Vapor

Cem.Lett. 1995/,1135 1995年
Precious Metal Loaded In/H-ZSM-5 for Low Concentration NO Reduction with Methane in the Presence of Water Vapor

Chem. Lett./日本化学会 1995 1995年

DOI
Effect of Spiltover Hydrogen on Stabilization of Catalytic Activities of Y-type zeolite and Pillared Montmorillonite for Disproportionation of 1,2,4-Trimethylbenzene

J. Catal. 154/,41 1995年

DOI
Effect of Spiltover Hydrogen on Stabilization of Catalytic Activities of Y-type zeolite and Pillared Montmorillonite for Disproportionation of 1,2,4-Trimethylbenzene

J. Catal. /Academic Press 154 1995年

DOI
Alkylation of Biphenyl with Propene on HNa Mordenite

Appl. Catal. 123/,205 1995年

DOI
窒素酸化物除去触媒

化学工業/化学工業社 46;12 1995年
液相FT合成用コバルト超微粒子触媒に対するクロムの添加効果

石油学会誌 38/, 1995年
水素透過膜を用いた触媒反応

触媒/触媒学会 37;5 1995年
ゼオライトを用いたNOx選択還元反応

ゼオライト/ゼオライト研究会 12;4 1995年

DOI
Effect of SiO₂/Al₂O₃ Ratio on the Catalytic Properties of Mordenite for Alkylation of Biphenyl with Propene

Appl.Catal. A131/,293 1995年

DOI
Effect of SiO2/Al2O3 Ratio on the Catalytic Properties of Mordenite for Alkylation of Biphenil with Propene

Appl. Catal. /Elsevier A131 1995年

DOI
Effect of SiO2/Al203 Ratio on the Catalytic Properties of Mordenite for Alkylation of Biphenil with Propene

Appl. Catal. A127/,293 1995年
Catalytic Properties of Copper-exchanged Clays for the Dehydrogenation of Methanol to Nethyl Formate

Appl.Catal. A126/,177 1995年

DOI
Catalytic Properties of Copper-exchanged Clays for the Dehydrogenation of Methanol to Methyl Formate

Appl. Catal. /Elsevier A126 1995年

DOI
Liquid-phase Methanol Synthesis on Cu-based Ultrafine Particles Prepared by Chemical Deposition in the Liquid Phase

Appl. Catal./Elsevier A125;2 1995年
Mechanism of Selective Catalytic Reduction of NO by Propene on Fe Silicate in Oxygen-rich atmosphere A Transient Response Study

ACS Symposium Series 587/,123 1995年
Mechanism of Selective Catalytic Reduction of NO by Propene on Fe Silicate in Oxygen-rich Atmosphere: A Transient Response Study

ACS Symposium Series/アメリカ化学会 587 1995年
Effects of Cr Addition on the Catalytic Properties of Ultrafine Particles of Co for Liquid Phase Fischer-Tropsch Synthesis

Sekiyu Gakkaishi /石油学会 38;5 1995年
Palladium/Ceramic Membranes for Selective Hydrogen Permeationand their Application to Membrane Reactor

Catalysis Today/Elsevier 25;3,4 1995年

DOI
Precious Metal Load In/H-ZSM-5 for Low Concentration No Reduction with Methane in the Presence of Water Vapor

Cem.Lett. 1995/,1135 1995年
Precious Metal Loaded In/H-ZSM-5 for Low Concentration NO Reduction with Methane in the Presence of Water Vapor

Chem. Lett./日本化学会 1995 1995年

DOI
Effect of Spiltover Hydrogen on Stabilization of Catalytic Activities of Y-type zeolite and Pillared Montmorillonite for Disproportionation of 1,2,4-Trimethylbenzene

J. Catal. 154/,41 1995年

DOI
Effect of Spiltover Hydrogen on Stabilization of Catalytic Activities of Y-type zeolite and Pillared Montmorillonite for Disproportionation of 1,2,4-Trimethylbenzene

J. Catal. /Academic Press 154 1995年

DOI
Alkylation of Biphenyl with Propene on HNa Mordenite

Appl. Catal. 123/,205 1995年

DOI
Selective catalytic reduction of nitrogen monoxide by methane on zeolite catalysts in an oxygen-rich atmosphere

Eiichi Kikuchi, Katsunori Yogo

Catalysis Today 22 ( 1 ) 73 - 86 1994年12月

　概要を見る

Selective reduction of NO by CH4 on zeolite catalysts has been studied. After an investigation of the catalytic features of various cation-exchanged zeolites, we found that Ga-ZSM-5 and In-ZSM-5 were highly active and selective for NO reduction by CH4. We also showed that this reaction was moderately promoted even by H-form ZSM-5, mordenite, and ferrierite. From the catalytic performance of Ga-and In-ZSM-5 in NO-CH4-O2, NO2-CH4-O2, and NO-O2 reactions, it is concluded that the selective reduction of NO on these catalysts proceeds in two stages: (1) NO is oxidized to NO2 on zeolite acid sites, (2) NO2 and CH4 react on gallium or indium sites. The highly selective features of Ga and In in the zeolite for the NO2-CH4 reaction seem to be attributed to the coordinatively unsaturated nature of these sites which adsorb both of these reactants on the same site. Effect of water vapor on NO conversion was also investigated. It was found that Ga-ZSM-5 was strongly inhibited by steam, while In-ZSM-5 was fairly active even in the presence of 10% steam. © 1994.

DOI
Reaction Mechanism of Selective Reduction of Nitric Oxide by Methane on Ga-and In-ZSM-5 Catalysts

Studies. in Surface Science and Catalysis 84/,1547 1994年
Selective Synthesis of 4,4'-Diisopropylbiphenyl Using Mordenite Catalysts

Stub. in Surface Science and Catalysis 83/,295 1994年
Characterization of Fe-silicates and their Catalytic Properties for the Selective Reduction of Nitric Oxide by Hydrocarbons

Microporous Materials 3/,39 1994年

DOI
Selective Catalytic Reduction of Nitrogen Monoxide by Methane on Zeolite Catalysts in Oxygen-rich Atmosphere

Catalysis Today 22/,73 1994年

DOI
Catalytic Combustion of Carbon Monoxide over YBa₂Cu₃Ox Electroconductive Catalyst

Chem. Lett. /,2207 1994年

DOI
GaおよびInイオン交換ゼオライト上でのメタンによるNOの選択還元反応機構

触媒 36 1994年
Reaction Mechanism of Selective Reduction of Nitric Oxide by Methane on Ga-and In-ZSM-5 Catalysts

Studies. in Surface Science and Catalysis 84/,1547 1994年
Selective Synthesis of 4,4'-Diisopropylbiphenyl Using Mordenite Catalysts

Stub. in Surface Science and Catalysis 83/,295 1994年
Characterization of Fe-silicates and their Catalytic Properties for the Selective Reduction of Nitric Oxide by Hydrocarbons

Microporous Materials 3/,39 1994年

DOI
Catalytic Combustion of Carbon Monoxide over YBa₂Cu₃Ox Electroconductive Catalyst

Chem. Lett. /,2207 1994年

DOI
Synthesis of symmetrical alkyl-aromatics by use of shape selective catalysts

T. Matsuda, E. Kikuchi

Research on Chemical Intermediates 19 ( 4 ) 319 - 332 1993年12月

　概要を見る

The concept of shape selectivity is available to produce symmetrical dinuclear aromatic hydrocarbons such as 2,6-dialkylnaphthalene and 4,4′-dialkylbiphenyl, which are the raw materials for liquid crystals and polyester with superior properties, respectively. The ZSM-5 catalyst exhibits high activity and selectivity for the formation of p-xylene in the disproportionation and alkylation of toluene. The catalytic activity of ZSM-5 for the conversion of naphthalene derivatives is markedly low due to its small pore size, although symmetrical dinuclear aromatic hydrocarbons are selectively formed. The high catalytic activity is obtained with twelve-membered ring zeolites. Among these zeolites, mordenite is the most selective catalyst to produce symmetrical dinuclear aromatic hydrocarbons. The precise controls of the size of pore opening and the acidic property are required to enhance the selectivity for symmetrical dinuclear aromatic hydrocarbons. The non-zeolitic molecular sieves also present a great opportunity in high selective synthesis of these compounds. © 1993 VSP.

DOI
Synthesis of symmetrical alkyl-aromatics by use of shape selective catalysts

T. Matsuda, E. Kikuchi

Research on Chemical Intermediates 19 ( 4 ) 319 - 332 1993年12月

　概要を見る

The concept of shape selectivity is available to produce symmetrical dinuclear aromatic hydrocarbons such as 2,6-dialkylnaphthalene and 4,4′-dialkylbiphenyl, which are the raw materials for liquid crystals and polyester with superior properties, respectively. The ZSM-5 catalyst exhibits high activity and selectivity for the formation of p-xylene in the disproportionation and alkylation of toluene. The catalytic activity of ZSM-5 for the conversion of naphthalene derivatives is markedly low due to its small pore size, although symmetrical dinuclear aromatic hydrocarbons are selectively formed. The high catalytic activity is obtained with twelve-membered ring zeolites. Among these zeolites, mordenite is the most selective catalyst to produce symmetrical dinuclear aromatic hydrocarbons. The precise controls of the size of pore opening and the acidic property are required to enhance the selectivity for symmetrical dinuclear aromatic hydrocarbons. The non-zeolitic molecular sieves also present a great opportunity in high selective synthesis of these compounds. © 1993 VSP.

DOI
Selective Catalytic Reduction of Nitric Oxide with Ethene on Gallium Ion Exchanged ZSM-5 under Oxygen Rich

Appl. Catal. Elsevier B2 1993年

DOI
Catalytic Properties and Crystalline Structures of Manganese Promoted Iron Ultrafine Particles for Liquid Phase Hydrogenation of Carbon Monoxide

Appl. Catal. Elsevier A96 1993年

DOI
The Effect of Spillover Hydrogen on Coke Formation Catalyzed by HY Zeolite and Pillared Montmorillonite

Stud. in Surf Sci. and Catal. Elsevier 77 1993年
Liquid Phase Hydrogenation of Carbon Monoxide Using Ultrafine Particles of Cobalt as Catalyst

Sekiyu Gakkaishi 36-5 1993年
Selective Reduction of Nitric Oxide by Methane on H-form Zeolite Catalysts in Oxygen-rich Atmosphere

Catal. Lett. 19 1993年

DOI
ゼオライト触媒上でのメタンによるNO選択還元

触媒 35 1993年
Selective Catalytic Reduction of Nitric Oxide with Ethene on Gallium Ion Exchanged ZSM-5 under Oxygen Rich

Appl. Catal. Elsevier B2 1993年

DOI
Catalytic Properties and Crystalline Structures of Manganese Promoted Iron Ultrafine Particles for Liquid Phase Hydrogenation of Carbon Monoxide

Appl. Catal. Elsevier A96 1993年

DOI
The Effect of Spillover Hydrogen on Coke Formation Catalyzed by HY Zeolite and Pillared Montmorillonite

Stud. in Surf Sci. and Catal. Elsevier 77 1993年
Liquid Phase Hydrogenation of Carbon Monoxide Using Ultrafine Particles of Cobalt as Catalyst

Sekiyu Gakkaishi 36-5 1993年
Selective Reduction of Nitric Oxide by Methane on H-form Zeolite Catalysts in Oxygen-rich Atmosphere

Catal. Lett. 19 1993年

DOI
Migration of Alkali and Alkaline Earth Elements into Carbon Black

Fuel 71 1992年

DOI
A New Classification of Alkali and Alkaline Earth Catalysts for Gasification of Carbon

Fuel 1992年

DOI
Migration of Alkali and Alkaline Earth Elements into Carbon Black

Fuel 71 1992年

DOI
A New Classification of Alkali and Alkaline Earth Catalysts for Gasification of Carbon

Fuel 1992年

DOI
Liquid Phase Fischer-Tropsch Synthesis on Ultrafine Particles of Iron : Effect of Preoxidation Treatment

Ａｐｐｌ．Ｃａｔａl． 77 1991年

DOI
Liquid Phase Fischer-Tropsch Synthesis on Manganese-Promoted Ultrafine Particles of Iron as a Catalyst

Applied Catalysis 77 1991年
Promotion of the Conversion of Propane to Aromatics by Use of Palladium Membrane Reactor

Applied Catalysis 76 1991年

DOI
Steam Reforming of Methane in a Hydrogen-permeating Membrane Reactor

Applied Catalysis 67 1991年

DOI
Separation of Hydrogen through Palladium Thin Film Supported on a Porous Glass Tube

J. Membrane Science 56 1991年

DOI
Hydrogen Permeable Palladium-Silver Alloy Membrane Supported on Porous Ceramics

J. Membrane Science 56 1991年

DOI
The Water Gas Shift Reaction Assisted by Palladium Membrane Reactor

Ind. Eng. Chem. Res 30 1991年

DOI
Selective Reduction of NO with Propene on Fe-silicate Catalysts

Chemistry Letters 1991 1991年

DOI
Liquid Phase Fischer-Tropsch Synthesis on Ultrafine Particles of Iron : Effect of Preoxidation Treatment

Ａｐｐｌ．Ｃａｔａl． 77 1991年

DOI
Liquid Phase Fischer-Tropsch Synthesis on Manganese-Promoted Ultrafine Particles of Iron as a Catalyst

Applied Catalysis 77 1991年
Promotion of the Conversion of Propane to Aromatics by Use of Palladium Membrane Reactor

Applied Catalysis 76 1991年

DOI
Steam Reforming of Methane in a Hydrogen-permeating Membrane Reactor

Applied Catalysis 67 1991年

DOI
Separation of Hydrogen through Palladium Thin Film Supported on a Porous Glass Tube

J. Membrane Science 56 1991年

DOI
Hydrogen Permeable Palladium-Silver Alloy Membrane Supported on Porous Ceramics

J. Membrane Science 56 1991年

DOI
The Water Gas Shift Reaction Assisted by Palladium Membrane Reactor

Ind. Eng. Chem. Res 30 1991年

DOI
Selective Reduction of NO with Propene on Fe-silicate Catalysts

Chemistry Letters 1991 1991年

DOI
Liquid Phase Hydrogenatun of Carbon Monoxide over Potassium-promoted Ultrafine Particles of Iron and Copper

Applied Catalysis 67 1990年

DOI
Auger Electron Spectroscopy and Electron Probe Microanalysis Observations of Barium and Calcium Located on Amorphous Carbon under Gasification Conditions

Energy and Fuels 1990 1990年

DOI
Liquid Phase Hydrogenatun of Carbon Monoxide over Potassium-promoted Ultrafine Particles of Iron and Copper

Applied Catalysis 67 1990年

DOI
Auger Electron Spectroscopy and Electron Probe Microanalysis Observations of Barium and Calcium Located on Amorphous Carbon under Gasification Conditions

Energy and Fuels 1990 1990年

DOI
Novel Catalyst for Liquid-Phase Fischer-Tropsch Synthesis : Potassium-promoted Copper-Iron Ultrafine Particles Prepared by Liquid-phase Chemical Deposition

Applied Catalysis 47 1989年

DOI
Quantitative Behavior of Potassium Species on an Amorphous Carbon under Steam Gasification Conditions

Energy and Fuels 1989 1989年

DOI
Novel Catalyst for Liquid-Phase Fischer-Tropsch Synthesis : Potassium-promoted Copper-Iron Ultrafine Particles Prepared by Liquid-phase Chemical Deposition

Applied Catalysis 47 1989年

DOI
Quantitative Behavior of Potassium Species on an Amorphous Carbon under Steam Gasification Conditions

Energy and Fuels 1989 1989年

DOI
Physical and Catalytic Properties of Smectite Clays Pillared by Alumina in Disproportionation of 1,2,4-Trimethylbenzene

Applied Catalysis 45 1988年

DOI
Hexane-Carbon Dioxide Reaction Catalyzed by Alkaline Earth Metal Oxides II Reaction Network

Ａｐｐｌ. Catal. 41 1988年

DOI
Properties and Product Selectivities of Iron Ultrafine Particles as a Catalyst for Liquid Phase Hydrogenation of Carbon Monoxide

Applied Catalysis 40 1988年

DOI
Effect of High-Temperature Treatment on the Activity of Montmorillonite Pillared by Alumina in the Conversion of 1,2,4-Trimethylbenzene

Applied Catalysis 38 1988年

DOI
Hexane-Carbon Dioxide Reaction Catalyzed by Alkaline Earth Oxides I. Catalytic Behavior and Intermediate

Applied Catalysis 37 1988年

DOI
Shape selective acid catalysis by pillared clays

E. Kikuchi, T. Matsuda

Catalysis Today 2 ( 2-3 ) 297 - 307 1988年

DOI
Interaction between Potassium Carbonate and Carbon Substrate at Sub-gasification Temperatures

Energy and Fuels 1988 1988年
Physical and Catalytic Properties of Smectite Clays Pillared by Alumina in Disproportionation of 1,2,4-Trimethylbenzene

Applied Catalysis 45 1988年

DOI
Hexane-Carbon Dioxide Reaction Catalyzed by Alkaline Earth Metal Oxides II Reaction Network

Ａｐｐｌ. Catal. 41 1988年

DOI
Properties and Product Selectivities of Iron Ultrafine Particles as a Catalyst for Liquid Phase Hydrogenation of Carbon Monoxide

Applied Catalysis 40 1988年

DOI
Effect of High-Temperature Treatment on the Activity of Montmorillonite Pillared by Alumina in the Conversion of 1,2,4-Trimethylbenzene

Applied Catalysis 38 1988年

DOI
Hexane-Carbon Dioxide Reaction Catalyzed by Alkaline Earth Oxides I. Catalytic Behavior and Intermediate

Applied Catalysis 37 1988年

DOI
Shape selective acid catalysis by pillared clays

E. Kikuchi, T. Matsuda

Catalysis Today 2 ( 2-3 ) 297 - 307 1988年

DOI
Interaction between Potassium Carbonate and Carbon Substrate at Sub-gasification Temperatures

Energy and Fuels 1988 1988年
The Effect of Spilled-over Hydrogen on the Activity of Montmorillonite Pillared by Aluminum Oxide for Conversion of Trimethylbenzenes

J. Catalysis 106 1987年

DOI
The Effect of Spilled-over Hydrogen on the Activity of Montmorillonite Pillared by Aluminum Oxide for Conversion of Trimethylbenzenes

J. Catalysis 106 1987年

DOI
Reaction of 1,2,4-Trimethylbenzene and Methanol on Montmorillonite Catalysts Pillared by Aluminium Hydroxyl Complexes

Applied Catalysis 21 1986年

DOI
Reaction of 1,2,4-Trimethylbenzene and Methanol on Montmorillonite Catalysts Pillared by Aluminium Hydroxyl Complexes

Applied Catalysis 21 1986年

DOI
Conversion of Trimethylbenzenes over Montmorillonites Pillared by Aluminium and Zirconium Oxides

Applied Catalysis 16 1985年

DOI
Conversion of Trimethylbenzenes over Montmorillonites Pillared by Aluminium and Zirconium Oxides

Applied Catalysis 16 1985年

DOI
Fischer-Tropsch Synthesis over Titania-supported Ruthenium Catalysts

Applied Catalysis 10 1984年

DOI
Fischer-Tropsch Synthesis over Titania-supported Ruthenium Catalysts

Applied Catalysis 10 1984年

DOI
Fischer-Tropsch Synthesis of Hydrocarbons on V₂O₃-supported Ruthenium Catalysts

Applied Catalysis 7 1983年

DOI
Supported Alkali Catalysts for Steam Gasification of Carbonaceous Residues from Petroleum

Fuel 62 1983年

DOI
Fischer-Tropsch Synthesis of Hydrocarbons on V₂O₃-supported Ruthenium Catalysts

Applied Catalysis 7 1983年

DOI
Supported Alkali Catalysts for Steam Gasification of Carbonaceous Residues from Petroleum

Fuel 62 1983年

DOI
The Location of Catalytic Iron in Reduced Graphite Ferric Chloride

J. Catalysis 62 1980年

DOI
The Location of Catalytic Iron in Reduced Graphite Ferric Chloride

J. Catalysis 62 1980年

DOI
Catalytic Synthesis of Hydrocarbons from Carbon Monoxide and Hydrogen on Lamellar Compound of Graphite Interealated by Ferric Chloride

J. Catalysis 57 1979年

DOI
Catalytic Synthesis of Hydrocarbons from Carbon Monoxide and Hydrogen on Lamellar Compound of Graphite Interealated by Ferric Chloride

J. Catalysis 57 1979年

DOI
The Reaction of n-Heptane on Rhodium Catalysts in the Presence of Steam

J. Catalysis 46 1977年

DOI
The Reaction of n-Heptane on Rhodium Catalysts in the Presence of Steam

J. Catalysis 46 1977年

DOI
Studies of the Enhancement of Hydrogen Adsorption during H₂-O₂ Titration on Supported Pt Catalysts

J. Catalysis 34 1974年

DOI
Studies of the Enhancement of Hydrogen Adsorption during H₂-O₂ Titration on Supported Pt Catalysts

J. Catalysis 34 1974年

DOI
Hydrogenolysis and Isomerization of n-Pentane on Group VIII Transition Metals

J. Catalysis 22 1971年
Hydrogenolysis and Isomerization of n-Pentane on Group VIII Transition Metals

J. Catalysis 22 1971年
Hydrogenolysis of n-Pentane on Nickel Catalyst

J. Catalysis 15 1969年
Hydrogenolysis of n-Pentane on Nickel Catalyst

J. Catalysis 15 1969年

▼全件表示

特定課題制度（学内資金）

ＣＯ変成用新規ペロブスカイト型酸化物触媒の開発

2006年

　概要を見る

燃料電池用の水素製造においては、改質ガス中のCO除去プロセス（COシフト反応→CO選択酸化）が必要不可欠となっており，現在のPt電極性能では10 ppm以下へのCO濃度低減が要求される．COシフト反応には工業的にCu-Zn系酸化物触媒が用いられているが，PEFC特有のDSS（デイリースタートアップ＆シャットダウン）運転では，酸化雰囲気に弱い従来のCu-Zn系酸化物触媒の使用は困難とされており，酸化雰囲気に強く，低温，高空間速度で高活性な新規触媒の開発が求められている．本研究では高い酸素イオン伝導性を有するペロブスカイト型酸化物に注目し，これを触媒担体として用いて，低温での水性ガスシフト反応を検討した．触媒の格子酸素が反応に寄与するRedox機構で進行させることができるのなら，DSSでの酸化に強い触媒系となることが期待される．さらにPt, Pdなどの活性金属を担持することで格子酸素の再生・放出を促進し，Redox領域の低温化を図り，検討を行った．その結果、Pt, PdとLaCoO3を組み合わせた触媒を用いた場合、Pt/LaCoO3とPd/LaCoO3は高いシフト活性を示した．活性が低い触媒の反応前後の結晶構造はほとんど変化していないのに対し，高活性を示したPt/LaCoO3, Pd/LaCoO3についてはLaCoO3に起因するピークが低角度側にシフトし，ブロードとなる変化がみられた．これは反応中に格子酸素が放出され，ペロブスカイト型構造が歪んでしまったためと考えられる．また，Air処理による検討から，活性低下の原因と反応中での結晶構造の変化には相関がないと考えられる．XPS測定により，Pt, Pdの電子状態を解析した．その結果，Pt/LaCoO3ではPt2+-2がシフト反応に大きく寄与していることがわかり，活性低下の原因はPt2+-2が反応中に還元されるためと考えられた．また，Pd/LaCoO3ではPd種がRedoxしており，安定した活性種となっていることが示唆された．これを受けて，安定なRedoxサイクルを進行するPd種がPt種の還元を抑制するようなシナジー効果を期待し，Pt-Pd/LaCoO3触媒を検討したところ，1 wt%Pt-0.5 wt%Pd/LaCoO3は商用触媒の活性を上回る高活性触媒となった．
非Ｌａｎｇｕｍｕｉｒ－Ｈｉｎｓｈｅｌｗｏｏｄ機構により進行する新規水素製造用触媒

2006年

　概要を見る

メタン水蒸気改質反応用Ni触媒としてペロブスカイト型酸化物を適用することで、工業的に用いられるアルミナなどの担体とした場合と比較し、高い耐炭素析出安定性が得られることが見出されている。これは担体中の格子酸素が反応に関与し、メタンがNi上に解離吸着して生成したCHXの酸化及び析出炭素前駆体の酸化除去を促進したためと考えられる。本研究では、H218Oを用いた過渡応答解析により、格子酸素が反応に関与するメカニズムの実証、また、格子酸素の挙動に影響する因子の検討を目的とした。実験では、ペロブスカイト担体として錯体重合法にて調製したLaAlO3, SrTiO3を用いた。これらペロブスカイトにニッケルを担持し触媒とした。反応における過渡応答解析は固定床常圧流通式反応器を用いた。反応は、あらかじめ水素気流で還元した触媒を用いて、反応温度1073 K,で行った。Heで60分間パージした後、CH4/H216O/Ar/He を60分間供給し、CH4/H218O/Ar/Heに切り替えて5分間保持し後、再びCH4/H216O/Ar/Heに切り替え、そのときの過渡応答を四重極形質量分析装置（QMS、HYDEN HAL201）により解析した。　格子酸素によるCH4酸化実験より、触媒活性と、格子酸素によるCHXの酸化速度との間に相関あることが示唆された。また、H2Oからの格子酸素補充の検討を行ったところ、格子酸素の補充には担持金属が大きく影響しており、担持金属が酸化された状態では格子酸素の補充が行われないと考えられる。そして、H218Oを用いた過渡応答解析より、ペロブスカイト担体の格子酸素が反応に関与することが明らかになった。反応温度が高いほど反応に関与する格子酸素量は多いと考えられ、またCHXの酸化により関与すると考えられる。最後に、格子酸素の反応には金属－担体界面が大きく関わっており、Ni粒子径が小さいほど、反応に関与する格子酸素量が多くなることがわかった。