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Research
1. Catalytic Cracking of Cellulose
Our aim is to synthesize sugar compounds by catalytic cracking of renewable biomass. Then we will convert the sugars into fuels and chemicals (Fig. 1). Cellulose is the most abundant organic compound in nature, but the utilization of cellulose is limited because cellulose is resistant to degradation. We have succeeded in the first catalytic cracking of cellulose into sorbitol over supported metal catalysts. (Fig. 2). Catalytic conversion of sorbitol is also studied for use of sorbitol as a precursor to valuable chemicals (Fig. 3).
Recently, we found that Ru/CMK-3 is a water-tolerant and reusable catalyst for the hydrolysis of cellulose, and exhibits high glucose yields and turnover numbers due to a synergistic effect between CMK-3 and Ru. CMK-3 contributes to the conversion of cellulose into oligosaccharides, while Ru promotes the hydrolysis of oligosaccharides to glucose (Fig. 4).


Figure 1. Catalytic biomass conversion.


Figure 2. Sorbitol synthesis by catalytic cellulose cracking



Figure 3. Use of sorbitol


Figure 4. Hydrolysis of cellulose by Ru/CMK.

2. Template Synthesis and Catalysis of Metal Nanoclusters in Mesoporous Materials

Our research topic is the template synthesis and catalysis of metal nanoclusters such as particles and wires in mesoporous materials (Fig. 1). Purpose of this study is to improve the catalytic activity and selectivity by the well-dispersed nanoclusters and to develop new reactions based on the concerted effect of the support.
Recently, we found that Pt nanoparticles in mesoporous silica (Pt/FSM-16) shows high activity, selectivity and good durability in PROX of CO in excess H2. From mechanistic study by IR with isotopic tracer technique, we propose that OH groups on the internal wall of the support is highly reactive toward CO on Pt (Fig. 2). We have thus demonstrated at the molecular level that the mesoporous silica has a promotional effect in catalysis that is not observed for the conventional silica.



Figure 1. Template synthesis of Pt nano-particles and -wires in mesoporous silica.

Figure 2. Preferential oxidation (PROX) of CO in hydrogen for fuel cells.


Figure 3. PROX of CO by supported Pt catalysts.


Figure 4. Proposed mechanism for PROX図4. PROX.
 
Member 
Position  Name E-mail address  Phone
+81-11-706-
CV
Professor Dr. Atsushi Fukuoka  fukuoka (@cat.hokudai.ac.jp)  9140  CV(Fukuoka)
Associate Professor Dr. Kenji Hara  hara (@cat.hokudai.ac.jp)  9136   
Assistant Professor  Dr. Hirokazu Kobayashi  kobayashi.hi (@cat.hokudai.ac.jp  9137  CV(Kobayashi)
Program Coordinator  Dr. Reiko Sadamoto   sadamoto (@cat.hokudai.ac.jp)    9146   
Postdoctoral fellow  Dr. Bo Feng  bo-feng (@cat.hokudai.ac.jp)  9137  
Research Assistant  Mayumi Segawa  seg (@cat.hokudai.ac.jp)  9138   
Administrative Assistant  Yoko Nakaya  nakaya (@cat.hokudai.ac.jp)  9138   
Graduate Student D2  Mizuho Yabushita   m.yabushita (@mail.sci.hokudai.ac.jp)  9137   
Graduate Student M2 Nobuhiro Ishito  ishito(@sci.hokudai.ac.jp) 9136   
Graduate Student M2 Chika Iwata ck.iwt(@mail.sci.hokudai.ac.jp) 9136   
Graduate Student M2 Kotaro Namba  K-Namba(@sci.hokudai.ac.jp) 9136   
Graduate Student M2 Yoshihiko Hirosaki hikoyoshi(@mail.sci.hokudai.ac.jp) 9137  
Graduate Student M1 Hiroyuki Kaiki  kaikihiroyuki1729(@ec.hokudai.ac.jp) 9137   
Graduate Student M1  Okimune Kawabata  gari-rado3 (@ec.hokudai.ac.jp)  9136   
Graduate Student M1  Kyoichi Kuroki  igonnathrowout (@ec.hokudai.ac.jp)  9137   
Undergraduate Student B4  Kota Techikawara  butani-sinjuku-daton (@ec.hokudai.ac.jp) 9137   

Former Group Members
Fumie Okada   
Tasuku Komanoya   Postdoctoral Fellow, Tokyo Institute of Technology 
Shogo Ito  Shin-Etsu Chemical Co., Ltd. 
Dr. Hidetoshi Ohta Assistant Professor, Ehime University
Dr. Pengfei Yang  Postdoctoral Fellow, The University of Tokyo
Yuto Hosaka Foundation for Promotion of Material Science and Technology of Japan
Masaya Yamamoto 
Dr. Sachin Jagtap  Manager R&D, Sudarshan Chemical Industries Ltd., India
Dr. Samar Kumar Guha Assistant Professor, Ahsanullah University of Science & Technology, Dacca, Bangladesh 
Dr. Prabhu Azhagapillai   
Saiko Akahane  Shin-Etsu Chemical Co., Ltd.
Yoshinori Kaji   
Yukiko Ito   
Hisateru Matsuhashi  Kokumin Drug Store 
Dr. Menglian Lin  Taiwan Semiconductor Manufacturing Company
Dr. Shengjun Huang Associate Professor, Dalian Institute of Chemical Physics, Dalian, China 
Mizuho Watanabe  AIST, Hokkaido 
Dr. Tatsuo Hamada  RIES, Hokkaido Univ. 
Dr. Paresh L. Dhepe  Scientist, National Chemical Laboratory, Pune, India
Koji Kasai   
Mayumi Kondo   
Kanae Goto   
Tadashi Oshio Nippon Oil Corp. (ENEOS) 
 
Publication list 
2013
[Refereed Papers]

1. H. Kobayashi, M. Yabushita, T. Komanoya, K. Hara, I. Fujita, A. Fukuoka
High-Yielding One-Pot Synthesis of Glucose from Cellulose Using Simple Activated Carbons and Trace Hydrochloric Acid
ACS Catal., 3 (4), 581-587 (2013). DOI:10.1021/cs300845f

2. T. Komanoya, H. Kobayashi, K. Hara, W.-J. Chun, A. Fukuoka
Simultaneous formation of sorbitol and gluconic acid from cellobiose using carbon-supported ruthenium catalysts
J. Energy Chem., 22, 290-295 (2013). DOI: 10.1016/S2095-4956(13)60035-2

3. C. Jiang, K. Hara, A. Fukuoka
Low-Temperature Oxidation of Ethylene over Platinum Nanoparticles Supported on
Mesoporous Silica
Angew. Chem. Int. Ed., 52 (24), 6265-6268 (2013). DOI: 10.1002/anie.201300496

4. H. Kobayashi, A. Fukuoka
Synthesis and utilisation of sugar compounds derived from lignocellulosic biomass
Green Chemistry, 15 (7), 1740-1763 (2013)., DOI:10.1039/c3gc00060e

5. M. Yabushita, H. Kobayashi, A. Fukuoka
Catalytic transformation of cellulose into platform chemicals
Appl. Catal. B: Environmental, in press, DOI:10.1016/j.apcatb.2013.01.052


2012
[Refereed Papers]

1. Y. Masuyama, Y. Sugioka, S. Chonan, N. Suzuki, M. Fujita,  K. Hara, A. Fukuoka, “Palladium(II)-Exchanged Hydroxyapatite-Catalyzed Suzuki-Miyaura-Type Cross-Coupling Reactions with Potassium Aryltrifluoroborates”, J. Mol. Catal. A: Chemical, 352, 81-85 (2012).

2. J. M. Nduko, W. Suzuki, K. Matsumoto, H. Kobayashi, T. Ooi, A. Fukuoka, S. Taguchi, “Polyhydroxyalkanoates production from cellulose hydrolyzate in Escherichia col LS5218 with superior resistance against 5-hydroxymethylfurfural”, J. Biosci. and Bioeng., 113(1), 70-72 (2012)

3. K. Hara, S. Akahane, J. W. Wiench, B. R. Burgin, N. Ishito, V. S.-Y. Lin, A. Fukuoka and M. Pruski, “Selective and Efficient Silylation of Mesoporous Silica with Trimethylsilyltriflate: A Quantitative Assessment of Synthetic Strategies”, J. Phys. Chem. C, 116 (12), 7083-7090 (2012).

4. S. Huang, K. Hara and A. Fukuoka, “Intrinsic Catalytic Role of Mesoporous Silica in Preferential Oxidation of Carbon Monoxide in Excess Hydrogen”, Chemistry in Europe, 18 (15), 4738-4747 (2012).

5. H. Kobayashi, H. Ohta, A. Fukuoka, “Conversion of lignocellulose into renewable chemicals by heterogeneous catalysis”, Catal. Sci. Tech., 2, 869-883 (2012). DOI:10.1039/C2CY00500J.

6. P. Yang, H. Kobayashi, K. Hara, and A. Fukuoka, “Phase-change of nickel phosphide catalysts in the conversion of cellulose into sorbitol”, ChemSusChem, 5 (5), 920-926 (2012).


2011
[Refereed Papers]

1. K. Matsumoto, H. Kobayashi, K. Ikeda, T. Komanoya, A. Fukuoka, and S. Taguchi, "Chemo-microbial conversion of cellulose into polyhydroxybutyrate through ruthenium-catalyzed hydrolysis of cellulose into glucose", Bioresource Technology, 102, 3564-3567 (2011).

2. H. Kobayashi, Y. Ito, T. Komanoya, Y. Hosaka, P. L. Dhepe, K. Kasai, K. Hara, A. Fukuoka, "Synthesis of Sugar Alcohols by Hydrolytic Hydrogenation of Cellulose over Supported Metal Catalysts", Green Chem., 13 (2), 326-333 (2011).

3. H. Kobayashi, H. Matsuhashi, T. Komanoya, K. Hara, A. Fukuoka, "Transfer Hydrogenation of Cellulose to Sugar Alcohols over Supported Ruthenium Catalysts", Chem. Commun., 47 (8), 2366-2368 (2011).

4. S. K. Guha, H. Kobayashi, K. Hara, H. Kikuchi, T. Aritsuka, A. Fukuoka, “Hydrogenolysis of sugar beet fiber by supported metal catalyst”, Catal. Comm., 12, 980-983 (2011).

5. M.-L. Lin, K. Hara, Y. Okubo, M. Yanagi, H. Nambu, A. Fukuoka, “Remarkable effect of ordered mesoporous carbon support in tantalum oxide-catalyzed selective epoxidation of cyclooctene”, Catal. Comm., 12, 1228-1230 (2011).


6. . P. Yang, H. Kobayashi, A. Fukuoka, “Recent Developments in the Catalytic Conversion of Cellulose into Valuable Chemicals”, Chin. J. Catal., 32, 716-722 (2011).

7. T. Komanoya, H. Kobayashi, K. Hara, W. -J. Chun, A. Fukuoka, “Catalysis and Characterization of Carbon-Supported Ruthenium for Cellulose Hydrolysis, Appl. Catal. A: Gen., 407, 188-194 (2011).

8. H. Ohta, H. Kobayashi, K. Hara, A. Fukuoka, “Hydrodeoxygenation of Phenols as Lignin Models under Acid-Free Conditions with Carbon-Supported Platinum Catalysts”, Chem. Commun., 47, 12209-12211 (2011).

9. H. Kobayashi, T. Komanoya, S. K. Guha, K. Hara, A. Fukuoka, “Conversion of cellulose into renewable chemicals by supported metal catalysis”, Appl. Catal. A: Gen., 409-410, 13-20 (2011).

10. Y. Masuyama, K. Yoshikawa, N. Suzuki, K. Hara, A. Fukuoka, “Hydroxyapatite-supported copper(II)-catalyzed azide-alkyne [3+2] cycloaddition with neither reducing agents nor bases in water”, Tetrahedron Lett., 52, 6916-6918 (2011).

[Other Publications]
1. 小林広和、福岡淳、”木質バイオマスからの糖誘導体の合成”、PETROTECH, 34 (1), 18-23 (2011).

2. 小林広和、福岡淳、“固体触媒によるセルロースの糖化”、日本エネルギー学会誌, 90 (6), 512-517 (2011).

3. 原賢二、福岡淳、Pt/メソポーラスシリカ、触媒調製ハンドブック、岩本正和 監修、pp. 594-595, エヌ・ティー・エス出版、東京 (2011).

4. 小林広和、福岡淳、Pt/Al2O3、触媒調製ハンドブック、岩本正和 監修、pp. 632-633、エヌ・ティー・エス出版、東京 (2011).

5. 小林広和、福岡淳、固体触媒によるセルロースの糖化技術 現状と課題、バイオリファイナリー触媒技術の新展開、pp. 222-228、シーエムシー出版、東京(2011)



2010
[Refereed Papers]


1. H. Kobayashi, T. Komanoya, K. Hara and A. Fukuoka, "Water-tolerant mesoporous carbon-supported ruthenium catalyst for hydrolysis of cellulose to glucose", ChemSusChem, 3 (4), 440-443 (2010).

[Reviews]

1. 小林広和、福岡淳、“触媒によるバイオマス資源の有効利用”、未来材料10 (1), 39-43 (2010).

2. 小林広和、福岡淳、“セルロースからの糖アルコール製造”、ファインケミカル39 (6), 13-19 (2010).

3. 福岡淳、バイオマス分解(セルロース・リグニン)、レアメタル便覧、丸善、(2010).

4. S. K. Guha, H. Kobayashi and A. Fukuoka, “Conversion of Cellulose to Sugars”, in Thermochemical Conversion of Biomass to Liquid Fuels and Chemicals, Mark Crocker ed., Royal Society of Chemistry, Chapter 13, 344-364 (2010).

5. 小林広和、福岡淳、環境を護る触媒3:セルロースのグルコース化、現代界面コロイド科学の事典−シャンプーから宇宙まで−、日本化学会・コロイドおよび界面化学部会、丸善、128-129 (2010).

2009

[Refereed papers]

1. S. Kawamorita, H. Ohmiya, K. Hara, A. Fukuoka and M. Sawamura, “Directed Ortho Borylation of Functionalized Arenes Catalyzed by a Silica-Supported Compact Phosphine Iridium System”, J. Am. Chem. Soc., 131 (14), 5058-5059 (2009).

2. T. Kimura, S. Huang, A. Fukuoka and K. Kuroda, “Properties of metal species in square-shape mesopores of KSW-2-based silica, J. Mater. Chem., 19 (23), 3859-3866 (2009).

3. A. Fukuoka and P. L. Dhepe, “Sustainable Green Catalysis by Supported Metal Nanoparticles”, The Chemical Record, 9, 224-235 (2009).

4. S. Huang, K. Hara, Y. Okubo, M. Yanagi, H. Nanbu, A. Fukuoka, “Preferential oxidation of carbon monoxide in excess hydrogen over platinum catalysts supported on different pore size mesoporous silica”, Appl. Catal. A. General, 365, 268-273 (2009).

5. S. Huang, K. Hara and A. Fukuoka, “Green catalysis for selective CO oxidation in hydrogen for fuel cell”, Energy & Environmental Science, 2, 1060-1068 (2009).

[Reviews]
1.福岡淳、渡辺瑞穂、“バイオマスを分解する固体触媒−低炭素社会をめざす技術開発、化学64 (4), 70-71 (2009).

2. P. L. Dhepe and A. Fukuoka, “Catalysis of Mesoporous Solid Acids for Environmentally Benign Processes” in Bottom-up Nanofabrication: Supramolecules, Self-Assemblies, and Organized Films” K. Ariga ed., American Scientific Publisher, Valencia, Chapter 14 pp. 365-384 (2009).

3. 小林広和、福岡淳、セルロースの解重合(触媒)、木質系有機資源の新展開U、舩岡正光監修、シーエムシー出版、176-182 (2009).


2008

[Refereed papers]

1. S. Kawamorita, G. Hamasaka, H. Ohmiya, K. Hara, A. Fukuoka and M. Sawamura, “Hydrogenation of Hindered Ketones Catalyzed by a Silica-Supported Compact Phosphine-Rh System”, Org. Lett., 10 (20), 4697-4700 (2008).

2. G. Hamasaka, S. Kawamorita, A. Ochida, R. Akiyama, K. Hara, A. Fukuoka, K. Asakura, W. J. Chun, H. Ohmiya and M. Sawamura, “Synthesis of Silica-Supported Compact Phosphines and Their Application to Rhodium-Catalyzed Hydrosilylation of Hindered Ketones with Triorganosilanes”, Organometallics, 27 (24), 6495-6506 (2008).

3. P. L. Dhepe and A. Fukuoka, “Cellulose Conversion by Heterogeneous Catalysis”, ChemSusChem, 1 (12), 969-975 (2008).

 
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