Measurements of surface reaction rates and design of active surfaces

• Project/Area Number: 19550008
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: The University of Tokyo
• Principal Investigator: SASAKI Takehiko The University of Tokyo, 大学院・新領域創成科学研究科, 准教授 (90242099)
• Project Period (FY): 2007 – 2009
• Project Status: Completed (Fiscal Year 2009)
• Budget Amount: ¥4,680,000 (Direct Cost: ¥3,600,000、Indirect Cost: ¥1,080,000); Fiscal Year 2009: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000); Fiscal Year 2008: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000); Fiscal Year 2007: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
• Keywords: 表面 / 界面 / 密度汎関数法 / ベンゼン酸化 / ゼオライト / TAP / レニウム / バイオガス / 合成ガス / 表面設計 / 蛍光寿命 / 光脱離 / 光反応 / テンソルLEED / ナノ粒子 / 結晶成長機構 / 電子刺激脱離 / パルス分子線 / 動的モンテカルロ法 / 遺伝的アルゴリズム

Research Abstract

The purpose of this research was to establish a method for measuring surface reaction rates as well as to establish a strategy for designing novel catalysts with high performances. Pulse molecular beam dosers and nitrogen Laser were installed in the Electron Stimulated Desorption system. TAP system was used to study a Ni catalyst prepared on silica support for reactions from biogas to syngas. For novel designed catalyst surfaces, immobilization of ionic liquid molecules on silica support surfaces and salt formation with chlorometallate anions were achieved. Shape control of nanocrystals of cobalt oxides and hydroxides were achieved. Density Functional Theory calculations were performed to obtain active structures of catalytic reactions and to clarify reaction mechanism for a Ru mononuclear complex attached on silica surface and Re cluster catalysts prepared in HZSM-5 framework.

Research Products

• [Journal Article] Alternative Selective Oxidation Pathways for Aldehyde Oxidation and Alkene Epoxidation on a SiO_2-Supported Ru-Monomer Complex Catalyst (2010)
  • Author(s): M. Tada, S. Muratsugu, M. Kinoshita, T. Sasaki, Y. Iwasawa
  • Journal Title: J.Am.Chem.Soc. 132 Pages: 713-724
  • Peer Reviewed
• [Journal Article] Co(OH)_3 Nanobelts : Synthesis, Characterization and Shape-preserved Transformation to Pseudo-single-crystalline Co_3O_4 Nanobelts (2010)
  • Author(s): J. Yang, H. Hyodo, K. Kimura, T. Sasaki
  • Journal Title: Nanotechnology 21 Pages: 45605-11
  • Peer Reviewed
• [Journal Article] Morphological Control of Single Crystalline Co_3O_4 Polyhedrons : Selective and Non-selective Growth of Crystal Planes Directed by Differently Charged Surfactants and Solvents (2010)
  • Author(s): J. Yang, T. Sasaki
  • Journal Title: Crystal Growth & Design 10 Pages: 1233-1236
  • Peer Reviewed
• [Journal Article] A novel mechanism for spectator CO-mediated reaction with unique cis-(NO)_2 dimer on a Co^<2+>-dimer/γ-Al_2O_3(110) model catalyst : Density functional theory calculations (2010)
  • Author(s): T. Taniike, M. Tada, R. Coquet, Y. Morikawa, T. Sasaki, Y. Iwasawa
  • Journal Title: Catal. Today
  • Peer Reviewed
• [Journal Article] Density Functional Theory Study on the Re Cluster/HZSM-5 catalysis for Direct Phenol Synthesis from Benzene and Molecular Oxygen : Active Re Structure and Reaction Mechanism (2009)
  • Author(s): T. Sasaki, M. Tada, Y. Iwasawa
  • Journal Title: Topics in Catalysis 52 Pages: 880-887
  • Peer Reviewed
• [Journal Article] TAP studies of the catalytic conversion of biogas to syngas over Ni/SiO_2 catalysts (2009)
  • Author(s): M. Olea, S. Hodgson, T. Sasaki, N. Aoki, K. Mae
  • Journal Title: Chemical Engineering Transactions 17 Pages: 7-12
  • Peer Reviewed
• [Journal Article] Density Functional Theory Study on the Re Cluster/HZSM-5 catalysis for Direct Phenol Synthesis from Benzene and Molecular Oxygen : Active Re Structure and Reaction Mechanism (2009)
  • Author(s): T.Sasaki, M.Tada, Y.Iwasawa
  • Journal Title: Topics in Catalysis 52 Pages: 880-887
  • Peer Reviewed
• [Journal Article] TAP studies of the catalytic conversion of biogas to syngas over Ni/SiO_2 catalysts (2009)
  • Author(s): M.Olea, S.Hodgson, T.Sasaki, N.Aoki, K.Mae
  • Journal Title: Chemical Engineering Transactions 17 Pages: 7-12
  • Peer Reviewed
• [Journal Article] Photoinduced Reversible Structural Transformation and Selective Oxidation Catalysis of Unsaturated Ruthenium Complexes Supported on SiO_2 (2008)
  • Author(s): M. Tada, Y. Akatsuka, Y. Yang, T. Sasaki, M. Kinoshita, K. Motokura, Y, Iwasawa
  • Journal Title: Angew.Chem.Int.Ed. 47 Pages: 9252-9255
  • Peer Reviewed
• [Journal Article] Synthesis of CoOOH Hierarchically Hollow Spheres by Nanorod Self Assembly through Bubble Templating (2008)
  • Author(s): J. Yang, T. Sasaki
  • Journal Title: Chem.Mater. 20 Pages: 2049-2056
  • Peer Reviewed
• [Journal Article] Immobilized Metal Ion-containing Ionic Liquids : Preparation, Structure and Catalytic Perfomances in Kharasch Addition Reaction and Suzuki Cross Coupling Reactions (2008)
  • Author(s): T. Sasaki, M. Tada, C. Zhong, T. Kume, Y. Iwasawa
  • Journal Title: J.Mol.Catal.A-Chemical 279 Pages: 200-209
  • Peer Reviewed
• [Journal Article] Photoinduced Reversible Structural Transformation and Selective Oxidation Cata lysis of Unsaturated Ruthenium Complexes Supported on SiO2 (2008)
  • Author(s): M. Tada, Y. Akatsuka, Y. Yang, T. Sasaki, M. Kinoshita, K. Motokura, and Y. Iwasawa
  • Journal Title: Angew. Chem. Int. Ed 47 Pages: 9252-9255
  • Peer Reviewed
• [Journal Article] Immobilized metal ion-containing ionic liquids: Preparation, structure and catalytic performances in Kharasch reaction and Suzuki reaction. (2008)
  • Author(s): Takehiko Sasaki, Mizuki Tada
  • Journal Title: J. Mol. Catal. A: Chemical 279 Pages: 200-209
  • Peer Reviewed
• [Journal Article] Synthesis of CoOOH Hierarchically Hollow Spheres by Nanorod Self-Assembly through Bubble Templating (2008)
  • Author(s): Jinhu Yang, Takehiko Sasaki
  • Journal Title: Chem. Mater. 20 Pages: 2049-2056
  • Peer Reviewed
• [Journal Article] Syntheses, Structure, and Properties of a Series of Metal Ion-Containing Dialkylimidazolium Ionic Liquids (2007)
  • Author(s): C. Zhong, T. Sasaki, A. Jimbo-Kobayashi, E. Fujiwara, A. Kobayashi, M. Tada, Y. Iwasawa
  • Journal Title: Bull.Chem.Soc.Jpn. 80 Pages: 2365-2374
  • NAID: 10020275688
  • Peer Reviewed
• [Journal Article] A new aspect of heterogeneous catalysis : Highly reactive cis-(NO)2 dimer and Eley-Rideal mechanism for NO-CO reaction on a Co-dimer/γ -alumina catalyst (2007)
  • Author(s): T. Taniike, M. Tada, R. Coquet, Y. Morikawa, T. Sasaki, Y. Iwasawa
  • Journal Title: Chem.Phys.Lett. 443 Pages: 66-70
  • Peer Reviewed
• [Journal Article] NH3-Promoted Direct Phenol Synthesis from Benzene with Molecular Oxygen on N-Interstitial Re10-Cluster/Zeolite Catalysts (2007)
  • Author(s): M. Tada, R. Bal, T. Sasaki, Y. Iwasawa
  • Journal Title: Stud.Surf.Sci.Catal. 172 Pages: 381-384
  • Peer Reviewed
• [Journal Article] A Novel Re-Cluster/HZSM-5 Catalyst for Highly Selective Phenol Synthesis from Benzene and O_2 : Performance and Reaction Mechanism (2007)
  • Author(s): M. Tada, R. Bal, T. Sasaki, Y. Uemura, Y. Inada, S. Tanaka, M. Nomura, Y. Iwasawa
  • Journal Title: J.Phys.Chem.C. 111 Pages: 10095-10104
  • Peer Reviewed
• [Journal Article] Synthesis, Structures,and Properties of a Series of Metal Ion-Contain-ing Dialkylimidazolium Ionic Liquids (2007)
  • Author(s): Chongmin Zhong, Takehiko Sasaki
  • Journal Title: Bull. Chem. Soc. Jpn. 80 Pages: 2365-2374
  • Peer Reviewed
• [Presentation] 密度汎関数法によるフェノール合成に活性なHZSM-5中に固定化したReクラスターの活性構造と反応機構の研究 (2009)
  • Author(s): 佐々木岳彦
  • Organizer: シンポジウム化学反応経路探索のニューフロンティア
  • Place of Presentation: 豊田理化学研究所
  • Year and Date: 2009-09-24
• [Presentation] 密度汎関数法によるフェノール合成に活性なHZSM-5中に固定化したReクラスターの活性構造と反応機構の研究 (2009)
  • Author(s): 佐々木岳彦
  • Organizer: 化学反応経路探索のニューフロンティア
  • Place of Presentation: 豊田理化学研究所
  • Year and Date: 2009-09-24
• [Presentation] Density Functional Theory Study on the Re Cluster/HZSM-5 catalysis for Direct Phenol Synthesis from Benzene and Molecular Oxygen : Active Re Structure and Reaction Mechanism (2008)
  • Author(s): T. Sasaki, M. Tada, Y. Iwasawa
  • Organizer: ICC 14 Pre-Symosium
  • Place of Presentation: 京都大学
  • Year and Date: 2008-07-08
• [Presentation] Density Functional Theory Study on the Re Cluster/HZSM-5 catalysis for Direct Phenol Synthesis from Benzene and Molecular Oxygen: Active Re Structure and Reaction Mechanism (2008)
  • Author(s): T. Sasaki, M. Tada and Y. Iwasawa
  • Organizer: ICC 14 Pre-Symosium
  • Place of Presentation: 京都大学
  • Year and Date: 2008-07-08
• [Presentation] 表面化学反応速度測定のための分子線-電子刺激脱離複合装置と動的モンテカルロシミュレーションプログラムの開発 (2007)
  • Author(s): 星野由美子, 佐々木岳彦
  • Organizer: 第1回分子科学討論会
  • Place of Presentation: 東北大学
  • Year and Date: 2007-09-20
• [Presentation] 表面化学反応速度測定のための分子線・電子刺激脱離複合装置と動的モンテカルロシミュレーションプログラムの開発 (2007)
  • Author(s): 星野由美子、佐々木岳彦
  • Organizer: 第1回分子科学討論会
  • Place of Presentation: 東北大学
  • Year and Date: 2007-09-20