A Theoretical Study on the catalytic activity of gold nanoparticles

• Project/Area Number: 22550001
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Physical chemistry
• Research Institution: Hokkaido University
• Principal Investigator: LYALIN Andrey 北海道大学, 大学院・理学研究院, 博士研究員 (70542273)
• Co-Investigator(Kenkyū-buntansha): TAKETSUGU Tetsuya 北海道大学, 大学院・理学研究院, 教授 (90280932)
• Project Period (FY): 2010 – 2012
• Project Status: Completed (Fiscal Year 2012)
• Budget Amount: ¥4,030,000 (Direct Cost: ¥3,100,000、Indirect Cost: ¥930,000); Fiscal Year 2012: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000); Fiscal Year 2011: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000); Fiscal Year 2010: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
• Keywords: 金ナノ粒子 / 触媒活性 / サイズ依存性 / 金クラスター / 選択的酸化 / 金属表面 / DFT 計算 / クラスター融合アルゴリズム / 金ナノクラスター / 酸素還元 / 酸化反応 / 担体効果 / 密度汎関数法 / 反応経路 / ボロンナイトライド / DFT計算

Research Abstract

Catalytic activity of small size-selected gold clusters for oxidation and hydrogen dissociation reactions has been studied theoretically using density functional theory. Cooperative effect in co-adsorption of C_2H_4 and O_2 on small gold clusters is found. It is demonstrated that co-adsorption of the reactant molecule can promote activation and dissociation of the molecular oxygen. The important role of the support effects on catalytic activity of gold clusters is studied. Two types of support are considered-the “inert” support of hexagonal boron nitride (h-BN) and the “active” support of rutile TiO_2(110). It is found that inert h-BN support can considerably affect catalytic activity of gold particles and modify barriers of chemical reactions catalyzed by gold. Electron-pushing mechanism of activation of the molecular O2 adsorbed on Au/h-BN is found. It is shown that h-BN support can be functionalized by N-doping and become catalytically active for oxygen reduction reaction. It is emonstrated that the active TiO_2 support considerably promotes H_2 dissociation on the supported gold clusters. It is shown theoretically that the catalytic activity of gold nanoparticles supported on the rutile TiO_2(110) surface is proportional to the length of the perimeter interface between the nanoparticle and the support.

Research Products

• [Journal Article] Theoretical predictions for hexagonal BN based nanomaterials as electrocatalysts for the oxygen reduction reaction (2013)
  • Author(s): A. Lyalin, A. Nakayama, K. Uosaki, and T.Taketsugu
  • Journal Title: Phys. Chem. Chem. Phys Volume: 15 Pages: 2809-2820
  • NAID: 120005356859
  • Peer Reviewed
• [Journal Article] COoxidation on h-BN supported Au atom (2013)
  • Author(s): M. Gao, A. Lyalin, and T. Taketsugu
  • Journal Title: J.Chem. Phys Volume: 138 Pages: 34701-34701
  • NAID: 120005228221
  • Peer Reviewed
• [Journal Article] Oxygen activation and dissociation on h-BN supported Au atoms (2013)
  • Author(s): M. Gao, A. Lyalin, and T. Taketsugu
  • Journal Title: Int. J. Quantum Chem Volume: 113 Pages: 443-452
  • Peer Reviewed
• [Journal Article] Theoretical predictions for hexagonal BN based nanomaterials as electrocatalysts for the oxygen reduction reaction (2013)
  • Author(s): Andrey Lyalin
  • Journal Title: Phys. Chem. Chem. Phys. Volume: 15 Issue: 8 Pages: 2809-2820
  • DOI: 10.1039/c2cp42907a
  • NAID: 120005356859
  • Peer Reviewed
• [Journal Article] CO oxidation on h-BN supported Au atom (2013)
  • Author(s): Min Gao
  • Journal Title: J. Chem. Phys. Volume: 138 Issue: 3 Pages: 34701-34701
  • DOI: 10.1063/1.4774216
  • Peer Reviewed
• [Journal Article] Catalytic activity of Au and Auon h-BN surface: adsorption and activation of O_2 (2012)
  • Author(s): M. Gao, A. Lyalin, and T. Taketsugu
  • Journal Title: J.Phys. Chem. C Volume: 116 Pages: 9054-9062
  • Peer Reviewed
• [Journal Article] Theoretical study of O2 dissociation on Au cluster on h-BN surface (2012)
  • Author(s): M.Gao
  • Journal Title: Int.J.Quantum Chem Volume: 113 Issue: 4 Pages: 443-452
  • DOI: 10.1002/qua.24066
  • Peer Reviewed
• [Journal Article] Catalytic activity of Au clusters supported on h-BN surface : Adsorption and activation of O2 (2012)
  • Author(s): M.Gao
  • Journal Title: J.Phys.Chem.C Volume: 116 Issue: 16 Pages: 9054-9062
  • DOI: 10.1021/jp300684v
  • Peer Reviewed
• [Journal Article] Role ofthe support effects on the catalytic activity ofgold clusters (2011)
  • Author(s): M. Gao, A. Lyalin, and T. Taketsugu
  • Journal Title: a density functional theory study, Catalysts Volume: 1 Pages: 18-39
  • Peer Reviewed
• [Journal Article] A computational investigation of H adsorption and dissociation on Au nanoparticles supported on TiO_22 surface (2011)
  • Author(s): A. Lyalin and T. Taketsugu
  • Journal Title: Faraday Discussions Volume: 152 Pages: 185-201
  • Peer Reviewed
• [Journal Article] A computational investigation of H_2 adsorption and dissociation on Au nanoparticles supported on TiO_2 surface (2011)
  • Author(s): A.Lyalin
  • Journal Title: Faraday Discussions Volume: 152 Pages: 185-201
  • DOI: 10.1039/c1fd00013f
  • Peer Reviewed
• [Journal Article] Role of support effects on the catalytic activity of gold clusters : A density functional theory study (2011)
  • Author(s): M.Gao
  • Journal Title: Catalysts Volume: 1 Pages: 18-39
  • Peer Reviewed
• [Journal Article] Reactant promoted oxygen dissociation on gold clusters (2010)
  • Author(s): A. Lyalin and T. Taketsugu
  • Journal Title: J. Phys. Chem. Lett Volume: 1 Pages: 1752-1757
  • Peer Reviewed
• [Journal Article] Adsorption of ethylene on neutral, anionic and cationic gold clusters (2010)
  • Author(s): A. Lyalin and T. Taketsugu
  • Journal Title: J. Phys. Chem. C Volume: 114 Pages: 2484-2493
  • Peer Reviewed
• [Journal Article] Adsorption of Ethylene on Neutral, Anionic and Cationic Gold Clusters (2010)
  • Author(s): A.Lyalin
  • Journal Title: J.Phys.Chem.C Volume: 114 Pages: 2484-2493
  • Peer Reviewed
• [Journal Article] Reactant Promoted Oxygen Dissociation on Gold Clusters (2010)
  • Author(s): A.Lyalin
  • Journal Title: J.Phys.Chem.Lett. Volume: 1 Pages: 1752-1757
  • Peer Reviewed
• [Presentation] A computational investigation of the unusual catalytic activity of h-BN based nanomaterials for oxygen reduction reaction (2012)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: The 10th Hokudai Simulation Salon (HSS) Workshop
  • Place of Presentation: Hokkaido University
  • Year and Date: 2012-02-17
• [Presentation] A computational investigation of the unusual catalytic activity of h-BN based nanomaterials for oxygen reduction reaction (2012)
  • Author(s): A.Lyalin
  • Organizer: The 10th Hokudai Simulation Salon (HSS) Workshop
  • Place of Presentation: Hokkaido University (sapporo)
  • Year and Date: 2012-02-17
• [Presentation] Role of the active and inert supports in enhanced catalytic activity of gold clusters (2012)
  • Author(s): A. Lyalin, M. Gao, T. Taketsugu
  • Organizer: DInternational Conference Dynamics of Systems on the Nanoscale" (DYSON 2012)
  • Place of Presentation: Saint Petersburg State Polytechnic University (Russia).
• [Presentation] Role of the support effects on the catalytic activity of gold clusters (2012)
  • Author(s): A. Lyalin, M. Gao, T. Taketsugu
  • Organizer: The Cluster-Surface Interactions (CSI) Workshop
  • Place of Presentation: University of Lyon (France)
• [Presentation] Catalytic Activity of Graphene and h-BN Based Nanomaterials for Oxygen Reduction Reaction (2012)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: The 6th General Meeting of ACCMS-VO
  • Place of Presentation: Tohoku University
• [Presentation] Role of the active and inert supports in enhanced catalytic activity of gold clusters (2012)
  • Author(s): Andrey Lyalin
  • Organizer: International Conference “Dynamics of Systems on the Nanoscale” (DYSON 2012)
  • Place of Presentation: Saint Petersburg State Polytechnic University (Russia)
  • Invited
• [Presentation] Catalytic Activity of Gold Particles Supported on h-BN Surface (2012)
  • Author(s): Andrey Lyalin
  • Organizer: The 6th International Conference GOLD 2012
  • Place of Presentation: Tokyo Metropolitan University (Tokyo)
• [Presentation] Catalytic Activity of Graphene and h-BN Based Nanomaterials for Oxygen Reduction Reaction (2012)
  • Author(s): A.Lyalin
  • Organizer: The 6th General Meeting of ACCMS-VO
  • Place of Presentation: Tohoku University (sendai)
• [Presentation] Role of support in the catalytic activity of gold nanoclusters (2011)
  • Author(s): A. Lyalin, M. Gao, T. Taketsugu
  • Organizer: 第9回Hokudai Simulation Salon ワークショップ
  • Place of Presentation: Hokkaido University
  • Year and Date: 2011-03-24
• [Presentation] Role of support in the catalytic activity of gold nanoclusters (2011)
  • Author(s): A.Lyalin
  • Organizer: 第9回Hokudai Simulation Salonワークショップ
  • Place of Presentation: Sapporo
  • Year and Date: 2011-03-24
• [Presentation] Catalytic Activity of Gold Particles Supported on h-BN Surface (2011)
  • Author(s): M. Gao, A. Lyalin, T. Taketsugu
  • Organizer: The 6th InternationalConference GOLD 2012
  • Place of Presentation: Tokyo Metropolitan University.
• [Presentation] Theoretical Investigation of the Oxygen Reduction Reaction on h-BN Monolayer (2011)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: The 5th Annual Meeting of Japan Society for Molecular Science
  • Place of Presentation: Sapporo Convention Center
• [Presentation] A computational investigation of H2 adsorption and dissociation on Au nanoparticles supported on TiO2 surface (2011)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: Faraday Discussion
  • Place of Presentation: Cardiff University (UK)
• [Presentation] Possibility of Oxygen Reduction Reaction on h-BN Monolayer with N Impurity Defect (2011)
  • Author(s): A. Lyalin, T. Taketsugu, On
  • Organizer: The 9th annual Meeting of Society of Nano Science and Technology: Nanoscience for sustainable society
  • Place of Presentation: Hokkaido University
• [Presentation] Theoretical Investigation of the Oxygen Reduction Reaction on h-BN Monolayer (2011)
  • Author(s): A.Lyalin
  • Organizer: The 5th Annual Meeting of Japan Society for Molecular Science
  • Place of Presentation: Hokkaido University (sapporo)
• [Presentation] A computational investigation of H_2 adsorption and dissociation on Au nanoparticles supported on TiO_2 surface (2011)
  • Author(s): A.Lyalin
  • Organizer: Faraday Discussion 152 : Gold
  • Place of Presentation: Cardiff University (UK)
• [Presentation] On Possibility of Oxygen Reduction Reaction on h-BN Monolayer with N Impurity Defect (2011)
  • Author(s): A.Lyalin
  • Organizer: The 9th annual Meeting of Society of Nano Science and Technology : Nanoscience for sustainable society
  • Place of Presentation: Hokkaido University (sapporo)
• [Presentation] Catalytic Activity of Au Clusters Supported on h-BN Surface (2011)
  • Author(s): M.Gao
  • Organizer: 2011年冬季研究発表会
  • Place of Presentation: 札幌
• [Presentation] Reactant promoted oxygen dissociation on gold clusters (2010)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: The 5th Asian Consortium on Computational Materials Science - Virtual Organization (ACCMS-VO)
  • Place of Presentation: Tohoku University
• [Presentation] Oxygen and hydrogen dissociation on gold clusters (2010)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: 第4回分子科学討論会
  • Place of Presentation: 大阪大学
• [Presentation] Reactant promoted oxygen dissociation on gold clusters (2010)
  • Author(s): A. Lyalin, T. Taketsugu
  • Organizer: 第13回理論化学討論会
  • Place of Presentation: 北海道大学
• [Presentation] Reactant promoted oxygen dissociation on gold clusters (2010)
  • Author(s): A.Lyalin
  • Organizer: 第13回理論化学討論会
  • Place of Presentation: 札幌
• [Presentation] Ab initio excited-state dynamics studies (2010)
  • Author(s): T.Taketsugu
  • Organizer: 13th International Conference on Theoretical Aspects of Catalysis
  • Place of Presentation: Matsushima 招待講演
• [Presentation] Oxygen and hydrogen dissociation on gold clusters (2010)
  • Author(s): A.Lyalin
  • Organizer: 第4回分子科学討論会
  • Place of Presentation: 大阪
• [Presentation] Theoretical study on the catalytic activity of Au cluster supported on the h-BN surface (2010)
  • Author(s): M.Gao
  • Organizer: The 4th GCOE international symposium
  • Place of Presentation: Sapporo
• [Presentation] Reactant promoted oxygen dissociation on gold clusters (2010)
  • Author(s): A.Lyalin
  • Organizer: The 5th Asian Consortium on Computational Materials Science-Virtual Organization (ACCMS-VO)
  • Place of Presentation: Sendai