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中国化学会第八届全国配位化学会议

作者： Wei-Wei Wang Chun-Jiang Jia Wen-Zhu Yu Rui Si School of Chemistry and Chemical Engineering Shandong University Shanghai Institute of Applied Physics Chinese Academy of Sciences

Copper-ceria as one of the very active catalysts for oxidation reactions has been widely investigated in heterogeneous *** this work,copper oxide(1 wt%Cu loading)deposited on both ceria nanospheres with{111}/{100}-terminated surface(1CuCe-NS)and nanorods exposing{110}/{100}faces(1CuCe-NR)have been prepared for the investigation on crystal plane effect for CO oxidation *** is found that the copper oxides were formed as subnanometer clusters those uniformly dispersed on the surface of ceria *** results from XAFS combining H-TPR reveal that more reducible CuO clusters with only CuO coordination structure were exclusively dominated in the surface of 1CuCe-NS,while the Cu species in1CuCe-NR existed in both CuO clusters and strongly interacted Cu-[O]-***-situ DRIFTS results demonstrate that CeO-{110}face induced strongly bound Cu-[O]-Ce structure in 1CuCe-NR which was adverse to the formation of reduced Cu(I)active site,resulting in low reactivity in CO oxidation(r:1.8×10 mol?g?s at 118°C);on the contrary,CuO clusters on CeO-{111}face was easily reduced to Cu(I)species when subjected to interaction with CO,which greatly enhanced the catalytic reactivity(r:5.7×10 mol?g?sat 104°C).Thus for copper-ceria catalyst,the difference in strength of the interaction between copper oxides and different exposed faces of ceria is intrinsically relevant to the different redox and catalytic properties.

关键词： copper-ceria catalyst CO oxidation in situ DRIFTS metal-support interaction crystal plane effect

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Theoretical studies of CO oxidation with lattice oxygen on Co_3O_4 surfaces

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Chinese Journal of Catalysis 2016年第1期37卷 193-198页

作者：王阳刚杨小峰李隽清华大学化学系有机光电子与分子工程教育部重点实验室北京100084 中国科学院大连化学物理研究所催化基础国家重点实验室辽宁大连116023

Low-temperature CO oxidation has attracted extensive interest in heterogeneous catalysis because of the potential applications in fuel cells,air cleaning,and automotive emission *** the present study,theoretical investigations have been performed using density functional theory to elucidate the crystal plane effect and structure sensitivity of Co3O4 nano-catalysts toward catalyzing CO *** is shown that the surface Co–O ion pairs are the active site for CO oxidation on the Co3O4 *** of stronger CO adsorption and easier removal of lattice oxygen ions,the Co3O4（011）surface is shown to be more reactive for CO oxidation than the Co3O4（001）surface,which is consistent with previous experimental *** comparing the reaction pathways at different sites on each surface,we have further elucidated the nature of the crystal plane effect on Co3O4 surfaces and attributed the reactivity to the surface *** results suggest that CO oxidation catalyzed by Co3O4 nanocrystals has a strong crystal plane effect and structure *** the vacancy formation energy of the oxide surface is key for high CO oxidation reactivity.

关键词： Carbon monoxide oxidation Cobalt oxide crystal plane effect Ion-pair active center

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Morphology-dependent structures and catalytic performances of Au nanostructures on Cu_2O nanocrystals synthesized by galvanic replacement reaction

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Journal of Energy Chemistry 2016年第6期25卷 1086-1091页

作者： Zhenhua Zhang Rui Song Tian Cao Weixin Huang Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Materials for Energy Conversion and Department of Chemical Physics University of Science and Technology of China

Au nanostructures were prepared on uniform Cu2O octahedra and rhombic dodecahedra via the galvanic replacement reaction between HAuCl 4 and Cu2O. The compositions and structures were studied by Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), High-Resolution Transmission Electron Microscope (HRTEM), X-Ray Diffraction (XRD), X-Ray Absorption Spectroscopy (XAS), X-ray Photoelectron Spectroscopy (XPS) and in-situ DRIFTS spectroscopy of CO adsorption. Different from the formation of Au-Cu alloys on Cu2O cubes by the galvanic replacement reaction (ChemNanoMat 2 (2016) 861-865), metallic Au particles and positively-charged Au clusters form on Cu2O octahedra and rhombic dodecahedra at very small Au loadings and only metallic Au particles form at large Au loadings. Metallic Au particles on Cu2O octahedra and rhombic dodecahedra are more active in catalyzing the liquid phase aerobic oxidation reaction of benzyl alcohol than positively-charged Au clusters. These results demonstrate an obvious morphology effect of Cu2O nanocrystals on the liquid-solid interfacial reactions and prove oxide morphology as an effective strategy to tune the surface reactivity and catalytic performance. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Au/Cu2O nanocomposites Galvanic replacement reaction Liquid-solid interfacial reaction crystal plane effect Aerobic oxidation of benzyl alcohol

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