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Structure of the catalytically active copper-ceria interfacial perimeter

文献类型：期刊论文

作者Sehested, Jens1; Chen, Aling3; Yu, Xiaojuan4; Zhou, Yan3; Miao, Shu3; Li, Yong3; Kuld, Sebastian1; Liu, Jingyue2; Aoki, Toshihiro7; Hong, Song6
刊名NATURE CATALYSIS
出版日期2019-04-01
卷号2期号:4页码:334-341
ISSN号2520-1158
DOI10.1038/s41929-019-0226-6
通讯作者Zhou, Yan(zhouyan@dicp.ac.cn) ; Sehested, Jens(jss@topsoe.dk) ; Wang, Yuemin(yuemin.wang@kit.edu) ; Shen, Wenjie(shen98@dicp.ac.cn)
英文摘要Cu/CeO2 catalysts are highly active for the low-temperature water-gas shift-a core reaction in syngas chemistry for tuning the H-2/CO/CO2 proportions in feed streams-but the direct identification and quantitative description of the active sites remain challenging. Here we report that the active copper clusters consist of a bottom layer of mainly Cu+ atoms bonded on the oxygen vacancies (O-v) of ceria, in a form of Cu+-O-v-Ce3+, and a top layer of Cu-0 atoms coordinated with the underlying Cu+ atoms. This atomic structure model is based on directly observing copper clusters dispersed on ceria by a combination of scanning transmission electron microscopy and electron energy loss spectroscopy, in situ probing of the interfacial copper-ceria bonding environment by infrared spectroscopy and rationalization by density functional theory calculations. These results, together with reaction kinetics, reveal that the reaction occurs at the copper-ceria interfacial perimeter via a site cooperation mechanism: the Cu+ site chemically adsorbs CO whereas the neighbouring O-v-Ce3+ site dissociatively activates H2O.
WOS关键词WATER-GAS SHIFT ; IN-SITU ; METHANOL SYNTHESIS ; OXYGEN VACANCIES ; CARBON-MONOXIDE ; CO OXIDATION ; METAL-OXIDE ; CATALYSTS ; CU ; ADSORPTION
资助项目National Natural Science Foundation of China[91645107] ; National Natural Science Foundation of China[21533009] ; National Natural Science Foundation of China[21621063] ; National Natural Science Foundation of China[21761132031] ; Deutsche Forschungsgemeinschaft[WA 2535/2-1] ; 'Science and Technology of Nanosystems' Programme of Germany[432202] ; EU-H2020 research and innovation programme[654360] ; China Scholarship Council
WOS研究方向Chemistry
语种英语
出版者NATURE PUBLISHING GROUP
WOS记录号WOS:000464248600013
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; Deutsche Forschungsgemeinschaft ; Deutsche Forschungsgemeinschaft ; 'Science and Technology of Nanosystems' Programme of Germany ; 'Science and Technology of Nanosystems' Programme of Germany ; EU-H2020 research and innovation programme ; EU-H2020 research and innovation programme ; China Scholarship Council ; China Scholarship Council ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Deutsche Forschungsgemeinschaft ; Deutsche Forschungsgemeinschaft ; 'Science and Technology of Nanosystems' Programme of Germany ; 'Science and Technology of Nanosystems' Programme of Germany ; EU-H2020 research and innovation programme ; EU-H2020 research and innovation programme ; China Scholarship Council ; China Scholarship Council ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Deutsche Forschungsgemeinschaft ; Deutsche Forschungsgemeinschaft ; 'Science and Technology of Nanosystems' Programme of Germany ; 'Science and Technology of Nanosystems' Programme of Germany ; EU-H2020 research and innovation programme ; EU-H2020 research and innovation programme ; China Scholarship Council ; China Scholarship Council ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Deutsche Forschungsgemeinschaft ; Deutsche Forschungsgemeinschaft ; 'Science and Technology of Nanosystems' Programme of Germany ; 'Science and Technology of Nanosystems' Programme of Germany ; EU-H2020 research and innovation programme ; EU-H2020 research and innovation programme ; China Scholarship Council ; China Scholarship Council
源URL[http://cas-ir.dicp.ac.cn/handle/321008/165684]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Sehested, Jens; Zhou, Yan; Wang, Yuemin; Shen, Wenjie
作者单位1.Haldor Topsoe Res Labs, Lyngby, Denmark
2.Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian, Peoples R China
4.Karlsruhe Inst Technol, Inst Funct Interfaces, Eggenstein Leopoldshafen, Germany
5.CNR, IOM, Trieste, Italy
6.Beijing Univ Chem Technol, Ctr Instrumental Anal, Beijing, Peoples R China
7.Arizona State Univ, LeRoy Eyring Ctr Solid State Sci, Tempe, AZ USA
推荐引用方式
GB/T 7714		 Sehested, Jens,Chen, Aling,Yu, Xiaojuan,et al. Structure of the catalytically active copper-ceria interfacial perimeter[J]. NATURE CATALYSIS,2019,2(4):334-341.
APA Sehested, Jens.,Chen, Aling.,Yu, Xiaojuan.,Zhou, Yan.,Miao, Shu.,...&Shen, Wenjie.(2019).Structure of the catalytically active copper-ceria interfacial perimeter.NATURE CATALYSIS,2(4),334-341.
MLA Sehested, Jens,et al."Structure of the catalytically active copper-ceria interfacial perimeter".NATURE CATALYSIS 2.4(2019):334-341.

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来源：大连化学物理研究所

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