Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions

doi:10.1021/acssuschemeng.9b01561

	Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions
	Yang, Bing 2,3,7; Yu, Xin ; Halder, Avik 3; Zhang, Xiaoben 2,7; Zhou, Xiong 1,5; Mannie, Gilbere J. A.5; Tyo, Eric 3; Pellin, Michael J.3; Seifert, Soenke 4; Su, Dangsheng 2,7
刊名	ACS SUSTAINABLE CHEMISTRY & ENGINEERING
	2019-09-03
卷号	7 期号:17 页码:14435-14442
关键词	CO2 conversion Synergistic interaction In situ characterization Copper catalyst Iron oxide
ISSN号	2168-0485
DOI	10.1021/acssuschemeng.9b01561
通讯作者	Yang, Bing(byang@dicp.ac.cn) ; Vajda, Stefan(stefan.vajda@jh-inst.cas.cz)
英文摘要	Atomically precise subnanometer catalysts are of significant interest because of their remarkable efficiency in a variety of catalytic reactions. However, the dynamic changes of active sites under reaction conditions, in particular, the transition of cluster-oxide interface structure have not yet been well-elucidated, lacking in situ measurements. By using multiple state-of-the-art in situ characterizations, here we show a dynamic interplay between copper tetramers and iron oxides in a single-size Cu-4/Fe2O3 catalyst, yielding an enrichment of surface Cu-4-Fe2+ species under reaction conditions that boosts CO2 hydrogenation at near-atmospheric pressures. During reaction, Cu-4 clusters facilitate the reduction of Fe2O3 producing surface-rich Fe2+ species in the proximate sites. The as-formed Fe2+ species in return promotes CO2 activation and transformation over Cu4 cluster, resulting in strikingly high methanol synthesis at low temperatures and C-1/C-3 hydrocarbon production in a high-temperature regime. The discovery of highly active Cu-4-Fe2+ sites thus provides new insights for the atomic-level design of copper catalyst toward high-efficiency CO2 conversion under mild conditions.
资助项目	U.S. Department of Energy, Office of Science, BES-Materials Sciences[DE-AC-02-06CH11357] ; U.S. Department of Energy, Scientific User Facilities[DE-AC-02-06CH11357] ; Talents Innovation Project of Dalian[2016RD04] ; National Natural Science Foundation of China[21872145] ; European Union[810310]
WOS关键词	OXYGEN REDUCTION REACTION ; CARBON-DIOXIDE ; ACTIVE-SITES ; CATALYSTS ; HYDROGENATION ; CU ; CLUSTERS ; WATER ; XPS ; INTERFACE
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Engineering
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000484071600015
资助机构	U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Scientific User Facilities ; U.S. Department of Energy, Scientific User Facilities ; Talents Innovation Project of Dalian ; Talents Innovation Project of Dalian ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; European Union ; European Union ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Scientific User Facilities ; U.S. Department of Energy, Scientific User Facilities ; Talents Innovation Project of Dalian ; Talents Innovation Project of Dalian ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; European Union ; European Union ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Scientific User Facilities ; U.S. Department of Energy, Scientific User Facilities ; Talents Innovation Project of Dalian ; Talents Innovation Project of Dalian ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; European Union ; European Union ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Office of Science, BES-Materials Sciences ; U.S. Department of Energy, Scientific User Facilities ; U.S. Department of Energy, Scientific User Facilities ; Talents Innovation Project of Dalian ; Talents Innovation Project of Dalian ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; European Union ; European Union
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/172834]
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	Yang, Bing; Vajda, Stefan
作者单位	1.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Argonne Natl Lab, Mat Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA 4.Argonne Natl Lab, Xray Sci Div, 9700 S Cass Ave, Argonne, IL 60439 USA 5.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuels, Beijing 101400, Peoples R China 6.Univ Chicago, Inst Mol Engn, 5640 S Ellis Ave, Chicago, IL 60637 USA 7.Univ Chinese Acad Sci, 19 A Yuquan Rd, Beijing 100049, Peoples R China 8.Czech Acad Sci, J Heyrovsky Inst Phys Chem, Dept Nanocatalysis, Dolejskova 3, Prague 18223, Czech Republic
推荐引用方式 GB/T 7714	Yang, Bing,Yu, Xin,Halder, Avik,et al. Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2019,7(17):14435-14442.
APA	Yang, Bing.,Yu, Xin.,Halder, Avik.,Zhang, Xiaoben.,Zhou, Xiong.,...&Vajda, Stefan.(2019).Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,7(17),14435-14442.
MLA	Yang, Bing,et al."Dynamic Interplay between Copper Tetramers and Iron Oxide Boosting CO2 Conversion to Methanol and Hydrocarbons under Mild Conditions".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 7.17(2019):14435-14442.