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DOI	10.1016/j.scib.2020.06.023
	Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction
	Bai H.; Cheng T.; Li S.; Zhou Z.; Yang H.; Li J.; Xie M.; Ye J.; Ji Y.; Li Y.; Zhou Z.; Sun S.; Zhang B.; Peng H.
发表日期	2021
ISSN	20959273
起始页码	62
结束页码	68
卷号	66 期号:1
英文摘要	Among all CO2 electroreduction products, methane (CH4) and ethylene (C2H4) are two typical and valuable hydrocarbon products which are formed in two different pathways: hydrogenation and dimerization reactions of the same CO intermediate. Theoretical studies show that the adsorption configurations of CO intermediate determine the reaction pathways towards CH4/C2H4. However, it is challenging to experimentally control the CO adsorption configurations at the catalyst surface, and thus the hydrocarbon selectivity is still limited. Herein, we seek to synthesize two well-defined copper nanocatalysts with controllable surface structures. The two model catalysts exhibit a high hydrocarbon selectivity toward either CH4 (83%) or C2H4 (93%) under identical reduction conditions. Scanning transmission electron microscopy and X-ray absorption spectroscopy characterizations reveal the low-coordination Cu0 sites and local Cu0/Cu+ sites of the two catalysts, respectively. CO-temperature programed desorption, in-situ attenuated total reflection Fourier transform infrared spectroscopy and density functional theory studies unveil that the bridge-adsorbed CO (COB) on the low-coordination Cu0 sites is apt to be hydrogenated to CH4, whereas the bridge-adsorbed CO plus linear-adsorbed CO (COB + COL) on the local Cu0/Cu+ sites are apt to be coupled to C2H4. Our findings pave a new way to design catalysts with controllable CO adsorption configurations for high hydrocarbon product selectivity. © 2020 Science China Press
关键词	CO adsorption CO2 electroreduction Dimerization Hydrogenation
英文关键词	Adsorption; Carbon dioxide; Catalyst selectivity; Copper metallography; Density functional theory; Electrolytic reduction; Ethylene; Fourier transform infrared spectroscopy; High resolution transmission electron microscopy; Hydrogenation; Mathematical transformations; Methane; Nanocatalysts; Product design; Reaction intermediates; Scanning electron microscopy; X ray absorption spectroscopy; Density functional theory studies; Dimerization reactions; Hydrocarbon product; Methane production; Reaction pathways; Reduction conditions; Scanning transmission electron microscopy; Situ attenuated total reflection-Fourier transform infrared spectroscopy; Copper compounds
语种	英语
来源期刊	Science Bulletin
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/207342
作者单位	State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai, 200438, China; Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China; Institute of Chemical Sciences and Engineering, École polytechnique fédérale de Lausanne, Lausanne, 1015, Switzerland; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
推荐引用方式 GB/T 7714	Bai H.,Cheng T.,Li S.,et al. Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction[J],2021,66(1).
APA	Bai H..,Cheng T..,Li S..,Zhou Z..,Yang H..,...&Peng H..(2021).Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction.Science Bulletin,66(1).
MLA	Bai H.,et al."Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction".Science Bulletin 66.1(2021).