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Title: Enhancing CO 2 electroreduction with the metal–oxide interface

Here, the electrochemical CO 2 reduction reaction (CO 2RR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO 2. We report here a strategy to enhance CO 2RR by constructing the metal–oxide interface. We demonstrate that Au–CeO x shows much higher activity and Faradaic efficiency than Au or CeO x alone for CO 2RR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au–CeO x interface is dominant in enhancing CO 2 adsorption and activation, which can be further promoted by the presence of hydroxyl groups. Density functional theory calculations indicate that the Au–CeO x interface is the active site for CO 2 activation and the reduction to CO, where the synergy between Au and CeO x promotes the stability of key carboxyl intermediate (*COOH) and thus facilitates CO 2RR. Similar interface-enhanced CO 2RR is further observed on Ag–CeO x, demonstrating the generality of the strategy for enhancing CO 2RR.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ; ORCiD logo [4] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1]
  1. Chinese Academy of Sciences, Dalian (China)
  2. Chinese Academy of Sciences, Dalian (China); Univ. of Chinese Academy of Sciences, Beijing (China)
  3. Univ. of Science and Technology of China, Hefei (China)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-114026-2017-JA
Journal ID: ISSN 0002-7863; R&D Project: CO040; KC0302010; TRN: US1702328
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 16; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1368679

Gao, Dunfeng, Zhang, Yi, Zhou, Zhiwen, Cai, Fan, Zhao, Xinfei, Huang, Wugen, Li, Yangsheng, Zhu, Junfa, Liu, Ping, Yang, Fan, Wang, Guoxiong, and Bao, Xinhe. Enhancing CO2 electroreduction with the metal–oxide interface. United States: N. p., Web. doi:10.1021/jacs.7b00102.
Gao, Dunfeng, Zhang, Yi, Zhou, Zhiwen, Cai, Fan, Zhao, Xinfei, Huang, Wugen, Li, Yangsheng, Zhu, Junfa, Liu, Ping, Yang, Fan, Wang, Guoxiong, & Bao, Xinhe. Enhancing CO2 electroreduction with the metal–oxide interface. United States. doi:10.1021/jacs.7b00102.
Gao, Dunfeng, Zhang, Yi, Zhou, Zhiwen, Cai, Fan, Zhao, Xinfei, Huang, Wugen, Li, Yangsheng, Zhu, Junfa, Liu, Ping, Yang, Fan, Wang, Guoxiong, and Bao, Xinhe. 2017. "Enhancing CO2 electroreduction with the metal–oxide interface". United States. doi:10.1021/jacs.7b00102. https://www.osti.gov/servlets/purl/1368679.
@article{osti_1368679,
title = {Enhancing CO2 electroreduction with the metal–oxide interface},
author = {Gao, Dunfeng and Zhang, Yi and Zhou, Zhiwen and Cai, Fan and Zhao, Xinfei and Huang, Wugen and Li, Yangsheng and Zhu, Junfa and Liu, Ping and Yang, Fan and Wang, Guoxiong and Bao, Xinhe},
abstractNote = {Here, the electrochemical CO2 reduction reaction (CO2RR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO2. We report here a strategy to enhance CO2RR by constructing the metal–oxide interface. We demonstrate that Au–CeOx shows much higher activity and Faradaic efficiency than Au or CeOx alone for CO2RR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au–CeOx interface is dominant in enhancing CO2 adsorption and activation, which can be further promoted by the presence of hydroxyl groups. Density functional theory calculations indicate that the Au–CeOx interface is the active site for CO2 activation and the reduction to CO, where the synergy between Au and CeOx promotes the stability of key carboxyl intermediate (*COOH) and thus facilitates CO2RR. Similar interface-enhanced CO2RR is further observed on Ag–CeOx, demonstrating the generality of the strategy for enhancing CO2RR.},
doi = {10.1021/jacs.7b00102},
journal = {Journal of the American Chemical Society},
number = 16,
volume = 139,
place = {United States},
year = {2017},
month = {4}
}