Enhancing CO2 electroreduction with the metal–oxide interface

Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen; Cai, Fan; Zhao, Xinfei; Huang, Wugen; Li, Yangsheng; Zhu, Junfa; Liu, Ping; Yang, Fan; Wang, Guoxiong; Bao, Xinhe

doi:10.1021/jacs.7b00102

Enhancing CO₂ electroreduction with the metal–oxide interface

Journal Article · Sun Apr 09 04:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b00102· OSTI ID:1368679

^[1]; Zhang, Yi ^[2]; ^[2]; Cai, Fan ^[2]; Zhao, Xinfei ^[2]; Huang, Wugen ^[2]; Li, Yangsheng ^[2]; Zhu, Junfa ^[3]; ^[4]; ^[1]; Wang, Guoxiong ^[1]; ^[1]

Chinese Academy of Sciences, Dalian (China)
Chinese Academy of Sciences, Dalian (China); Univ. of Chinese Academy of Sciences, Beijing (China)
Univ. of Science and Technology of China, Hefei (China)
Brookhaven National Lab. (BNL), Upton, NY (United States)

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–CeO_x shows much higher activity and Faradaic efficiency than Au or CeO_x alone for CO₂RR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au–CeO_x 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–CeO_x interface is the active site for CO₂ 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 CO₂RR. Similar interface-enhanced CO₂RR is further observed on Ag–CeO_x, demonstrating the generality of the strategy for enhancing CO₂RR.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI ID:: 1368679

Report Number(s):: BNL--114026-2017-JA; KC0302010

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 16 Vol. 139; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Highly efficient binary copper−iron catalyst for photoelectrochemical carbon dioxide reduction toward methane Zhou, Baowen; Ou, Pengfei; Pant, Nick Proceedings of the National Academy of Sciences, Vol. 117, Issue 3 https://doi.org/10.1073/pnas.1911159117	journal	January 2020
Optimized Pt-Based Catalysts for Oxygen Reduction Reaction in Alkaline Solution: A First Principle Study Liu, Shizhong; Liu, Ping Journal of The Electrochemical Society, Vol. 165, Issue 15 https://doi.org/10.1149/2.0171815jes	journal	January 2018
Kinetic control of CeO2 nanoparticles for catalytic CO oxidation Han, Bingqi; Li, Huixia; Li, Liping Journal of Materials Research, Vol. 34, Issue 13 https://doi.org/10.1557/jmr.2018.456	journal	February 2019
Electrochemical CO2 Reduction to CO Catalyzed by 2D Nanostructures Hiragond, Chaitanya B.; Kim, Hwapyong; Lee, Junho Catalysts, Vol. 10, Issue 1 https://doi.org/10.3390/catal10010098	journal	January 2020
Comparative Study between Pristine Ag and Ag Foam for Electrochemical Synthesis of Syngas with Carbon Dioxide and Water Yu, Yan; Zhong, Na; Fang, Jinhui Catalysts, Vol. 9, Issue 1 https://doi.org/10.3390/catal9010057	journal	January 2019
Microfabricated electrodes unravel the role of interfaces in multicomponent copper-based CO2 reduction catalysts Larrazábal, Gastón O.; Shinagawa, Tatsuya; Martín, Antonio J. ETH Zurich https://doi.org/10.3929/ethz-b-000260950	text	January 2018

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