Computational and experimental demonstrations of one-pot tandem catalysis for electrochemical carbon dioxide reduction to methane

Zhang, Haochen; Chang, Xiaoxia; Chen, Jingguang G.; Goddard, William A.; Xu, Bingjun; Cheng, Mu-Jeng; Lu, Qi

doi:10.1038/s41467-019-11292-9

Computational and experimental demonstrations of one-pot tandem catalysis for electrochemical carbon dioxide reduction to methane

Journal Article · Fri Jul 26 00:00:00 EDT 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-11292-9· OSTI ID:1610780

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Tsinghua Univ., Beijing (China); DOE/OSTI
Univ. of Delaware, Newark, DE (United States)
Columbia Univ., New York, NY (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)
National Cheng Kung Univ., Tainan City (Taiwan)
Tsinghua Univ., Beijing (China)

Electroreduction of carbon dioxide to hydrocarbons and oxygenates on copper involves reduction to a carbon monoxide adsorbate followed by further transformation to hydrocarbons and oxygenates. Simultaneous improvement of these processes over a single reactive site is challenging due to the linear scaling relationship of the binding strength of key intermediates. Herein, we report improved electroreduction of carbon dioxide by exploiting a one-pot tandem catalysis mechanism based on computational and electrochemical investigations. By constructing a well-defined copper-modified silver surface, adsorbed carbon monoxide generated on the silver sites is proposed to migrate to surface copper sites for the subsequent reduction to methane, which is consistent with insights gained from operando attenuated total reflectance surface enhanced infrared absorption spectroscopic investigations. Our results provide a promising approach for designing carbon dioxide electroreduction catalysts to enable one-pot reduction of products beyond carbon monoxide and formate.

View Accepted Manuscript (DOE)

Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1610780

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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