CO electroreduction on single-atom copper

Wang, Yuxuan; Li, Boyang; Xue, Bin; Libretto, Nicole; Xie, Zhenhua; Shen, Hao; Wang, Canhui; Raciti, David; Marinkovic, Nebojsa; Zong, Han; Xie, Wenjun; Li, Ziyuan; Zhou, Guangye; Vitek, Jeff; Chen, Jingguang G.; Miller, Jeffery; Wang, Guofeng; Wang, Chao

doi:10.1126/sciadv.ade3557

CO electroreduction on single-atom copper

Journal Article · Wed Jul 26 00:00:00 EDT 2023 · Science Advances

DOI:https://doi.org/10.1126/sciadv.ade3557· OSTI ID:2396915

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Johns Hopkins University, Baltimore, MD (United States); The Johns Hopkins University
University of Pittsburgh, PA (United States)
Johns Hopkins University, Baltimore, MD (United States); Shanghai Ocean University (China)
Purdue University, West Lafayette, IN (United States)
Columbia University, New York City, NY (United States)
Johns Hopkins University, Baltimore, MD (United States)
National Institute of Standards and Technology (NIST), Gaithersburg, MD (United States)
Columbia University, New York City, NY (United States)

Electroreduction of carbon dioxide (CO₂) or carbon monoxide (CO) toward C₂₊ hydrocarbons such as ethylene, ethanol, acetate and propanol represents a promising approach toward carbon-negative electrosynthesis of chemicals. Fundamental understanding of the carbon–carbon (C-C) coupling mechanisms in these electrocatalytic processes is the key to the design and development of electrochemical systems at high energy and carbon conversion efficiencies. Here, we report the investigation of CO electreduction on single-atom copper (Cu) electrocatalysts. Atomically dispersed Cu is coordinated on a carbon nitride substrate to form high-density copper–nitrogen moieties. Chemisorption, electrocatalytic, and computational studies are combined to probe the catalytic mechanisms. Unlike the Langmuir-Hinshelwood mechanism known for copper metal surfaces, the confinement of CO adsorption on the single-copper-atom sites enables an Eley-Rideal type of C-C coupling between adsorbed (*CO) and gaseous [CO(g)] carbon moxide molecules. The isolated Cu sites also selectively stabilize the key reaction intermediates determining the bifurcation of reaction pathways toward different C₂₊ products.

View Accepted Manuscript (DOE)

Research Organization:: Johns Hopkins University, Baltimore, MD (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Bioenergy Technologies Office (BETO)

Grant/Contract Number:: EE0008501

OSTI ID:: 2396915

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 30 Vol. 9; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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