CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment

Zesong Ma, Zhilong Yang, Wenchuan Lai (), Qiyou Wang, Yan Qiao, Haolan Tao, Cheng Lian, Min Liu, Chao Ma, Anlian Pan and Hongwen Huang ()
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Zesong Ma: Hunan University
Zhilong Yang: Hunan University
Wenchuan Lai: Hunan University
Qiyou Wang: Central South University
Yan Qiao: Hunan University
Haolan Tao: East China University of Science and Technology
Cheng Lian: East China University of Science and Technology
Min Liu: Central South University
Chao Ma: Hunan University
Anlian Pan: Hunan University
Hongwen Huang: Hunan University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm−2, single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K+ and OH−) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO2 conversion. We find that the K+ cations facilitate C-C coupling through local interaction between K+ and the key intermediate *OCCO.

Date: 2022
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DOI: 10.1038/s41467-022-35415-x

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