Coverage enhancement accelerates acidic CO2 electrolysis at ampere-level current with high energy and carbon efficiencies

Xiaohan Yu, Yuting Xu, Le Li, Mingzhe Zhang, Wenhao Qin, Fanglin Che () and Miao Zhong ()
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Xiaohan Yu: Nanjing University
Yuting Xu: University of Massachusetts Lowell
Le Li: Nanjing University
Mingzhe Zhang: Nanjing University
Wenhao Qin: Nanjing University
Fanglin Che: University of Massachusetts Lowell
Miao Zhong: Nanjing University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Acidic CO2 electroreduction (CO2R) using renewable electricity holds promise for high-efficiency generation of storable liquid chemicals with up to 100% CO2 utilization. However, the strong parasitic hydrogen evolution reaction (HER) limits its selectivity and energy efficiency (EE), especially at ampere-level current densities. Here we present that enhancing CO2R intermediate coverage on catalysts promotes CO2R and concurrently suppresses HER. We identified and engineered robust Cu6Sn5 catalysts with strong *OCHO affinity and weak *H binding, achieving 91% Faradaic efficiency (FE) for formic acid (FA) production at 1.2 A cm−2 and pH 1. Notably, the single-pass carbon efficiency reaches a new benchmark of 77.4% at 0.5 A cm−2 over 300 hours. In situ electrochemical Fourier-transform infrared spectroscopy revealed Cu6Sn5 enhances *OCHO coverage ~2.8× compared to Sn at pH 1. Using a cation-free, solid-state-electrolyte-based membrane-electrode-assembly, we produce 0.36 M pure FA at 88% FE over 130 hours with a marked full-cell EE of 37%.

Date: 2024
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DOI: 10.1038/s41467-024-45988-4

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