Electrochemical Assembly of a Defective Cu Catalyst for High Current CO <sub>2</sub> Electrolysis to Methane in a Zero‐Gap Electrolyzer

Abstract CO 2 electrolysis to methane offers a promising route toward enabling long‐term storage of renewable energy. However, electrolysis in zero‐gap membrane electrode assembly (MEA) systems using conventional Cu‐based electrocatalysts is typically limited by relatively low methane productivity and Faradaic efficiency (FE). Here, we conceived an electrochemical assembly strategy that forms a Cu(111)‐dominant catalyst with vacancy defects. In an MEA system at a total current of 1.5 A, the catalyst (Def‐Cu 6 ) achieved a record methane FE of 71.46% and production rate of 0.28 µmol s −1 cm −2 , with relatively stable operation over 10 h. Density functional theory calculations reveal the crucial role of vacancy defects in a Cu(111) surface, which favors the hydrogenation of CO* and promotes methane formation over the competing CO* coupling pathway that leads to multicarbon products. Our findings demonstrate how vacancy defects can be tuned to control catalytic outcomes.

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Publication Details

Journal
Angewandte Chemie
Published
2025-10-04
DOI
https://doi.org/10.1002/ange.202515396
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
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article

Electrochemical Assembly of a Defective Cu Catalyst for High Current CO 2 Electrolysis to Methane in a Zero‐Gap Electrolyzer

Wan Ru Leow, Yiwei Shen, Yanwei Lum, Qin Yang et al.
Angewandte Chemie
CO2 Reduction Techniques and Catalysts
article

Electrochemical Assembly of a Defective Cu Catalyst for High Current CO 2 Electrolysis to Methane in a Zero‐Gap Electrolyzer

Wan Ru Leow, Yiwei Shen, Yanwei Lum, Qin Yang, Lei Wang, Sung‐Fu Hung, Tanmay Ghosh, Yuqi Yang, Tao Wang, Zainul Aabdin, Mingsheng Zhang, Ziyun Wang, Jiguang Zhang, Ziyu Mi, Langhuan Huang, Kang‐Shun Peng, Ruoou Yang
article en

Abstract

Abstract CO 2 electrolysis to methane offers a promising route toward enabling long‐term storage of renewable energy. However, electrolysis in zero‐gap membrane electrode assembly (MEA) systems using conventional Cu‐based electrocatalysts is typically limited by relatively low methane productivity and Faradaic efficiency (FE). Here, we conceived an electrochemical assembly strategy that forms a Cu(111)‐dominant catalyst with vacancy defects. In an MEA system at a total current of 1.5 A, the catalyst (Def‐Cu 6 ) achieved a record methane FE of 71.46% and production rate of 0.28 µmol s −1 cm −2 , with relatively stable operation over 10 h. Density functional theory calculations reveal the crucial role of vacancy defects in a Cu(111) surface, which favors the hydrogenation of CO* and promotes methane formation over the competing CO* coupling pathway that leads to multicarbon products. Our findings demonstrate how vacancy defects can be tuned to control catalytic outcomes.

Angewandte ChemieVol. 137(49)
Agency for Science, Technology and Research (SG), National Yang Ming Chiao Tung University (TW), University of Auckland (NZ), National University of Singapore (SG), ShanghaiTech University (CN), Singapore Institute for Clinical Sciences (SG), Institute of Materials Research and Engineering (SG), Henan Normal University (CN)
Openalex Percentile: Top 82%
CO2 Reduction Techniques and Catalysts
DOISourceOpenAlex
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