Electrochemical Assembly of a Defective Cu Catalyst for High Current CO <sub>2</sub> Electrolysis to Methane in a Zero‐Gap Electrolyzer
CO<sub>2</sub> 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<sub>6</sub>) achieved a record methane FE of 71.46% and production rate of 0.28 µmol s<sup>-1</sup> cm<sup>-2</sup>, 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.
Authors
- Wan Ru Leow (ORCID: https://orcid.org/0000-0002-8189-4813)
- Yiwei Shen (ORCID: https://orcid.org/0009-0009-2753-1155)
- Yanwei Lum (ORCID: https://orcid.org/0000-0001-7261-2098)
- Qin Yang (ORCID: https://orcid.org/0000-0001-6700-475X)
- Lei Wang (ORCID: https://orcid.org/0000-0001-7275-4846)
- Sung‐Fu Hung (ORCID: https://orcid.org/0000-0002-7423-2723)
- Tanmay Ghosh (ORCID: https://orcid.org/0000-0003-0532-2407)
- Tao Wang (ORCID: https://orcid.org/0000-0003-4045-2434)
- Zainul Aabdin (ORCID: https://orcid.org/0000-0002-0436-1327)
- Mingsheng Zhang (ORCID: https://orcid.org/0000-0002-1905-9198)
- Ziyun Wang (ORCID: https://orcid.org/0000-0002-2817-8367)
- Jiguang Zhang (ORCID: https://orcid.org/0000-0002-8212-1361)
- Ziyu Mi
- Langhuan Huang
- Kang‐Shun Peng
- Ruoou Yang
- Yuqi Yang (ORCID: https://orcid.org/0000-0002-6116-9198)
Institutions
- 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)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-10-04
- DOI
- https://doi.org/10.1002/anie.202515396
- Citations
- 1
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 0.36