Metal-organic double layer to stabilize selective multi-carbon electrosynthesis
Date
2025
Authors
Cheng, J.
Chen, L.
Zhang, Y.
Wang, M.
Zheng, Z.
Jiang, L.
Deng, Z.
Wei, Z.
Ma, M.
Xiong, L.
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Journal article
Citation
Nature Communications, 2025; 16(1):3743-1-3743-15
Statement of Responsibility
Jian Cheng, Ling Chen, Yanzhi Zhang, Min Wang, Zhangyi Zheng, Lin Jiang, Zhao Deng, Zhihe Wei, Mutian Ma, Likun Xiong, Wei Hua, Daqi Song, Wenxuan Huo, Yuebin Lian, Wenjun Yang, Fenglei Lyu, Yan Jiao, Yang Peng
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Abstract
Stable operation of the gas diffusion electrodes is key for industrial-scale electrochemical CO₂ reduction (eCO₂R). To enhance the electrolytic stability, we shield the Cu-coated gas diffusion electrode with a polycationic sheath via electrospinning and propose a Metal-Organic Double Layer (MODL) scheme to depict the triphasic interface. The as-fabricated electrode exhibits a high multi-carbon Faradaic efficiency of 91.2 ± 3.8%, along with operational stability for over 300 h at 300 mA cm⁻² in an alkaline flow cell. In a membrane electrode assembly with pure water as the anolyte, it further achieves an ethylene Faradaic efficiency over 50% at 200 mA cm¯². Mechanistic investigations unveil that replacing hydrated cationic counter ions in the conventional double layer with hydrogen bond-woven polycationic groups in the MODL allows simultaneously tailoring the local electric field and interfacial water structure. This study introduces a molecular-level redesign of the electric double layer in eCO₂R systems, achieving precisely tunable electrostatic characteristics and tailored chemical microenvironments while leveraging sustainable electrolysis systems to enable highly efficient and stable multi-carbon production.
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© The Author(s) 2025. This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http:// creativecommons.org/licenses/by-nc-nd/4.0/.