Unraveling the electrolyte-free interface in membrane CO₂ electrolysers
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(Accepted version)
Date
2025
Authors
Ren, W.
Zheng, Y.
Qiao, S.-Z.
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Journal article
Citation
Energy and Environmental Science, 2025; 18(15):7402-7412
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Wenhao Ren, Yao Zheng and Shi-Zhang Qiao
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Abstract
Zero-gap membrane electrode assembly electrolysers represent the benchmark architecture for scalable CO2 electrolysis and beyond. However, their device-level performance, particularly regarding energy efficiency and long-term stability, remains inadequate for practical deployment. Here, we argue that a key constraint of membrane electrolysers lies in the absence of catholytes, which creates a local reaction environment fundamentally distinct from that of aqueous H-type or flow cell systems, thereby reshaping electrocatalytic behaviour at the device level. We highlight the profound impacts of this catholyte-free interface, including altered proton availability, carbonate issues, mass transport limitations, product crossover, and re-oxidation—each representing a forefront challenge for CO2 electrolysis. By examining these emerging interfacial phenomena, we propose key strategies for advancing membrane CO2 electrolysers, including membrane-anolyte integration, ionomer engineering, and in situ device diagnostics. Collectively, these insights aim to bridge the interfacial gap between traditional half-cell studies (catalyst–electrolyte interfaces) and modern full-cell devices (catalyst–membrane interfaces).
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First published 07 Jul 2025
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This journal is © The Royal Society of Chemistry 2025