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Unraveling the electrolyte-free interface in membrane CO₂ electrolysers

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dc.contributor.authorRen, W.
dc.contributor.authorZheng, Y.
dc.contributor.authorQiao, S.-Z.
dc.date.issued2025
dc.descriptionFirst published 07 Jul 2025
dc.description.abstractZero-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).
dc.description.statementofresponsibilityWenhao Ren, Yao Zheng and Shi-Zhang Qiao
dc.identifier.citationEnergy and Environmental Science, 2025; 18(15):7402-7412
dc.identifier.doi10.1039/d5ee02408k
dc.identifier.issn1754-5692
dc.identifier.issn1754-5706
dc.identifier.orcidRen, W. [0000-0002-8769-3131]
dc.identifier.orcidZheng, Y. [0000-0002-2411-8041]
dc.identifier.orcidQiao, S.-Z. [0000-0002-1220-1761] [0000-0002-4568-8422]
dc.identifier.urihttps://hdl.handle.net/2440/146288
dc.language.isoen
dc.publisherRoyal Society of Chemistry
dc.relation.granthttp://purl.org/au-research/grants/arc/DE230100324
dc.relation.granthttp://purl.org/au-research/grants/arc/DP230102027
dc.relation.granthttp://purl.org/au-research/grants/arc/CE230100032
dc.rightsThis journal is © The Royal Society of Chemistry 2025
dc.source.urihttps://doi.org/10.1039/d5ee02408k
dc.titleUnraveling the electrolyte-free interface in membrane CO₂ electrolysers
dc.title.alternativeUnraveling the electrolyte-free interface in membrane CO2 electrolysers
dc.typeJournal article
pubs.publication-statusPublished

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