Document Type

Article

Publication Date

11-15-2026

Department

Department of Materials Science and Engineering

Abstract

Gas-fed electrochemical CO2 reduction (CO2R) to multicarbon products is fundamentally constrained by mass-transport limitations that suppress selectivity and stability at industrially relevant current densities. Here, we demonstrate that these bottlenecks can be overcome by engineering a porous aerophilic polymer microenvironment around a simple CuxO electrocatalyst without altering the intrinsic catalyst. By systematically replacing conventional PFSA ionomers with mixed aerophilic binders and applying a mild thermal treatment, we construct mechanically stabilized, gas-accessible overlayers that regulate the local gas-liquid microenvironment balance at the three-phase boundary (TPB). This approach drives a dramatic enhancement in ethylene production, increasing the partial current density from 135 mA cm−2 at 27 ± 5% Faradaic efficiency for CuxO with PFSA ionomer to over 650 mA cm−2 at 65 ± 4% Faradaic efficiency upon incorporation of a porous and aerophilic FEP/PTFE overlayer. Comprehensive microscopy and spectroscopy reveal intimate polymer-catalyst integration and overlayer consolidation, while COMSOL multiphysics modeling links enhanced CO2 availability to mitigated flooding rather than intrinsic kinetic acceleration. These results establish transport engineering as a powerful, catalyst-agnostic lever for advancing gas-phase electrosynthesis under high-rate operating conditions.

Publisher's Statement

© 2026 The Authors. Published by Elsevier B.V. Publisher’s version of record: 10.1016/j.cej.2026.181442

Publication Title

Chemical Engineering Journal

Creative Commons License

Creative Commons Attribution 4.0 International License
This work is licensed under a Creative Commons Attribution 4.0 International License.

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