Deoxygenation‐Induced Lattice Distortion in CuO x for Efficient Methane Diolate Anion Oxidation and Bipolar Hydrogen Evolution

作者：Kaiyang Xu, Chenyue Zhang, Yang Lü, Yaowen Xu, Binwen Zeng, Qianwang Chen, Bowen Li, Yang Zhao, Zhipeng Yu, Haoliang Huang, Wenlong Wang, Lecheng Liang, Shuqin Song, Lifeng Liu · 发表于：Advanced Functional Materials · 年份：2025 · DOI：10.1002/adfm.202510268 · 被引用次数：8 · 研究领域：Catalytic Processes in Materials Science、Copper-based nanomaterials and applications、Electrocatalysts for Energy Conversion

Abstract Hybrid water electrolysis represents apromising approach for energy‐efficient hydrogen (H 2 ) production. Herein, a highly active and selective electrocatalyst is reported for formaldehyde oxidation reaction (FOR), comprised of electrochemically deoxygenated copper nanosheet arrays supported on copper foam (D O ‐Cu‐NS/CF). Comprehensive in‐situ and ex‐situ characterization confirms the formation of a Cu‐rich, defect‐abundant surface during deoxygenation. Using solid paraformaldehyde (p‐HCHO) as anodic feedstock, D O ‐Cu‐NS/CF achieves remarkable current densities of 500 and 963.3 mA cm −2 at low potentials of merely 0.199 and 0.495 V versus RHE, respectively. Theoretical simulations demonstrate that p‐HCHO exists primarily as methane diolate anions (MDA) in alkaline media, and the lattice distortion in D O ‐Cu‐NS/CF significantly enhances MDA adsorption and oxidative dehydrogenation, leading to outstanding FOR performance. A membrane electrode assembly (MEA) utilizing D O ‐Cu‐NS/CF as the anode enables efficient bipolar H 2 production at 0.7 V for 280 h with a current density up to 500 mA cm −2 . This work highlights the crucial role of lattice engineering inenhancing FOR activity and offers new insights into the electrooxidation process of p‐HCHO. The D O ‐Cu‐NS/CF electrode developed shows significant potential for use as a cost‐effective anode for energy‐saving, high‐rate production of H 2 through hybrid water electrolysis.