Selective Sieving Effect of Multi‐Atomic Bismuth Interfaces for Efficient Formate Electrosynthesis and Evolution at Industrial Current Density

作者：Mengyang Zhang, Wei Zhu, Zhengyang Liu, Shirui Chen, Dingyang Zhou, Xueqin Mu, Zechao Zhuang, Shengchen Wang, Jiarui Yang, Yapeng Du, Xiang Luo, Qinghua Zhang, Suli Liu, Dingsheng Wang, Zhihui Dai · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202510206 · 被引用次数：29 · 研究领域：Electrocatalysts for Energy Conversion、CO2 Reduction Techniques and Catalysts、Catalytic Processes in Materials Science

Abstract Constructing multi‐atomic interfaces architectures is promising for electrocatalytic CO 2 conversion, yet their synthesis and stability under industrial current densities remain challenging. Herein, multi‐atomic Bi interfaces (Bi 0 /Bi δ+ −O moiety) were precisely engineered by embedding atomically dispersed Bi centers, encompassing Bi single atoms and Bi atomic clusters into the substrate of porous Bi 2 O 3‐x nanosheets. The composite showcases outstanding CO 2 conversion performance across a wide pH range, attaining remarkable Faradaic efficiency for formate (FE formate ) of 96.48% (at ultralow potential of −0.5 V versus RHE) and 92.26% in alkaline and neutral electrolytes, along with exceptional long‐term stability over 150 h. Depending on the designed CH 3 OH electrooxidation catalyst (CuO x /ZnCo(OH) x ) at the anode to couple with CO 2 conversion, symmetrical/asymmetrical electrolyzers were developed. The approach could obtain high‐added value products with FE formate >90% at both electrodes, achieving a production rate of 4980 µmol h −1 cm −2 under industrial current density. Combined in situ characterizations and theoretical calculations unravel that multiple atomic interfaces featuring interfacial atomic sieving effects effectively enhance preferential binding of *H and *CO 2 to form *OCHO, while simultaneously suppressing the undesired recombination of hydrogen species into H 2 , rationalizing the high selectivity. Further intermediacy of concentrated fo...