Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels
Xinyang Gao, Yongjun Jiang, Jiyuan Liu, Guoshuai Shi, Chunlei Yang, Qinshang Xu, Yeonhee Yun, Yuluo Shen, Ming‐Wei Chang, Chenyuan Zhu, Tingyu Lu, Yin Wang, Gang Du, Shuzhou Li, Sheng Dai, Liming Zhang
Abstract
A bimetallic heterostructure has been shown effective to enhance the multi-carbon (C2+) product selectivity in CO2 electroreduction. Clarifying the interfacial structure under electrolysis and its decisive role in the pathway selection are crucial, yet challenging. Here, we conceive a well-defined Ag-Cu biphasic heterostructure to understand the interfacial structure-steered product selectivity: The Cu-rich interface prefers ethylene, while the dominant product switch to alcohols with an increasing Ag fraction, and finally to CO as Ag occupying the main surface. We unravel a *CO intermediate-regulated interfacial restructuring, and observe abundant of Cu atoms migrating onto the neighboring Ag surface under a locally high *CO concentration. The evolving structure alters the oxyphilic characteristic at the interface, which profoundly determines the hydrogenation energetics of CO2 and ultimately, the dominant C2+ product. This work explicitly links the evolving interfacial structure with distinct C2+ pathway, formulating design guidelines for bimetallic electrocatalysts with selectively enhanced C2+ yields. Probing the interfacial structure of catalysts under CO2 electrolysis is crucial. Here, the authors report a well-defined bimetallic silver-copper heterostructure to unravel an intermediate-regulated interfacial restructuring behavior, which promotes CO2 electroreduction to multi-carbon products.