文献类型：期刊文献

英文题名：Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels

作者：Gao, Xinyang[1];Jiang, Yongjun[2];Liu, Jiyuan[3];Shi, Guoshuai[1];Yang, Chunlei[1];Xu, Qinshang[1];Yun, Yuanqing[1];Shen, Yuluo[1];Chang, Mingwei[1];Zhu, Chenyuan[1];Lu, Tingyu[1];Wang, Yin[1];Du, Guanchen[1];Li, Shuzhou[3];Dai, Sheng[2];Zhang, Liming[1]

机构：[1]Fudan Univ, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, iChEM Collaborat Innovat Ctr Chem Energy Mat, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Key Lab Adv Mat & Joint Int Res Lab Precis Chem &, Shanghai, Peoples R China;[3]Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore, Singapore

年份：2024

卷号：15

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001367613400024)】；

基金：This work is funded by the National Key R&D Program of China (2022YFA1505200), Natural Science Foundation of China (Grants 22072030, 22272029, and 22376062), Science and Technology Commission of Shanghai Municipality (Grant 22520711100, 22ZR1415700, and 23ZR1406900), the Fundamental Research Funds for the Central Universities (20720220008), Shanghai Rising-star Program (20QA1402400), Academic Research Fund Tier 1 (No. RG5/22), Academic Research Fund Tier 2 (MOE-T2EP10220-0005), Academic Research Fund Tier 2 (MOE-T2EP20221-0004) and the computing resources from National Supercomputing Center Singapore (NSCC). Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology.

语种：英文

摘要：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.