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, Yuanqing Yun, Yuluo Shen, Mingwei Chang, Chenyuan Zhu, Tingyu Lu, Yin Wang, Guanchen Du, Shuzhou Li (), Sheng Dai () and Liming Zhang ()
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Xinyang Gao: Fudan University
Yongjun Jiang: East China University of Science and Technology
Jiyuan Liu: Nanyang Technological University
Guoshuai Shi: Fudan University
Chunlei Yang: Fudan University
Qinshang Xu: Fudan University
Yuanqing Yun: Fudan University
Yuluo Shen: Fudan University
Mingwei Chang: Fudan University
Chenyuan Zhu: Fudan University
Tingyu Lu: Fudan University
Yin Wang: Fudan University
Guanchen Du: Fudan University
Shuzhou Li: Nanyang Technological University
Sheng Dai: East China University of Science and Technology
Liming Zhang: Fudan University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-54630-2

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