Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels
A bimetallic heterostructure has been shown effective to enhance the multi-carbon (C<sub>2+</sub>) product selectivity in CO<sub>2</sub> 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 CO<sub>2</sub> and ultimately, the dominant C<sub>2+</sub> product. This work explicitly links the evolving interfacial structure with distinct C<sub>2+</sub> pathway, formulating design guidelines for bimetallic electrocatalysts with selectively enhanced C<sub>2+</sub> yields.
Authors
- Yongjun Jiang (ORCID: https://orcid.org/0000-0002-9936-698X)
- Qinshang Xu
- Sheng Dai (ORCID: https://orcid.org/0000-0001-5787-0179)
- Chenyuan Zhu (ORCID: https://orcid.org/0000-0002-1017-9564)
- Guoshuai Shi (ORCID: https://orcid.org/0000-0001-9588-3368)
- Gang Du (ORCID: https://orcid.org/0009-0008-6106-9948)
- Tingyu Lu (ORCID: https://orcid.org/0000-0001-9665-6394)
- Shuzhou Li (ORCID: https://orcid.org/0000-0002-2159-2602)
- Ming‐Wei Chang (ORCID: https://orcid.org/0000-0002-0137-8895)
- Yuluo Shen
- Liming Zhang (ORCID: https://orcid.org/0000-0001-6795-3381)
- Jiyuan Liu (ORCID: https://orcid.org/0000-0001-7905-6282)
- Chunlei Yang
- Yeonhee Yun (ORCID: https://orcid.org/0009-0008-9676-3630)
- Yin Wang
- Xinyang Gao
Institutions
- East China University of Science and Technology (CN)
- Nanyang Technological University (SG)
- Fudan University (CN)
- Collaborative Innovation Center of Chemistry for Energy Materials (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-11-28
- DOI
- https://doi.org/10.1038/s41467-024-54630-2
- Citations
- 60
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 6.14
Funders
- National Natural Science Foundation of China
- East China University of Science and Technology
- Science and Technology Commission of Shanghai Municipality
- Ministry of Education, India
- Shanghai Rising-Star Program
- Fundamental Research Funds for the Central Universities
- National Supercomputing Center, Korea Institute of Science and Technology Information