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 (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 A...
| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2025
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| Online Access: | https://hdl.handle.net/10356/182038 |
| _version_ | 1826117555510575104 |
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| author | Gao, Xinyang Jiang, Yongjun Liu, Jiyuan Shi, Guoshuai Yang, Chunlei Xu, Qinshang Yun, Yuanqing Shen, Yuluo Chang, Mingwei Zhu, Chenyuan Lu, Tingyu Wang, Yin Du, Guanchen Li, Shuzhou Dai, Sheng Zhang, Liming |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Gao, Xinyang Jiang, Yongjun Liu, Jiyuan Shi, Guoshuai Yang, Chunlei Xu, Qinshang Yun, Yuanqing Shen, Yuluo Chang, Mingwei Zhu, Chenyuan Lu, Tingyu Wang, Yin Du, Guanchen Li, Shuzhou Dai, Sheng Zhang, Liming |
| author_sort | Gao, Xinyang |
| collection | NTU |
| description | 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. |
| first_indexed | 2025-03-09T11:56:51Z |
| format | Journal Article |
| id | ntu-10356/182038 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-03-09T11:56:51Z |
| publishDate | 2025 |
| record_format | dspace |
| spelling | ntu-10356/1820382025-01-10T15:50:27Z Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels Gao, Xinyang Jiang, Yongjun Liu, Jiyuan Shi, Guoshuai Yang, Chunlei Xu, Qinshang Yun, Yuanqing Shen, Yuluo Chang, Mingwei Zhu, Chenyuan Lu, Tingyu Wang, Yin Du, Guanchen Li, Shuzhou Dai, Sheng Zhang, Liming School of Materials Science and Engineering Engineering Electrochemical method Reduction 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. Ministry of Education (MOE) National Supercomputing Centre (NSCC) Singapore Published version 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. 2025-01-06T04:46:13Z 2025-01-06T04:46:13Z 2024 Journal Article Gao, X., Jiang, Y., Liu, J., Shi, G., Yang, C., Xu, Q., Yun, Y., Shen, Y., Chang, M., Zhu, C., Lu, T., Wang, Y., Du, G., Li, S., Dai, S. & Zhang, L. (2024). Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels. Nature Communications, 15(1), 10331-. https://dx.doi.org/10.1038/s41467-024-54630-2 2041-1723 https://hdl.handle.net/10356/182038 10.1038/s41467-024-54630-2 39609452 2-s2.0-85211177826 1 15 10331 en MOE-T2EP10220-0005 MOE-T2EP20221-0004 RG5/22) Nature Communications © 2024 The Author(s). Open Access. This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http:// creativecommons.org/licenses/by-nc-nd/4.0/. application/pdf |
| spellingShingle | Engineering Electrochemical method Reduction Gao, Xinyang Jiang, Yongjun Liu, Jiyuan Shi, Guoshuai Yang, Chunlei Xu, Qinshang Yun, Yuanqing Shen, Yuluo Chang, Mingwei Zhu, Chenyuan Lu, Tingyu Wang, Yin Du, Guanchen Li, Shuzhou Dai, Sheng Zhang, Liming Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels |
| title | Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels |
| title_full | Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels |
| title_fullStr | Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels |
| title_full_unstemmed | Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels |
| title_short | Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels |
| title_sort | intermediate regulated dynamic restructuring at ag cu biphasic interface enables selective co2 electroreduction to c2 fuels |
| topic | Engineering Electrochemical method Reduction |
| url | https://hdl.handle.net/10356/182038 |
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