Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products
Abstract Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology....
| Main Authors: | , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-10-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-41871-w |
| _version_ | 1797558545050238976 |
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| author | Cheng Du Joel P. Mills Asfaw G. Yohannes Wei Wei Lei Wang Siyan Lu Jian-Xiang Lian Maoyu Wang Tao Guo Xiyang Wang Hua Zhou Cheng-Jun Sun John Z. Wen Brian Kendall Martin Couillard Hongsheng Guo ZhongChao Tan Samira Siahrostami Yimin A. Wu |
| author_facet | Cheng Du Joel P. Mills Asfaw G. Yohannes Wei Wei Lei Wang Siyan Lu Jian-Xiang Lian Maoyu Wang Tao Guo Xiyang Wang Hua Zhou Cheng-Jun Sun John Z. Wen Brian Kendall Martin Couillard Hongsheng Guo ZhongChao Tan Samira Siahrostami Yimin A. Wu |
| author_sort | Cheng Du |
| collection | DOAJ |
| description | Abstract Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm−2 working current density at −0.65 V in a flow cell with alkaline electrolyte. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain. |
| first_indexed | 2024-03-10T17:32:56Z |
| format | Article |
| id | doaj.art-c5dc1754313445bd8311d4c504052466 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-10T17:32:56Z |
| publishDate | 2023-10-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-c5dc1754313445bd8311d4c5040524662023-11-20T09:58:41ZengNature PortfolioNature Communications2041-17232023-10-0114111010.1038/s41467-023-41871-wCascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon productsCheng Du0Joel P. Mills1Asfaw G. Yohannes2Wei Wei3Lei Wang4Siyan Lu5Jian-Xiang Lian6Maoyu Wang7Tao Guo8Xiyang Wang9Hua Zhou10Cheng-Jun Sun11John Z. Wen12Brian Kendall13Martin Couillard14Hongsheng Guo15ZhongChao Tan16Samira Siahrostami17Yimin A. Wu18Department of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Chemistry, University of CalgaryDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Chemistry, University of CalgaryX-Ray Science Division, Argonne National LaboratoryDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooX-Ray Science Division, Argonne National LaboratoryX-Ray Science Division, Argonne National LaboratoryDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Earth and Environmental Sciences, University of WaterlooEnergy, Mining and Environment Research Center, National Research Council CanadaEnergy, Mining and Environment Research Center, National Research Council CanadaDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooDepartment of Chemistry, University of CalgaryDepartment of Mechanical and Mechatronics Engineering, Waterloo Institute for Nanotechnology, Materials Interfaces Foundry, University of WaterlooAbstract Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm−2 working current density at −0.65 V in a flow cell with alkaline electrolyte. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain.https://doi.org/10.1038/s41467-023-41871-w |
| spellingShingle | Cheng Du Joel P. Mills Asfaw G. Yohannes Wei Wei Lei Wang Siyan Lu Jian-Xiang Lian Maoyu Wang Tao Guo Xiyang Wang Hua Zhou Cheng-Jun Sun John Z. Wen Brian Kendall Martin Couillard Hongsheng Guo ZhongChao Tan Samira Siahrostami Yimin A. Wu Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products Nature Communications |
| title | Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products |
| title_full | Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products |
| title_fullStr | Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products |
| title_full_unstemmed | Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products |
| title_short | Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products |
| title_sort | cascade electrocatalysis via agcu single atom alloy and ag nanoparticles in co2 electroreduction toward multicarbon products |
| url | https://doi.org/10.1038/s41467-023-41871-w |
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