Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction
Abstract Designing asymmetrical structures is an effective strategy to optimize metallic catalysts for electrochemical carbon dioxide reduction reactions. Herein, we demonstrate a transient pulsed discharge method for instantaneously constructing graphene-aerogel supports asymmetric copper nanoclust...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56534-1 |
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| author | Kaiyuan Liu Hao Shen Zhiyi Sun Qiang Zhou Guoqiang Liu Zhongti Sun Wenxing Chen Xin Gao Pengwan Chen |
| author_facet | Kaiyuan Liu Hao Shen Zhiyi Sun Qiang Zhou Guoqiang Liu Zhongti Sun Wenxing Chen Xin Gao Pengwan Chen |
| author_sort | Kaiyuan Liu |
| collection | DOAJ |
| description | Abstract Designing asymmetrical structures is an effective strategy to optimize metallic catalysts for electrochemical carbon dioxide reduction reactions. Herein, we demonstrate a transient pulsed discharge method for instantaneously constructing graphene-aerogel supports asymmetric copper nanocluster catalysts. This process induces the convergence of copper atoms decomposed by copper chloride onto graphene originating from the intense current pulse and high temperature. The catalysts exhibit asymmetrical atomic and electronic structures due to lattice distortion and oxygen doping of copper clusters. In carbon dioxide reduction reaction, the selectivity and activity for ethanol production are enhanced by the asymmetric structure and abundance of active sites on catalysts, achieving a Faradaic efficiency of 75.3% for ethanol and 90.5% for multicarbon products at −1.1 V vs. reversible hydrogen electrode. Moreover, the strong interactions between copper nanoclusters and graphene-aerogel support confer notable long-term stability. We elucidate the key reaction intermediates and mechanisms on Cu4O-Cu/C2O1 moieties through in situ testing and density functional theory calculations. This study provides an innovative approach to balancing activity and stability in asymmetric-structure catalysts for energy conversion. |
| format | Article |
| id | doaj-art-35bbb8a043f14e87b4d1d15bea9ebc23 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-35bbb8a043f14e87b4d1d15bea9ebc232025-02-02T12:31:16ZengNature PortfolioNature Communications2041-17232025-01-0116111310.1038/s41467-025-56534-1Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreductionKaiyuan Liu0Hao Shen1Zhiyi Sun2Qiang Zhou3Guoqiang Liu4Zhongti Sun5Wenxing Chen6Xin Gao7Pengwan Chen8School of Mechatronical Engineering, Beijing Institute of TechnologySchool of Materials Science and Engineering, Jiangsu UniversityEnergy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of TechnologyChina Academy of Ordnance ScienceSchool of Materials Science and Engineering, Anhui University of TechnologySchool of Materials Science and Engineering, Jiangsu UniversityEnergy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of TechnologySchool of Mechatronical Engineering, Beijing Institute of TechnologySchool of Mechatronical Engineering, Beijing Institute of TechnologyAbstract Designing asymmetrical structures is an effective strategy to optimize metallic catalysts for electrochemical carbon dioxide reduction reactions. Herein, we demonstrate a transient pulsed discharge method for instantaneously constructing graphene-aerogel supports asymmetric copper nanocluster catalysts. This process induces the convergence of copper atoms decomposed by copper chloride onto graphene originating from the intense current pulse and high temperature. The catalysts exhibit asymmetrical atomic and electronic structures due to lattice distortion and oxygen doping of copper clusters. In carbon dioxide reduction reaction, the selectivity and activity for ethanol production are enhanced by the asymmetric structure and abundance of active sites on catalysts, achieving a Faradaic efficiency of 75.3% for ethanol and 90.5% for multicarbon products at −1.1 V vs. reversible hydrogen electrode. Moreover, the strong interactions between copper nanoclusters and graphene-aerogel support confer notable long-term stability. We elucidate the key reaction intermediates and mechanisms on Cu4O-Cu/C2O1 moieties through in situ testing and density functional theory calculations. This study provides an innovative approach to balancing activity and stability in asymmetric-structure catalysts for energy conversion.https://doi.org/10.1038/s41467-025-56534-1 |
| spellingShingle | Kaiyuan Liu Hao Shen Zhiyi Sun Qiang Zhou Guoqiang Liu Zhongti Sun Wenxing Chen Xin Gao Pengwan Chen Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction Nature Communications |
| title | Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction |
| title_full | Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction |
| title_fullStr | Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction |
| title_full_unstemmed | Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction |
| title_short | Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction |
| title_sort | transient pulsed discharge preparation of graphene aerogel supports asymmetric cu cluster catalysts promote co2 electroreduction |
| url | https://doi.org/10.1038/s41467-025-56534-1 |
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