Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products
Abstract The recognition of the surface reconstruction of the catalysts during electrochemical CO2 reduction (CO2RR) is essential for exploring and comprehending active sites. Although the superior performance of Cu–Zn bimetallic sites toward multicarbon C2+ products has been established, the dynami...
| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2023-10-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202303726 |
| _version_ | 1797663864055136256 |
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| author | Yufei Jia Yunxuan Ding Tao Song Yunlong Xu Yaqing Li Lele Duan Fei Li Licheng Sun Ke Fan |
| author_facet | Yufei Jia Yunxuan Ding Tao Song Yunlong Xu Yaqing Li Lele Duan Fei Li Licheng Sun Ke Fan |
| author_sort | Yufei Jia |
| collection | DOAJ |
| description | Abstract The recognition of the surface reconstruction of the catalysts during electrochemical CO2 reduction (CO2RR) is essential for exploring and comprehending active sites. Although the superior performance of Cu–Zn bimetallic sites toward multicarbon C2+ products has been established, the dynamic surface reconstruction has not been fully understood. Herein, Zn‐doped Cu2O nano‐octahedrons are used to investigate the effect of the dynamic stability by the leaching and redeposition on CO2RR. Correlative characterizations confirm the Zn leaching from Zn‐doped Cu2O, which is redeposited at the surface of the catalysts, leading to dynamic stability and abundant Cu–Zn bimetallic sites at the surface. The reconstructed Zn‐doped Cu2O catalysts achieve a high Faradaic efficiency (FE) of C2+ products (77% at –1.1 V versus reversible hydrogen electrode (RHE)). Additionally, similar dynamic stability is also discovered in Al‐doped Cu2O for CO2RR, proving its universality in amphoteric metal‐doped catalysts. Mechanism analyses reveal that the OHC–CHO pathway can be the C–C coupling processes on bare Cu2O and Zn‐doped Cu2O, and the introduction of Zn to Cu can efficiently lower the energy barrier for CO2RR to C2H4. This research provides profound insight into unraveling surface dynamic reconstruction of amphoteric metal‐containing electrocatalysts and can guide rational design of the high‐performance electrocatalysts for CO2RR. |
| first_indexed | 2024-03-11T19:22:01Z |
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| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-03-11T19:22:01Z |
| publishDate | 2023-10-01 |
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| series | Advanced Science |
| spelling | doaj.art-4dd956a73e3d44c68bfda2b04f44c82d2023-10-07T03:51:49ZengWileyAdvanced Science2198-38442023-10-011028n/an/a10.1002/advs.202303726Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ ProductsYufei Jia0Yunxuan Ding1Tao Song2Yunlong Xu3Yaqing Li4Lele Duan5Fei Li6Licheng Sun7Ke Fan8State Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT‐KTH Joint Education and Research Centre on Molecular Devices Institute for Energy Science and Technology Dalian University of Technology Dalian 116024 P. R. ChinaCenter of Artificial Photosynthesis for Solar Fuels, Department of Chemistry School of Science Westlake University Hangzhou 310024 P. R. ChinaDepartment of Chemistry and Shenzhen Grubbs Institute Southern University of Science and Technology Shenzhen 518055 P. R. ChinaState Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT‐KTH Joint Education and Research Centre on Molecular Devices Institute for Energy Science and Technology Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT‐KTH Joint Education and Research Centre on Molecular Devices Institute for Energy Science and Technology Dalian University of Technology Dalian 116024 P. R. ChinaDepartment of Chemistry and Shenzhen Grubbs Institute Southern University of Science and Technology Shenzhen 518055 P. R. ChinaState Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT‐KTH Joint Education and Research Centre on Molecular Devices Institute for Energy Science and Technology Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT‐KTH Joint Education and Research Centre on Molecular Devices Institute for Energy Science and Technology Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis DUT‐KTH Joint Education and Research Centre on Molecular Devices Institute for Energy Science and Technology Dalian University of Technology Dalian 116024 P. R. ChinaAbstract The recognition of the surface reconstruction of the catalysts during electrochemical CO2 reduction (CO2RR) is essential for exploring and comprehending active sites. Although the superior performance of Cu–Zn bimetallic sites toward multicarbon C2+ products has been established, the dynamic surface reconstruction has not been fully understood. Herein, Zn‐doped Cu2O nano‐octahedrons are used to investigate the effect of the dynamic stability by the leaching and redeposition on CO2RR. Correlative characterizations confirm the Zn leaching from Zn‐doped Cu2O, which is redeposited at the surface of the catalysts, leading to dynamic stability and abundant Cu–Zn bimetallic sites at the surface. The reconstructed Zn‐doped Cu2O catalysts achieve a high Faradaic efficiency (FE) of C2+ products (77% at –1.1 V versus reversible hydrogen electrode (RHE)). Additionally, similar dynamic stability is also discovered in Al‐doped Cu2O for CO2RR, proving its universality in amphoteric metal‐doped catalysts. Mechanism analyses reveal that the OHC–CHO pathway can be the C–C coupling processes on bare Cu2O and Zn‐doped Cu2O, and the introduction of Zn to Cu can efficiently lower the energy barrier for CO2RR to C2H4. This research provides profound insight into unraveling surface dynamic reconstruction of amphoteric metal‐containing electrocatalysts and can guide rational design of the high‐performance electrocatalysts for CO2RR.https://doi.org/10.1002/advs.202303726amphoteric metal‐doped Cu2OCO2 reductionelectrocatalysisleachingredeposition |
| spellingShingle | Yufei Jia Yunxuan Ding Tao Song Yunlong Xu Yaqing Li Lele Duan Fei Li Licheng Sun Ke Fan Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products Advanced Science amphoteric metal‐doped Cu2O CO2 reduction electrocatalysis leaching redeposition |
| title | Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products |
| title_full | Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products |
| title_fullStr | Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products |
| title_full_unstemmed | Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products |
| title_short | Dynamic Surface Reconstruction of Amphoteric Metal (Zn, Al) Doped Cu2O for Efficient Electrochemical CO2 Reduction to C2+ Products |
| title_sort | dynamic surface reconstruction of amphoteric metal zn al doped cu2o for efficient electrochemical co2 reduction to c2 products |
| topic | amphoteric metal‐doped Cu2O CO2 reduction electrocatalysis leaching redeposition |
| url | https://doi.org/10.1002/advs.202303726 |
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