Title | Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials |
Author | |
Corresponding Author | Cao, Changsheng |
Publication Years | 2023-02-01
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Source Title | |
ISSN | 2096-5168
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EISSN | 2639-5274
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Volume | 2023 |
Abstract | Transition metal-based single-atom catalysts (TM-SACs) are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO2 reduction reaction. However, developing TM-SACs with high activity and selectivity at low overpotentials is challenging. Herein, a novel Fe-based SAC with Si doping (Fe-N-C-Si) was prepared, which shows a record-high electrocatalytic performance toward the CO2-to-CO conversion with exceptional current density (> 350.0 mA cm(-2)) and similar to 100% Faradaic efficiency (FE) at the overpotentials of < 400 mV, far superior to the reported Fe-based SACs. Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO2 battery delivers an outstanding performance with a maximal power density of 2.44 mW cm(-2) at the output voltage of 0.30 V, as well as the high cycling stability and FE (> 90%) for CO production. Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulates the electronic structure of the atomic Fe sites in Fe-N-C-Si to significantly accelerate the key pathway involving *CO intermediate desorption, inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO2RR performance. This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on single-atom sites to improve their electrocatalytic performance. |
URL | [Source Record] |
Indexed By | |
Language | English
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SUSTech Authorship | Others
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Funding Project | National Key R&D Program of China[2021YFA1500402]
; National Natural Science Foundation of China (NSFC)["22105203","22175174"]
; Natural Science Foundation of Fujian Province["2020J01116","2021J06033"]
; China Postdoctoral Science Foundation["2021TQ0332","2021M703215"]
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WOS Research Area | Science & Technology - Other Topics
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WOS Subject | Multidisciplinary Sciences
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WOS Accession No | WOS:000928828300001
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Publisher | |
Data Source | Web of Science
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Citation statistics |
Cited Times [WOS]:3
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Document Type | Journal Article |
Identifier | http://kc.sustech.edu.cn/handle/2SGJ60CL/489998 |
Department | Southern University of Science and Technology 工学院_材料科学与工程系 |
Affiliation | 1.Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China 2.Fujian Sci & Technol Innovat Lab Optoelect Informa, Fuzhou 350108, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.King Abdullah Univ Sci & Technol KAUST, KAUST Catalysis Ctr KCC, Thuwal 239556900, Saudi Arabia 5.City Univ Hong Kong, Dept Chem, Hong Kong 999077, Peoples R China 6.Chinese Acad Sci, CAS Key Lab Design & Assembly Funct Nanostruct, Fujian Struct Matter, Fuzhou 350002, Peoples R China 7.Kyoto Univ, Inst Integrated Cell Mat Sci iCeMS, Kyoto 6068501, Japan 8.SUSTech Kyoto Univ Adv Energy Mat Joint Innovat La, Shenzhen Key Lab Micro Nanoporous Funct Mat SKLPM, Shenzhen 518055, Peoples R China 9.Southern Univ Sci & Technol SUSTech, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China |
Recommended Citation GB/T 7714 |
Cao, Changsheng,Zhou, Shenghua,Zuo, Shouwei,et al. Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials[J]. RESEARCH,2023,2023.
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APA |
Cao, Changsheng.,Zhou, Shenghua.,Zuo, Shouwei.,Zhang, Huabin.,Chen, Bo.,...&Zhu, Qi-Long.(2023).Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials.RESEARCH,2023.
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MLA |
Cao, Changsheng,et al."Si-doping induced electronic structure regulation of single-atom Fe sites for boosted CO2 electroreduction at low overpotentials".RESEARCH 2023(2023).
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