Autor: |
Changsheng Cao, Shenghua Zhou, Shouwei Zuo, Huabin Zhang, Bo Chen, Junheng Huang, Xin-Tao Wu, Qiang Xu, Qi-Long Zhu |
Jazyk: |
angličtina |
Rok vydání: |
2023 |
Předmět: |
|
Zdroj: |
Research, Vol 6 (2023) |
Druh dokumentu: |
article |
ISSN: |
2639-5274 |
DOI: |
10.34133/research.0079 |
Popis: |
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 ~100% Faradaic efficiency (FE) at the overpotential of 90%) for CO production. Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly 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. |
Databáze: |
Directory of Open Access Journals |
Externí odkaz: |
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