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 ~100% Faradaic efficiency (FE) at the overpotentials of 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.
Original language | English (US) |
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Journal | Research |
DOIs | |
State | Published - Feb 1 2023 |
Bibliographical note
KAUST Repository Item: Exported on 2023-02-08Acknowledgements: This work was supported by the National Key R&D Program of China (2021YFA1500402), the National Natural Science Foundation of China (NSFC) (22105203 and 22175174), the Natural Science Foundation of Fujian Province (2020J01116 and 2021J06033) and the China Postdoctoral Science Foundation (2021TQ0332 and 2021M703215).