Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO2 Electroreduction at Low Overpotentials

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