期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 9, 期 3, 页码 1705-1712出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta08496d
关键词
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资金
- National Natural Science Foundation of China [21908090]
- Natural Science Foundation of Jiangxi Province [20192ACB21015]
The research demonstrates a hydrogen-bonding promoted strategy significantly enhances the efficiency of CO production on a Cu-N-C catalyst, showing potential application prospects in efficient CO2 electroreduction.
The ability to manipulate the binding strengths of intermediates on a catalyst is extremely challenging but essential for active and selective CO2 electroreduction (CO2RR). Single-atom copper anchored on a nitrogenated carbon (Cu-N-C) structure is still rarely unexplored for efficient CO production. Herein, we demonstrate a plausible hydrogen-bonding promoted strategy that significantly enhances the *COOH adsorption and facilitates the *CO desorption on a Cu-N-C catalyst. The as-prepared Cu-N-C catalyst with Cu-N-3 coordination achieves a high CO faradaic efficiency (FE) of 98% at -0.67 V (vs. reversible hydrogen electrode) as well as superior stability (FE remains above 90% over 20 h). Notably, in a three-phase flow cell configuration, a remarkable CO2 to CO FE of 99% at -0.67 V accompanying a large CO partial current density of 131.1 mA cm(-2) at -1.17 V was observed. Density functional theory calculations reveal that the Cu-N-3 coordination is potentially stabilized by an extended carbon plane with six nitrogen vacancies, while three unoccupied N sites are spontaneously saturated by protons during the CO2RR. Therefore, the hydrogen bonds formed between the adsorbed *COOH and adjacent protons significantly reduce the energy barrier of *COOH formation. After the first proton-coupled electron transfer process, the adsorbed *CO species are easily released to boost the CO production.
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