Promoting Electrochemical CO_2 Reduction via Boosting Activation of Adsorbed Intermediates on Iron Single-Atom Catalyst

Chen Jiayi; Wang Tingting; Wang XinyueYang BinSang XiahanZheng SixingYao SiyuLi ZhongjianZhang QinghuaLei LechengXu JiangDai LimingHou Yang

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Promoting Electrochemical CO_2 Reduction via Boosting Activation of Adsorbed Intermediates on Iron Single-Atom Catalyst

机译：Promoting Electrochemical CO_2 Reduction via Boosting Activation of Adsorbed Intermediates on Iron Single-Atom Catalyst

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Single-atom catalysts show great promise as non-precious electrocatalysts for CO2 electroreduction reaction (CO2ER). However, it is still challenging to gain a fundamental understanding of the complicated dynamic behavior of CO2 activation to achieve high product selectivity. Herein, the authors report an unusual iron single-atom catalyst, containing atomically dispersed Fe-N-4 species and Fe3C nanoparticles (NPs) (Fe3C|Fe1N4). Having a fragmental-rock-shaped nanocarbon architecture, isolated Fe-N-4 sites uniformly disperse with adjacent Fe3C NPs (30 nm) in a carbon matrix. Benefiting from the strong coupling effect between Fe3C and Fe1N4 and unique spatial nanostructure, Fe3C|Fe1N4 displays exceptional CO2ER activity with a low onset potential of -0.3 V and high Faradaic efficiency of 94.6% at -0.5 V for CO production, acting as one of the most active Fe-N-C catalysts and even exceeding most other carbon supported non-precious metal NPs. Experimental observations discover that the excellent CO2ER activity of Fe3C|Fe1N4 catalyst is attributable to the presence of Fe3C NPs that optimizes J(CO) of the coexisted Fe-N-4 active sites. In situ attenuated total reflectance-Fourier transform infrared analysis and theoretical calculations reveal that the Fe3C NPs strengthen the adsorption of CO2 on the isolated Fe-N-4 sites to accelerate the formation of *COOH intermediate, and hence enhance the whole CO2ER performance.

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《Advanced functional materials》 |2022年第21期|2110174.1-2110174.9|共9页
作者
Chen Jiayi; Wang Tingting; Wang XinyueYang BinSang XiahanZheng SixingYao SiyuLi ZhongjianZhang QinghuaLei LechengXu JiangDai LimingHou Yang;
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作者单位

Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China;

Wuhan Univ Technol, Sch Mat Sci & Engn, Res & Testing Ctr Mat, Wuhan 430070, Peoples R China;

Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China|Inst Zhejiang Univ Quzhou, Quzhou 324000, Peoples R ChinaZhejiang Univ, Coll Environm & Resource Sci, Hangzhou 310058, Peoples R ChinaUniv New South Wales, Sch Chem Engn, Sydney, NSW 2052, Australia;

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atomic Fe-N; (4) sites; CO; (2) electroreduction; nanostructured Fe; C-3; strengthen CO; (2) adsorption; Zn-CO; (2) batteries;

Promoting Electrochemical CO_2 Reduction via Boosting Activation of Adsorbed Intermediates on Iron Single-Atom Catalyst

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