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Electrochemical CO2 reduction reaction (CO2RR) into value-added chemicals/fuels is crucial for realizing the sustainable carbon cycle while mitigating the energy crisis. However, it is impeded by the relatively high overpotential and low energy efficiency due to the lack of efficient electrocatalysts. Herein, we develop an isolated single-atom Ni catalyst regulated strategy to activate and stabilize the iron phthalocyanine molecule (Ni SA@FePc) toward a highly efficient CO2RR process at low overpotential. The well-defined and homogenous catalytic centers with unique structures confer Ni SA@FePc with a significantly enhanced CO2RR performance compared to single-atom Ni catalyst and FePc molecule and afford the atomic understanding on active sites and catalytic mechanism. As expected, Ni SA@FePc exhibits a high selectivity of more significant Faraday efficiency (≥ 95%) over a wide potential range, a high current density of ~ 252 mA·cm−2 at low overpotential (390 mV), and excellent long-term stability for CO2RR to CO. X-ray absorption spectroscopy measurement and theoretical calculation indicate the formation of NiN4-O2-FePc heterogeneous structure for Ni SA@FePc. And CO2RR prefers to occur at the raised N centers of NiN4-O2-FePc heterogeneous structure for Ni SA@FePc, which enables facilitated adsorption of *COOH and desorption of CO, and thus accelerated overall reaction kinetics.

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Publication history
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Acknowledgements

Publication history

Received: 09 January 2022
Revised: 24 January 2022
Accepted: 25 January 2022
Published: 18 April 2022
Issue date: July 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

H. X. Z. acknowledges funding from the Alexander von Humboldt Foundation. This work was supported by the National Natural Science Foundation of China (No. 21725103), National Key R&D Program of China (No. 2019YFA0705704), the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDA21010210), Jilin Province Science and Technology Development Plan Funding Project (No. 20200201079JC), Changchun Science and Technology Development Plan Funding Project (No. 19SS010), Jilin Province Capital Construction Funds Project (No. 2020C026-1), and the K. C. Wong Education Foundation (No. GJTD-2018-09).

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