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Efficient electroreduction of CO2 into CO and other chemicals turns greenhouse gases into fuels and value-added chemicals, holding great promise for a closed carbon cycle and the alleviation of climate changes. However, there are still challenges in the large-scale application of CO2 electroreduction due to the sluggish kinetics. Herein we develop a self-assembly strategy to synthesize a highly efficient CO2 reduction electrocatalyst with atomically dispersed Ni-N4 active centers anchored on polymer-derived mesh-like N-doped carbon nanofibers (Ni-N4/NC). The Ni-N4/NC exhibits high selectivity for CO2 reduction reaction with CO Faradaic efficiency (CO FE) above 90% over a wide potential range from −0.6 to −1.0 V vs. RHE. The catalyst reaches a maximum CO FE up to 98.4% at −0.8 V with a TOF of 1.28 x 105 h–1 and Tafel slope of 113 mV·dec–1. The catalyst also exhibits remarkable stability, with little change in current density and CO FE over a 10-hour durability test at –0.8 V vs. RHE. This method provides a new route for the synthesis of highly efficient CO2 reduction electrocatalyst.

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Publication history
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Acknowledgements

Publication history

Received: 30 August 2021
Revised: 11 December 2021
Accepted: 15 December 2021
Published: 15 January 2022
Issue date: May 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2018YFA0702003), the National Natural Science Foundation of China (Nos. 21890383 and 21971137) and Beijing Municipal Science & Technology Commission (No. Z191100007219003).

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