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As one of the most promising CO2 utilization techniques, electrochemical CO2 reduction has recently received considerable attention. Cu is a unique electrocatalyst that can convert CO2 to value-added multi-carbon chemicals. Nevertheless, Cu catalysts are always limited by the poor selectivity and stability. Here, we report that using copper-tetracyanoquinodimethane (CuTCNQ) derived Cu nanoparticles as efficient electrocatalysts for conversion of CO2 to ethylene characteristic with high selectivity and stability, showing 56% Faradaic efficiency (FE) to C2H4 at −1.3 V vs. reversible hydrogen electrode (RHE). Upon the electrochemical CO2 reduction, CuTCNQ slowly reconstructs to Cu nanoparticles with abundant grain boundaries and residual Cu+ on the surface. Theoretical calculation and operando characterization disclose that both as-formed Cu nanoparticle grain boundaries and residual Cu+ endow the catalyst with high selectivity toward ethylene. Furthermore, during the reconstruction of CuTCNQ to Cu nanoparticles, the grain boundaries Cu surface is slowly refreshed by continual addition of Cu atoms, thus inhibiting the surface passivation and guaranteeing the electrocatalytic stability.

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Publication history

Received: 20 March 2022
Revised: 17 April 2022
Accepted: 19 April 2022
Published: 08 June 2022
Issue date: September 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

The authors acknowledge financial support from the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB36000000, Z. Y. T.), National Key Basic Research Program of China (No. 2021YFA1200302, Z. Y. T.), and National Natural Science Foundation of China (Nos. 92056204, 21890381, and 21721002, Z. Y. T.). The authors wish to thank support of 1W1B and 4B9A beamline of Beijing Synchrotron Radiation Facility (BSRF).

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Email: nanores@tup.tsinghua.edu.cn

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