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Coupling Ni–Cu atomic pair to promote CO2 electroreduction with near-unity CO selectivity

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Abstract

The electrocatalytic reduction of CO2 towards CO is one of the most desirable routines to reduce atmospheric CO2 concentration and maintain a global carbon balance. In this work, a novel porous NiCu-embedded ZIF-derived N-doped carbon nanoparticle (NiCu@NCNPs) catalyst has been identified as an active, highly selective, stable, and cost-effective catalyst in CO2 reduction. A CO selectivity as high as 100% has been achieved on NiCu@NCNPs which is the highest reported to date. The particle current density of CO on NiCu@NCNPs is around 15 mA cm–2 under the optimized potential at −0.9 V vs. RHE. The NiCu@NCNPs electrode also exhibits excellent stability during the five sequential CO2 electroreduction experiments. The superior catalytic performance of NiCu@NCNPs in CO2RR can be related to its microstructure with high electrochemical surface area and low electron transfer resistance. Furthermore, a kinetic analysis has shown the formation of intermediate *COOH is the rate-determining step in CO2RR towards CO. According to the results of density functional theory (DFT) calculations, a low Gibbs-free energy change (∆G) for the rate-determining step leads to the enhanced catalytic performance of CO2RR on NiCu@NCNPs.

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Data obtained and analyzed in this study are included in this article and available on reasonable request from the corresponding author.

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Funding

This work was supported by the National Natural Science Foundation of China (Grants 21908199 and 22076168), the Fundamental Research Funds for the Provincial Universities of Zhejiang (Grant RF-A2020011), and Zhejiang Soft Science Research Program (Grant 2022C15006).

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Authors and Affiliations

  1. College of Environment, Zhejiang University of Technology, Hangzhou, 310032, People’s Republic of China

    Weiting Yu, Jieyun Zhu, Sizhuo Chen, Juntao Tang, Jiexu Ye & Shuang Song

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  1. Weiting Yu
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  2. Jieyun Zhu
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  3. Sizhuo Chen
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  4. Juntao Tang
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  5. Jiexu Ye
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  6. Shuang Song
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Contributions

Weiting Yu: supervision and writing. Jieyun Zhu: data curation and investigation. Sizhuo Chen: formal analysis. Juntao Tang: validation. Jiexu Ye: validation. Shuang Song: supervision and resources.

Corresponding author

Correspondence to Shuang Song.

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The authors have not submitted the manuscript to a preprint server before submitting it to Environmental Science and Pollution Research. This work is not under consideration for publication anywhere else and is approved by all co-authors for publication in Environmental Science and Pollution Research.

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Yu, W., Zhu, J., Chen, S. et al. Coupling Ni–Cu atomic pair to promote CO2 electroreduction with near-unity CO selectivity. Environ Sci Pollut Res 30, 51876–51886 (2023). https://doi.org/10.1007/s11356-023-25975-w

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