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Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration

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Abstract

The electrochemical reduction of NO3− to NH3 holds promise for economic and environmental benefits, presenting an energy-efficient alternative to the traditional Haber–Bosch method. However, challenges exist due to its sluggish kinetics, multiple intermediates, and various reaction pathways. In this study, Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO3−-to-NH3 conversion. The doping of Mn into Cu resulted in exceptional performance, achieving a FE of 95.8% and an NH3 yield rate of 0.91 mol g−1 h−1 at −0.6 V in a neutral electrolyte at low NO3− concentration. Detailed experimental studies and theoretical calculations revealed that the Mn dopant enhanced the kinetic rate of NO2−-to-NH3 and induced a distinct configuration of *NO. This alteration decreased the energy barrier of *NO-to-*NOH, consequently promoting the conversion of NO3−-to-NH3.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (22293015, 22203099, and 22121002), Strategic Priority Research Program (A) of the Chinese Academy of Sciences (XDA0390400), and Photon Science Center for Carbon Neutrality. The X-ray absorption spectroscopy measurements were performed at Beamline 4B9A at Beijing Synchrotron Radiation Facility (BSRF).

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China

    Limin Wu, Shunhan Jia, Libing Zhang, Ruhan Wang, Xiaofu Sun & Buxing Han

  2. School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China

    Limin Wu, Shunhan Jia, Libing Zhang, Ruhan Wang, Xiaofu Sun & Buxing Han

  3. College of Chemical Engineering and Environment, China University of Petroleum, Beijing, 102249, China

    Jiaqi Feng

  4. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China

    Buxing Han

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  1. Limin Wu
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  2. Shunhan Jia
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  4. Ruhan Wang
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Correspondence to Xiaofu Sun or Buxing Han.

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Conflict of interest The authors declare no conflict of interest.

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Published in virtual special issue “Sustainable nitrogen chemistry”

Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

Supplementary Information

11426_2024_2040_MOESM1_ESM.pdf

Efficient Nitrate Electroreduction over Mn-doped Cu Catalyst via Regulating N-containing Intermediates Adsorption Configuration

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Wu, L., Jia, S., Zhang, L. et al. Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration. Sci. China Chem. (2024). https://doi.org/10.1007/s11426-024-2040-8

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  • DOI: https://doi.org/10.1007/s11426-024-2040-8

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