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Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO2 reduction

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Abstract

The atomic-level interfacial regulation of single metal sites through heteroatom do** can significantly improve the characteristics of the catalyst and obtain surprising activity. Herein, nickel single-site catalysts (SSCs) with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed (denoted as Ni-PxNy, x = 1, 2 and y = 3, 2). In CO2 reduction reaction (CO2RR), the CO current density on Ni-PxNy was significantly higher than that of Ni-N4 catalyst without phosphorus modification. Besides, Ni-P1N3 performed the highest CO Faradaic efficiency (FECO) of 85.0%–98.0% over a wide potential range of −0.65 to −0.95 V (vs. the reversible hydrogen electrode (RHE)). Experimental and theoretical results revealed that the asymmetric Ni-P1N3 site was beneficial to CO2 intermediate adsorption/desorption, thereby accelerating the reaction kinetics and boosting CO2RR activity. This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance, targetting to CO2RR applications.

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Acknowledgements

This work was supported by the Bei**g Natural Science Foundation (No. 2212018), China National Petroleum Corporation (CNPC) Innovation Found (No. 2021DQ02-0202), and the National Natural Science Foundation of China (No. 51902013). The authors thank the BL14W1 in the Shanghai Synchrotron Radiation Facility (SSRF), and BL10B and BL12B in the National Synchrotron Radiation Laboratory (NSRL) for help with characterizations. T. W. also acknowledges the start-up fund of Westlake University and Westlake University High Performance Computing (HPC) Center for computation support.

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  1. Ming Qu, Zhe Chen, and Zhiyi Sun contributed equally to this work.

Authors and Affiliations

  1. Unconventional Petroleum Research Institute, China University of Petroleum (Bei**g), Bei**g, 102249, China

    Ming Qu & Tuo Liang

  2. Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou, 310024, China

    Zhe Chen & Tao Wang

  3. Energy & Catalysis Center, School of Materials Science and Engineering, Bei**g Institute of Technology, Bei**g, 100081, China

    Zhiyi Sun, Danni Zhou, Wen**g Xu, Hao Tang, Hongfei Gu & Zhuo Chen

  4. School of Chemistry, Beihang University, Bei**g, 100191, China

    Pengfei Hu & Binbin Jia

  5. Research Institute of Aero-Engine, Beihang University, Bei**g, 102206, China

    Pengfei Hu

  6. Research Institude of Petroleum Processing, Sinopec Group (SINOPEC), Bei**g, 100083, China

    Guangwen Li

  7. Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, 201204, China

    Yu Wang

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Qu, M., Chen, Z., Sun, Z. et al. Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO2 reduction. Nano Res. 16, 2170–2176 (2023). https://doi.org/10.1007/s12274-022-4969-z

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