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Nano Research 2023, 16(2): 2170-2176 https://doi.org/10.1007/s12274-022-4969-z
Research Article | Issue | Published: 12 October 2022

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

Show Author's Information Ming Qu1,§,  Zhe Chen2,§,  Zhiyi Sun3,§,  Danni Zhou3,  Wenjing Xu3,  Hao Tang3,  Hongfei Gu3,  Tuo Liang1,  Pengfei Hu4,5,  Guangwen Li6,  Yu Wang7,  Zhuo Chen3( ),  Tao Wang2( ),  Binbin Jia4( )
Unconventional Petroleum Research Institute, China University of Petroleum (Beijing), Beijing 102249, China
Center of Artificial Photosynthesis for Solar Fuels, School of Science, Westlake University, Hangzhou 310024, China
Energy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
School of Chemistry, Beihang University, Beijing 100191, China
Research Institute of Aero-Engine, Beihang University, Beijing 102206, China
Research Institude of Petroleum Processing, Sinopec Group (SINOPEC), Beijing 100083, China
Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai 201204, China

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

Keywords:
CO2 reduction reaction, asymmetric coordination, nickel single-site catalysts, atomic interface
Topics:
Electrocatalysis
Cite this article:
Qu M, Chen Z, Sun Z, et al. Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO2 reduction. Nano Research, 2023, 16(2): 2170-2176. https://doi.org/10.1007/s12274-022-4969-z
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Abstract Electronic supplementary material About this article

The atomic-level interfacial regulation of single metal sites through heteroatom doping 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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Publication history
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Acknowledgements

Publication history

Received: 07 August 2022
Revised: 24 August 2022
Accepted: 25 August 2022
Published: 12 October 2022
Issue date: February 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the Beijing 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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