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Research Article

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

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.

Show Author Information

Graphical Abstract

The atomic-level interfacial regulation of transition metal single-site catalysts (SSCs) through heteroatom doping can significantly improve the characteristics and obtain surprising catalytic activity. P and N dual-coordinated Ni SSCs were designed for electrocatalytic CO2 reduction reaction (CO2RR) to CO. The catalytic activity and selectivity of Ni-P1N3 were both higher than those of P-free catalysts. This work provides a new type of highly efficient SSCs for CO2RR.

Abstract

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.

Keywords

nickel single-site catalystsasymmetric coordinationCO2 reduction reactionatomic interface

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Nano Research
Volume 16 Issue 2,
February 2023
Pages 2170-2176
DOI: 10.1007/s12274-022-4969-z
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
Topics:
Electrocatalysis

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Received: 07 August 2022
Revised: 24 August 2022
Accepted: 25 August 2022
Published: 12 October 2022
© Tsinghua University Press 2022
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