Issue 11, 2022

Atomically-dispersed NiN4–Cl active sites with axial Ni–Cl coordination for accelerating electrocatalytic hydrogen evolution

Abstract

Single-atom catalysts (SACs) regulated by heteroatoms have displayed great potential as electrocatalysts for highly efficient hydrogen evolution reaction (HER); however, the controllable synthesis of an axial coordination structure of SACs to achieve robust HER performance remains a great challenge. Herein, we have proposed a doping-adsorption-pyrolysis strategy to construct NiN4–Cl active sites with axial Cl coordination for accelerating electrocatalytic HER. The obtained NiN4–Cl SAs/NC catalyst exhibits superior HER activity with low over-potential, small Tafel slope, high turnover frequency, and long-term stability. Density functional theory calculation reveals that the excellent HER performance of NiN4–Cl SAs/NC originates from the axial Cl-coordination-induced electronic localization enhancement, which is beneficial for the adsorption and activation of H* intermediate, thus accelerating the HER process. This work opens a new opportunity for rational design and construction of high-performance SAC catalysts by axial coordination strategy for electrocatalytic application.

Graphical abstract: Atomically-dispersed NiN4–Cl active sites with axial Ni–Cl coordination for accelerating electrocatalytic hydrogen evolution

Supplementary files

Article information

Article type
Paper
Submitted
26 Sep 2021
Accepted
05 Dez 2021
First published
08 Dez 2021

J. Mater. Chem. A, 2022,10, 6007-6015

Atomically-dispersed NiN4–Cl active sites with axial Ni–Cl coordination for accelerating electrocatalytic hydrogen evolution

M. Li, M. Wang, D. Liu, Y. Pan, S. Liu, K. Sun, Y. Chen, H. Zhu, W. Guo, Y. Li, Z. Cui, B. Liu, Y. Liu and C. Liu, J. Mater. Chem. A, 2022, 10, 6007 DOI: 10.1039/D1TA08287F

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