Issue 14, 2022

Doping-engineered biphenylene as a metal-free electrocatalyst for the hydrogen evolution reaction

Abstract

The rational design of metal-free electrocatalysts with excellent catalytic activity and high chemical stability is at the core of large-scale hydrogen production from water splitting. Herein, using first-principles calculations, we investigated the hydrogen evolution reaction (HER) electrocatalytic activity of X-doped (X = B, N, P, S) biphenylene (BPN). BPN was successfully synthesized experimentally and our results show that heteroatom doping can effectively enhance the electrocatalytic activity towards the HER. The β-site P-doped BPN has an optimal Gibbs free energy for hydrogen (ΔGH*) value of 0.01 eV and excellent exchange current density (−1.48 A cm−2). In addition, we also revealed that the electrocatalytic activity is better when the heteroatom replaces a β-site C atom instead of an α-site C atom. According to the results of the band structure of X-doped BPN, P atom doping can enhance the charge transfer from hydrogen to C atoms, corresponding to an appropriate p-band center. Furthermore, we demonstrated that P-doped BPN prefers the Volmer–Heyrovsky mechanism for the HER, and the reaction energy barrier is only 0.8 eV. Our work provides a strategy for designing a new metal-free HER electrocatalyst, which is predicted to be employed in HER catalysis with low cost and high performance.

Graphical abstract: Doping-engineered biphenylene as a metal-free electrocatalyst for the hydrogen evolution reaction

Article information

Article type
Paper
Submitted
11 May 2022
Accepted
13 Jun 2022
First published
13 Jun 2022

Sustainable Energy Fuels, 2022,6, 3446-3452

Doping-engineered biphenylene as a metal-free electrocatalyst for the hydrogen evolution reaction

J. Hao, Z. Zhao, C. Chen, C. Zhang, L. Li, S. Gao, B. Jia and P. Lu, Sustainable Energy Fuels, 2022, 6, 3446 DOI: 10.1039/D2SE00658H

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