Precisely Control Relationship between Sulfur Vacancy and H Absorption for Boosting Hydrogen Evolution Reaction

Jing Jin; Xinyao Wang; Yang Hu; Zhuang Zhang; Hongbo Liu; Jie Yin; Pinxian Xi

doi:10.1007/s40820-023-01291-3

Precisely Control Relationship between Sulfur Vacancy and H Absorption for Boosting Hydrogen Evolution Reaction

Nanomicro Lett. 2024 Jan 2;16(1):63. doi: 10.1007/s40820-023-01291-3.

Authors

Jing Jin^#¹, Xinyao Wang^#¹, Yang Hu¹, Zhuang Zhang¹, Hongbo Liu¹, Jie Yin², Pinxian Xi³

Affiliations

¹ College of Chemistry and Chemical Engineering, Frontiers Science Center for Rare Isotopes, State Key Laboratory of Applied Organic Chemistry, Lanzhou University, Lanzhou, 730000, People's Republic of China.
² College of Chemistry and Chemical Engineering, Frontiers Science Center for Rare Isotopes, State Key Laboratory of Applied Organic Chemistry, Lanzhou University, Lanzhou, 730000, People's Republic of China. yinj@lzu.edu.cn.
³ College of Chemistry and Chemical Engineering, Frontiers Science Center for Rare Isotopes, State Key Laboratory of Applied Organic Chemistry, Lanzhou University, Lanzhou, 730000, People's Republic of China. xipx@lzu.edu.cn.

^# Contributed equally.

Abstract

Effective and robust catalyst is the core of water splitting to produce hydrogen. Here, we report an anionic etching method to tailor the sulfur vacancy (V_S) of NiS₂ to further enhance the electrocatalytic performance for hydrogen evolution reaction (HER). With the V_S concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS₂-V_S 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential (68 mV) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy (ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S- H* peak of the NiS₂-V_S 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the NiS₂-V_S 5.9% has the optimal |ΔG_H*| of 0.17 eV. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.

Keywords: Adsorption; H; Hydrogen evolution reaction; Nanosheet; S vacancies.