Reversible active bridging sulfur sites grafted on Ni3S2 nanobelt arrays for efficient hydrogen evolution reaction

Dan Yang; Liyun Cao; Jianfeng Huang; Gengsheng Jiao; Donghua Wang; Qianqian Liu; Guodong Li; Chaozheng He; Liangliang Feng

doi:10.1016/j.jcis.2023.06.082

Reversible active bridging sulfur sites grafted on Ni₃S₂ nanobelt arrays for efficient hydrogen evolution reaction

J Colloid Interface Sci. 2023 Nov:649:194-202. doi: 10.1016/j.jcis.2023.06.082. Epub 2023 Jun 16.

Authors

Dan Yang¹, Liyun Cao², Jianfeng Huang³, Gengsheng Jiao⁴, Donghua Wang⁴, Qianqian Liu⁵, Guodong Li⁶, Chaozheng He⁷, Liangliang Feng⁸

Affiliations

¹ School of Material Science and Engineering, International S&T Cooperation, Foundation of Shaanxi Province, Xi'an Key Laboratory of Green Manufacture of Ceramic Materials, Shaanxi University of Science and Technology, Xi'an 710021, PR China; College of Chemistry and Materials Science, WeiNan Normal University, Weinan 714099, PR China.
² School of Material Science and Engineering, International S&T Cooperation, Foundation of Shaanxi Province, Xi'an Key Laboratory of Green Manufacture of Ceramic Materials, Shaanxi University of Science and Technology, Xi'an 710021, PR China. Electronic address: caoliyun@sust.edu.cn.
³ School of Material Science and Engineering, International S&T Cooperation, Foundation of Shaanxi Province, Xi'an Key Laboratory of Green Manufacture of Ceramic Materials, Shaanxi University of Science and Technology, Xi'an 710021, PR China.
⁴ College of Chemistry and Materials Science, WeiNan Normal University, Weinan 714099, PR China.
⁵ College of Materials Science and Engineering, Xi'an University of Science and Technology, Xi'an 710054, PR China.
⁶ State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, PR China.
⁷ Institute of Environmental and Energy Catalysis, School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China. Electronic address: hecz2019@xatu.edu.cn.
⁸ School of Material Science and Engineering, International S&T Cooperation, Foundation of Shaanxi Province, Xi'an Key Laboratory of Green Manufacture of Ceramic Materials, Shaanxi University of Science and Technology, Xi'an 710021, PR China. Electronic address: fengll@sust.edu.cn.

PMID: 37348339
DOI: 10.1016/j.jcis.2023.06.082

Abstract

Elaborate and rational design of cost-effective and high-efficiency non-noble metal electrocatalysts for pushing forward the sustainable hydrogen fuel production is of great significance. Herein, a novel VS₄ nanoparticle decorated Ni₃S₂ nanobelt array in-situ grown on nickel foam (VS₄/Ni₃S₂/NF NBs) was prepared by a self-templated synthesis strategy. Benefitting from the unique nanobelt array structure, abundant highly active bridge S₂^2- sites and strong electronic interaction between VS₄ and Ni₃S₂ on the heterointerface, the integrated VS₄/Ni₃S₂/NF NBs exhibited excellent electrocatalytic hydrogen evolution activity and robust stability. The density functional theory (DFT) further revealed the reversible conversion catalysis mechanism of bridging S₂^2- sites in VS₄/Ni₃S₂/NF NBs during HER process. Notably, bidentate bridging SS bonds as the predominant catalytically active centers can spontaneously open once H adsorbed its surface, leading to the aggregation of negative charges on S atoms and thus facilitating the generation of H* intermediates, and spontaneously close when H* desorption is going to form H₂. Our work provides fresh insights for developing potential polysulfides as high-performance hydrogen-evolving electrocatalysts for prospective clean energy production from water splitting.

Keywords: Bridging S–S; Hydrogen evolution reaction; Nanobelt arrays; Ni(3)S(2)/VS(4); Reversible.