Controlling Hydrogen Evolution Reaction of Janus MoSSe by Defect and Strain Engineering

doi:10.16553/j.cnki.issn1000-985x.2025.0020

Abstract

Abstract: Janus transition metal dichalcogenides （TMDs） exhibit exceptional electronic， optical， and catalytic properties due to their unique asymmetric structure， showing broad application prospects in fields such as nanocatalysis and thermoelectrics. This study employs first-principles calculations to systematically investigate the stability and hydrogen evolution reaction （HER） performance of monolayer Janus MoSSe with typical vacancy defects. The results demonstrate that the Gibbs free energy of monolayer Janus MoSSe during the HER process is significantly reduced to approximately 0.5 eV， markedly lower than that of pristine MoSSe and conventional MoS₂ monolayers. Further research reveals that the introduction of external strain can effectively modulate the HER performance of defective Janus MoSSe. The performance enhancement is primarily attributed to the adaptive release of concentrated strain by dangling bonds in the defect regions， resulting in a notable tunable mode. This study elucidates the underlying mechanism of strain engineering in improving the HER performance of MoSSe， providing a theoretical foundation for the optimized design of efficient HER catalysts based on defective Janus TMDs.

Key words: transition metal dichalcogenide （TMD）; first-principle; hydrogen evolution reaction （HER）; Gibbs free energy; strain engineering; defective structure

CLC Number:

O463.36

LIU Jingsong, SHEN Lu, REN Longjun, HUANG Xizhong. Controlling Hydrogen Evolution Reaction of Janus MoSSe by Defect and Strain Engineering[J]. Journal of Synthetic Crystals, 2025, 54(6): 1034-1041.

Figures/Tables 5

Fig.1 Structure and stability of monolayer defected Janus MoSSe. （a） Atomic configurations （top） and corresponding STM images （bottom） of six Janus MoSSe monolayers with vacancy defects；（b） formation energy；（c） surface defect density

Fig.2 HER characteristics of defected Janus MoSSe. Most stable adsorption sites for VMo （a）， VS （b）， VSe （c）， VSeS （d）， VMoS3 （e）， and VMoSe3 （f）；（g） Gibbs free energy

Fig.3 Electronic properties of defected MoSSe monolayer. （a） Projected density of states；（b） charge density difference；（c） projected band centers

Fig.4 Strain response of defected MoSSe monolayer. （a） Gibbs free energy；（b） work function and built-in electric field

Fig.5 Difference and structure of MoSSe monolayer under different external strains. （a） Bond strain and charge density difference of defect MoSSe and VMo configuration monolayers；（b） relationship between bond strain and external strain for Bond-a and Bond-b

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