High-throughput screening of H2 production catalysts from doped In2SSe monolayer: Valence electrons-based descriptor

Abstract

Recently, the novel Janus In2SSe monolayer attracts great attention as a potential catalyst for hydrogen evolution reaction (HER). In this work, high-throughput calculations are carried out to screen the numerous transition-metal-doped In2SSe monolayers for designing hydrogen production catalysts. A series of doped In2SSe monolayers have been screened out with comparable or even better catalytic activity than that of Pt (111). Particularly, The AuS@In2SSe possess the best catalytic performance with a hydrogen adsorption free energy of 0 eV. These results suggest that the catalytic activity is influenced by the local environment of the active center. In addition to the revised pz band center, the valence electrons of the dopants also have a highly linear relationship with the hydrogen adsorption free energy, which can be used as a new descriptor for screening efficient HER catalysts. Machine learning is used to reveal the intrinsic relationship between structure and catalytic performance. Our work offers a new perspective for the design of novel HER catalysts.