Prediction of structured void-containing 1T-PtTe2 monolayer with potential catalytic activity for hydrogen evolution reaction**Project supported by the National Key R&D Program of China (Grant Nos. 2016YFA0202300, 2018YFA0305800, and 2019YFA0308500), the National Natural Science Foundation of China (Grant Nos. 61888102, 51872284, and 51922011), and the Strategic Priority Research Program of Chinese Academy of Sciences (Grant No. XDB30000000).

Abstract

Two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted considerable attention because of their unique properties and great potential in nano-technology applications. Great efforts have been devoted to fabrication of novel structured TMD monolayers by modifying their pristine structures at the atomic level. Here we propose an intriguing structured 1T-PtTe2 monolayer as hydrogen evolution reaction (HER) catalyst, namely, Pt4Te7, using first-principles calculations. It is found that Pt4Te7 is a stable monolayer material verified by the calculation of formation energy, phonon dispersion, and ab initio molecular dynamics simulations. Remarkably, the novel structured void-containing monolayer exhibits superior catalytic activity toward HER compared with the pristine one, with a Gibbs free energy very close to zero (less than 0.07 eV). These features indicate that Pt4Te7 monolayer is a high-performance HER catalyst with a high platinum utilization. These findings open new perspectives for the functionalization of 2D TMD materials at an atomic level and its application in HER catalysis.