Two-dimensional Janus MXTe (M = Hf, Zr; X = S, Se) piezoelectrocatalysts: a comprehensive investigation of its electronic, synthesis feasibility, electric polarization, and hydrogen evolution reaction activity

Abstract

We computationally investigated potential piezoelectrocatlysts, two-dimensional (2D) Janus MXTe (M = Hf, Zr; X = S, Se). The structural and electronic properties, synthesis feasibility, piezoelectric properties, and hydrogen evolution reaction were calculated. Our results showed that these 2D Janus MXTe are narrow-gap seminconductors, indicating great conductivity for electrocatalysis. The feasibility of synthesis was found to be comparable to the already synthesized Janus materials. To exhibit piezoelectrocatalytic effect, the material has to be piezoelectric and catalytically effective simultaneously. As the Janus structure breaks the centrosymmetry, the
considered MXTe are intrinsically piezoelectric. We therefore calculated the dipole moments and the variation of out-of-plane polarization upon strain. The computed piezoelectric coefficient e31 is within the same order of magnitude with that of other Janus 2D materials. Finally, although pristine 2D Janus MXTe were inert to hydrogen evolution reaction, incorporation of single atom defects was found to significantly boost hydrogen adsorption. The catalytic efficacy can be further tuned by biaxial tensile strain, effectively controlling the Gibbs free energy of adsorption to be close to the thermoneutral value that is indicative of an excellent hydrogen evolution reaction activity, at least for ZrSTe Janus monolayer. In summary, this work proposed and comprehensively investigated a new class of possible piezoelectrocatalysts, 2D Janus materials, which is feasible to be synthesized, catalytically effective, and has great conductivity.