Strain Modulated Catalytic Activity of Pt2XSe3 (X = Hg, Zn) for Hydrogen Evolution Reaction

TL;DR

This study uses ab initio simulations to show how strain engineering can optimize the catalytic activity of Pt2XSe3 (X = Hg, Zn) for hydrogen evolution by modulating hydrogen binding energy through lattice deformation.

Contribution

It introduces strain engineering as a novel approach to enhance and tune the catalytic properties of 2D mineral-based materials for HER.

Findings

Late transition metal sites (Hg and Zn) show high HER activity.

Lattice strain can achieve near-thermoneutral H adsorption.

Strain modulates d-band centers and charge distribution, affecting H-metal bonds.

Abstract

The catalytic properties of Pt2XSe3 (X = Hg, Zn) in hydrogen-electrode- (HER-) based catalysts have been investigated based on state-of-the-art ab initio simulations. Our results show that the late transition metal sites (Hg and Zn) exhibit the best activity for HER in an acidic environment. Furthermore, lattice stretching and compression can effectively modulate the H binding energy, achieving almost thermoneutral adsorption at 3% compressive strain. The changes are attributed to the modulation in the d-band centers of late transition metal sites, as well as the depletion of charge population on bonding states, contributing to the destabilization of the H-metal bonds. Our contribution explores strain engineering as an effective strategy to tailor the activity of 2D mineral-based catalyst materials for HER, advancing our understanding of how mechanical manipulation can effectively modulate the catalytic properties of these materials.