Strain-Engineered Jacutingaite Analogs as Efficient 2D Catalysts for Hydrogen Evolution Reactions

The catalytic properties of Pt₂XSe₃ (X = Hg, Zn) for Hydrogen Evolution Reactions (HER) have been investigated based on state-of-the-art ab initio simulations. Our findings indicate that the late transition metal sites (Hg and Zn) demonstrate superior activity for HER under acidic conditions. Moreover, lattice stretching or compression can significantly influence the H binding energy, achieving near-thermoneutral adsorption at a 3% compressive strain. This effect is attributed to the alterations in the d-band centers of late transition metal (X) sites and changes in the bonding strength, demonstrated by the changes in the integrated Crystal Orbital Hamilton Population (ICOHP). Furthermore, charge difference analysis reveals how charge accumulation between the X and Pt atoms changes as the structure is stretched (tensile strain), weakening the interactions with the H adsorbate due to the increased electrostatic repulsion. Our contribution explores strain engineering as an effective approach to tailor the catalytic activity of 2D materials for HER by providing insights into the role of mechanical manipulation in altering electronic properties and boosting catalytic performance.