An asymmetrical Zr2CO/VSe2 heterostructure as an efficient electrocatalyst for the hydrogen evolution reaction

Abstract

This study uses first-principles calculations to investigate the asymmetric Zr₂CO/VSe₂ heterostructure for hydrogen evolution reaction (HER) applications, focusing on its interlayer interactions, electronic structures, and HER performance across six stacking angles. Our findings demonstrate remarkable structural stability, characterized by interlayer distances of 2.1 Å to 2.7 Å and binding energies from −150.521 to −257.939 meV Å⁻². Band structure analyses highlight the heterostructures' exceptional conductivity, essential for catalytic efficiency. Additionally, charge density difference calculations reveal significant charge transfer and redistribution at the interface, providing insights into the interlayer interactions and their influence on catalytic activity. Notably, the Gibbs free energy of hydrogen adsorption (ΔG_H*) remains within ±0.1 eV across all configurations, indicating superior HER activity. Further analysis shows that the work function (Φ) serves as a critical electronic structure descriptor, influencing HER performance. The relationship between work function and ΔG_H* across different interlayer distances underscores the predictive value of the work function for HER activity. These insights provide a theoretical foundation for developing advanced and effective non-noble metal HER catalysts, paving the way for innovations in sustainable energy technologies.