Te Vacancy Defect Engineering on Fe3GeTe2 (001) Basal Planes for Enhanced Oxygen Evolution Reaction: A First-Principles Study

Photocatalytic water splitting for hydrogen production is an attractive renewable energy technology, but the oxygen evolution reaction (OER) at the anode is severely constrained by a high overpotential. The two-dimensional vdW ferromagnetic material Fe3GeTe2, with its good stability and excellent metallic conductivity, has potential as an electrocatalyst, but its sluggish surface catalytic reactivity limits its large-scale application. In this work, we adapted DFT calculations to introduce surface Te vacancies to boost OER performance of the Fe3GeTe2 (001) surface. Te vacancies induce the charge redistribution of active sites, optimizing the adsorption and desorption of oxygen-containing intermediates. Consequently, the overpotential of the rate-determining step in the OER process of Fe3GeTe2 is reduced to 0.34 V, bringing the performance close to that of the benchmark IrO2 catalyst (0.56 V). Notably, the vacancies’ concentration and configuration significantly modify the electronic structure and thus influence OER activity. This study provides important theoretical evidence for defect engineering in OER catalysis and offers new design strategies for developing efficient and stable electrocatalysts for sustainable energy conversion.