Theoretical screening of multifunctional single-atom catalysts supported by VS2 monolayer for the electrocatalytic hydrogen evolution, oxygen evolution and oxygen reduction reactions

Exploring highly efficient multifunctional electrocatalysts for the HER, OER, and ORR is of great significance. In this work, transition metal atoms anchored on VS₂ monolayer (TM@VS₂) as single-atom catalysts were systematically investigated for their HER, OER, and ORR performance through first-principles calculations. The results indicate that all TM@VS₂ show high thermal stability and excellent electrical conductivity. Pt@VS₂ and Au@VS₂ are predicted to be the promising HER/OER bifunctional electrocatalysts for overall water-splitting with lower overpotentials of −0.07/0.59 V and − 0.07/0.62 V, respectively, and Ni@VS₂, Pd@VS₂ and Au@VS₂ are potential OER/ORR bifunctional electrocatalysts for metal-air batteries with ultralow overpotentials of 0.26/0.33 V, 0.34/0.28 V and 0.62/0.41 V, respectively. In addition, Au@VS₂ is a promising trifunctional electrocatalyst for the HER/OER/ORR with relatively low overpotentials of −0.07/0.62/0.41 V. The electronic origin of the enhanced HER/OER/ORR activity of TM@VS₂ catalysts can be well understood by the amendatory d-band center model.