Theoretical screening of transition metal atoms doped two-dimensional VSe2 monolayers as single-atom catalysts for HER, OER and ORR

Single-atom catalysts (SACs) have attracted considerable attention because of their excellent atomic utilization and catalytic performance. However, the choice of the carrier in SACs plays a decisive role in the catalytic performance. In this work, a series of single transition metal atoms (Fe, Co, Ni, Cu. Zn, Ru, Rh, Pd, Ag, Cd, Os, Ir, Pt, Au, Hg) doped on the two-dimensional(2D) VSe2 monolayer were selected as electrocatalysts, then we sys-tematically calculated and investigated hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), as well as electrocatalytic oxygen reduction reaction (ORR) performance for a transition metal atom, doped VSe2 (TM@VSe2) through first-principle calculation. The results show that among all SACs, And Au@VSe2 has the lowest overpotential of 0.45 V, exhibiting excellent catalytic performance of OER. Meanwhile, Pt@VSe2 shows a good catalytic performance of HER with Delta GH* of 0.11 eV and certain catalytic performance of OER as well as ORR (eta OER = 0.72 eV, eta ORR = 0.85 eV), indicating that Pt@VSe2 may be utilized as a moderate triple-functional single-atom catalyst. This work broadens the view of designing multifunctional catalysts based on 2D VSe2 materials and provides a new paradigm for the study of advanced single-atom catalysts.