Cooperative 3d-metals doping MoSe2 catalysts for enhanced electrocatalytic hydrogen evolution reaction

Molybdenum diselenide(MoSe2) has attracted great interest as a promising nonprecious metal catalyst for hydrogen evolution reaction(HER). However, scarce catalytic sites and unsatisfactory electrocatalytic activity seriously impede its practical application. Single- and dual-atom catalysts play a crucial role in catalyzing of HER due to their unique electronic properties, highest atom utilization and synergistic effects. Herein, we screen a series of single- and dual-atom 3d-metals(Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu and Zn) doping MoSe2 as potential HER electrocatalysts based on density functional theory calculations. All 3d-metals doping MoSe2 exhibit highly thermodynamically and electrochemical stabilities, which show significantly promoting adsorption-activity by 3d-metals dopants, due to synergistic interaction between active Se site and neighboring 3d-metals dopants. Specially, we screen out that dual Cu-Co-MoSe2 shows the best HER activity with low overpotential(only 30 mV), markedly lower than single Co-MoSe2(360 mV) and crystal Pt(90 mV), indicating promising candidate for nonnoble metal HER catalyst. Furthermore, we find descriptors of Delta dp and ICOHP can well predict materials' HER performance and exhibit linear relationship with H-binding strength. This study will provide in-depth understanding for designing and screening of high-efficiency MoSe2-based catalysts for HER.