Theoretical studies of non-noble metal single-atom catalyst Ni1/MoS2: Electronic structure and electrocatalytic CO2 reduction

Single-atom catalysts (SACs) have aroused significant interest in heterogeneous catalysis recent years because of their high catalytic selectivity and tunable activity various chemical reactions. Herein, non-noble metal SACs with 3d-series single atoms (M1) (M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) supported on MoS2 are computationally screened by using first-principles quantum-chemical theory. The Ni1/MoS2 catalyst is found to be the most stable among those due optimal binding energy. In order provide a fundamental understanding intrinsic stability bonding interaction between support, electronic structure, including spin density populations, charge difference (CDD), electron localization function (ELF), band states (DOS), crystal orbital Hamiltonian populations (COHP) systematically examined. solid-state quantum theory molecules (QTAIM) also applied further characterize Ni—S Mo—S covalent ionic nature support. It that addition bonding, there exists Ni—Mo critical for stability, properties catalyst. As typical application this catalyst, electrocatalytic mechanism reaction pathway CO2 reduction (CO2RR) been investigated. MoS2-supported Ni exhibit CO2RR methanol. calculational results theoretical insights towards design highly efficient MoS2-based functional materials.