▎ 摘　　要

Single-atom Fe-1 catalyst supported by graphene-based substrates (Fe/GS) has the potential to replace noble metal catalysts in water splitting reaction due to its high activity, high selectivity, and low cost. Here we have constructed four kinds of Fe/GS to probe its application in water splitting reaction. The adsorption characteristics of the water molecule and the reaction path of water splitting on single atom Fe-1 catalysts with four types of graphene-based substrates were studied systematically by using the density functional theory (DFT) method. PDOS results show that the 3d orbitals of Fe single atom and 2p orbitals of O atom are highly hybridized and overlapped which are responsible for the strong chemisorption of H2O molecules on Fe/GS surface. Depending on the reaction pathway analysis, the water splitting reaction performs a catalytic activity trend of Fe/DV-GN, Fe/SV-N3, Fe/SV-GN, Fe/DV-N4. While strong metal-support interactions (SMSI) play a key role in the process of water splitting reaction. Furthermore, the reaction kinetics of water splitting was investigated based on transition state theory. This study aims to develop a highly efficient single-atom Fe-1 catalyst for water splitting.