Modulating the stability, electronic and reactivity properties of single-atom catalyst anchored graphene by coordination environments

Abstract The formation geometry, electronic property and catalytic activity of single-atom (SAs) Fe anchored graphene with different kinds and number of coordinated B and N atoms (xB-yN-graphene-SAs, x + y = 1–3) are comparably investigated by using the density functional theory (DFT) calculations. It is found that the coordinated 1B, 1 N, 2B–1N atoms can more effectively control the stability of SAs Fe on graphene sheet than other coordination structures, and these formation configurations exhibit the high thermal stability. Among these xB-yN-graphene-Fe sheets, the formation of 3N-graphene-Fe exhibits the high gas sensoring for the single gas molecule and coadsorbed gas reactants. Meanwhile, these gas adsorbed systems exhibit the various electronic and magnetic properties by promoting the charge transfer between adsorbates and substrates. By investigation the Langmuir-Hinshelwood (LH) and Eley-Rideal (ER) mechanisms for NO and CO oxidations, the 1B–1N-graphene-Fe and 1B-graphene-Fe sheets exhibit the more activity (