Single Pt Atoms on N-Doped Graphene: Atomic Structure and Local Electronic States

Single-atom catalysts are attracting attention due to their superior catalytic activity and cost. Nitrogen (N) enhances the stability of single platinum (Pt) atoms on graphene because Pt atoms dispersed by plasma sputtering in an N-2 atmosphere are less likely to aggregate. However, the atomic structure of Pt and N on graphene has not been clarified. Here, we experimentally revealed the atomic arrangement of Pt, N, and carbon (C) by scanning transmission electron microscopy and electron energy loss spectroscopy. Pt and N atoms were adsorbed near the step edge of nanographene stacked on single-layer pristine graphene rather than on the terrace. The density functional theory (DFT) calculations using the experimental structure confirmed that the single Pt atom has high stability because N strengthens the bond between Pt and C at the step edge. In addition to a large decrease in the population of Pt 5d(xy)-orbital, an increase in the population of 5d(yz)-orbital was observed.

Automated summary

Nitrogen (N) enhances the stability of single Pt atoms on graphene, as Pt and N atoms prefer adsorption near the step edge. Experimental and theoretical studies confirm that N strengthens the bond between Pt and C, increasing the stability of single Pt atoms on graphene.