▎ 摘　　要

In single-atom catalysis, the atomic structure and local electronic states of single atoms on a supporting material remain a fundamental question. We experimentally and theoretically solved these problems for single Pt atoms dispersed on freestanding graphene using plasma sputtering. Electron microscopy revealed the atomic arrangements of Pt atoms binding to carbon atoms at the step edges of nanographene flakes. X-ray photoelectron spectroscopy revealed a large binding energy shift of the Pt 4f state of a single Pt atom. First-principles calculations elucidated that the Pt 5d(xy)-orbital in the step edge plays a crucial role in the formation of chemical bonds to C atoms and in the considerable charge transfer from Pt to C atoms, resulting in the large binding energy shift of the Pt 4f state.