One-Pot Pyrolysis to N-Doped Graphene with High-Density Pt Single Atomic Sites as Heterogeneous Catalyst for Alkene Hydrosilylation

Abstract

Development of noble-metal single atomic site catalysts with high metal loading is highly required for many important chemical reactions but proves to be very challenging. Herein, we report a Na2CO3 salt-assisted one-pot pyrolysis strategy from EDTA–Pt complex to N-doped graphene with isolated Pt single atomic sites (Pt-ISA/NG) with Pt loading up to 5.3 wt %. The X-ray absorption fine structure analysis and spherical aberration-correction electron microscopy demonstrate an atomic dispersion of single Pt species on graphene support and stabilized by nitrogen in Pt–N4 structure. The Pt-ISA/NG catalyst exhibits high catalytic activity and reusability for anti-Markovnikov hydrosilylation of various terminal alkenes with industrially relevant tertiary silanes under mild conditions. In hydrosilylation of 1-octene, the Pt-ISA/NG catalyst delivers an overall turnover frequency of 180 h–1, which is a 4-fold enhancement compared with commercial Pt/C.