In Situ High-Temperature Reaction-Induced Local Structural Dynamic Evolution of Single-Atom Pt on Oxide Support

Abstract

The dynamic evolution of active site coordination structure during a high-temperature reaction is critically significant but often difficult for the research of efficient single-atom catalysts (SACs). Herein, we for the first time report the in situ activation behaviors of the local coordination structure of Pt single atoms (Pt1) during the high-temperature oxidation of light alkanes. The distinctly enhanced activity of the catalyst is attributed to the in situ evolved Pt1–oxygen vacancy (Pt1–OV) combination ensemble as an efficient and stable active site. Theoretical calculations reveal that the lattice oxygen adjacent to Pt1 and the H dissociated from CH4 constitute the lattice hydroxyl, which is the initial step in the formation of the Pt1–OV combination. Pt1 and nearby unsaturated Mn can donate the charge back to O–O to promote the dissociation of O2. This work provides molecular-level insight into the in situ reaction-induced evolution of a single-atom coordination environment for designing efficient SACs under harsh conditions.