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

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.