摘要
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(Pt_(1))during the high-temperature oxidation of light alkanes.The distinctly enhanced activity of the catalyst is attributed to the in situ evolved Pt_(1)−oxygen vacancy(Pt_(1)−OV)combination ensemble as an efficient and stable active site.Theoretical calculations reveal that the lattice oxygen adjacent to Pt_(1)and the H dissociated from CH4 constitute the lattice hydroxyl,which is the initial step in the formation of the Pt_(1)−OV combination.Pt_(1)and nearby unsaturated Mn can donate the charge back to O−O to promote the dissociation of O_(2).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.
基金
the National Nature Science Foundation of China[No.21976172,22172030]
the Strategic Priority Research Program of the Chinese Academy of Sciences[No.XDPB1902].
