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 (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.
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PRECISION CHEMISTRY
Year: 2023
Issue: 5
Volume: 1
Page: 299-308
Cited Count:
SCOPUS Cited Count: 6
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
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