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Abstract：
Single noble metal atoms and ultrafine metal clusters catalysts tend to sinter into aggregated particles at elevated temperatures, driven by the decrease of metal surface free energy. Herein, we report an unexpected phenomenon that noble metal nanoparticles (Pd, Pt, Au-NPs) can be transformed to thermally stable single atoms (Pd, Pt, Au-SAs) above 900 degrees C in an inert atmosphere. The atomic dispersion of metal single atoms was confirmed by aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structures. The dynamic process was recorded by in situ environmental transmission electron microscopy, which showed competing sintering and atomization processes during NP-to-SA conversion. Further, density functional theory calculations revealed that high-temperature NP-to-SA conversion was driven by the formation of the more thermodynamically stable Pd-N-4 structure when mobile Pd atoms were captured on the defects of nitrogen-doped carbon. The thermally stable single atoms (Pd-SAs) exhibited even better activity and selectivity than nanoparticles (Pd-NPs) for semi-hydrogenation of acetylene.
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Source ：
NATURE NANOTECHNOLOGY
ISSN： 1748-3387
Year： 2018
Issue： 9
Volume： 13
Page： 856-,
3 8 . 3 0 0
JCR@2022
ESI Discipline： MATERIALS SCIENCE;
ESI HC Threshold：260
JCR Journal Grade：1
Cited Count：
WoS CC Cited Count： 864
SCOPUS Cited Count： 892
ESI Highly Cited Papers on the List： 36 Unfold All
WanFang Cited Count：
Chinese Cited Count：
30 Days PV： 3
