Journal
ACS CATALYSIS
Volume 9, Issue 5, Pages 3978-3990Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b04885
Keywords
single-atom catalysis; thermal stability; ionic Pt; catalyst preparation; atom trapping
Categories
Funding
- US Department of Energy (DOE) [DE-FG02-05ER15712]
- US National Science Foundation [EEC-1647722]
- National Natural Science Foundation of China [21673040]
- US Air Force Office of Scientific Research [FA9550-15-1-0305, FA9550-18-1-0413]
- China Scholarship Council [201608360178]
- U.S. DOE [DE-AC02-06CH11357]
- Environmental Molecular Sciences Laboratory located at Pacific Northwest National Laboratory - U.S. DOE Office of Biological and Environmental Research
- DOE
- MRCAT member institutions
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Single-atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt % Pt), without forming any clusters or 3D aggregates when heated in air at 800 degrees C. The mechanism of trapping involves a reaction of the mobile PtO2 with under-coordinated cerium cations present at CeO2(111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single-atom species with the support, present during catalyst sintering and regeneration, helps explain the sintering resistance of ceria-supported metal catalysts.
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