4.8 Article

Aliovalent Doping of CeO2 Improves the Stability of Atomically Dispersed Pt

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 44, Pages 52736-52742

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c18330

Keywords

aliovalent doping; catalysis; metal-support; single atom; vacancies

Funding

  1. U.S. DOE BES grant [DE-SC0022199]
  2. Program Development fund [21-017]
  3. U.S. DOE BES [DE-SC0012704]
  4. U.S. DOE Early Career Award
  5. Department of Chemistry at the University of Illinois
  6. DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
  7. Synchrotron Catalysis Consortium (U.S. DOE, Office of Basic Energy Sciences) [DE-SC0012335]
  8. U.S. Department of Energy (DOE) [DE-SC0022199] Funding Source: U.S. Department of Energy (DOE)

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By combining aliovalent doping and oxygen vacancy generation, the study demonstrates an enhancement in the thermal stability of supported single-atom configurations.
Atomically dispersed supported catalysts hold considerable promise as catalytic materials. The ability to employ and stabilize them against aggregation in complex process environments remains a key challenge to the elusive goal of 100% atom utilization in catalysis. Herein, using a Gd-doped ceria support for atomically dispersed surface Pt atoms, we establish how the combined effects of aliovalent doping and oxygen vacancy generation provide dynamic mechanisms that serve to enhance the stability of supported single-atom configurations. Using correlated, in situ X-ray absorption, photoelectron, and vibrational spectroscopy methods for the analysis of samples on the two types of support (with and without Gd doping), we establish that the Pt atoms are located proximal to Gd dopants, forming a speciation that serves to enhance the thermal stability of Pt atoms against aggregation.

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