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Thermodynamics and kinetics of interconversion between platinum nanoparticles and cations in zeolites

Journal Article · · Journal of Catalysis
 [1];  [2];  [2];  [3];  [2]
  1. University of Virginia, Charlottesville, VA (United States); Purdue University
  2. University of Virginia, Charlottesville, VA (United States)
  3. Purdue University, West Lafayette, IN (United States)
In metal-containing zeolites, sintering and redispersion processes exercise control over the identity of metal site structures, but the thermodynamic and kinetic factors that influence these molecular-level processes are not completely understood. Furthermore, we assess the ability of first principles informed free energy models (for supported and unsupported nanoparticles) and kinetic models integrating Ostwald ripening with atom trapping to describe the interconversion between Pt cations and nanoparticles encapsulated in chabazite (CHA) zeolites. Density functional theory-derived thermodynamic phase diagrams show that the interconversion between cations, favored in oxidizing environments, and particles, favored in reducing environments, is fully reversible within a wide range of their respective conditions (temperatures and pressures) for CHA and several other zeolite topologies. Kinetic Monte Carlo simulations of Pt redispersion are consistent with experimentally observed redispersion kinetics of encapsulated Pt nanoparticles in CHA zeolites, and model results suggest the zeolite host imparts additional stability for Pt nanoparticles. We envision our thermodynamic and kinetic models for Pt-CHA are also capable of describing nanoparticle and cation interconversions for other zeolite frameworks under similar conditions.
Research Organization:
Purdue University, West Lafayette, IN (United States)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0019026
OSTI ID:
2339570
Alternate ID(s):
OSTI ID: 2346249
Journal Information:
Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 434; ISSN 0021-9517
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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