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Reversible transformation of Pt nanoparticles into single atoms inside high-silica shabazite zeolite

AutorMoliner Marín, Manuel; Gabay, Jadeene E.; Kliewer, Chris E.; Carr, Robert T.; Guzman, Javier; Casty, Gary L.; Serna Merino, Pedro; Corma, Avelino
Fecha de publicación2016
EditorAmerican Chemical Society
CitaciónJournal of the American Chemical Society 138(48): 15743-15750 (2016)
ResumenWe report the encapsulation of platinum species in highly siliceous chabazite (CHA) crystallized in the presence of N,N,N-trimethyl-1-adamantammonium and a thiol-stabilized Pt complex. When compared to Pt/SiO2 or Pt-containing Al-rich zeolites, the materials in this work show enhanced stability toward metal sintering in a variety of industrial conditions, including H2, O2, and H2O. Remarkably, temperatures in the range 650–750 °C can be reached without significant sintering of the noble metal. Detailed structural determinations by X-ray absorption spectroscopy and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy demonstrate subtle control of the supported metal structures from ∼1 nm nanoparticles to site-isolated single Pt atoms via reversible interconversion of one species into another in reducing and oxidizing atmospheres. The combined used of microscopy and spectroscopy is critical to understand these surface-mediated transformations. When tested in hydrogenation reactions, Pt/CHA converts ethylene (∼80%) but not propylene under identical conditions, in contrast to Pt/SiO2, which converts both at similar rates. These differences are attributed to the negligible diffusivity of propylene through the small-pore zeolite and provide final evidence of the metal encapsulation.
Versión del editorhttps://doi.org/10.1021/jacs.6b10169
Identificadoresdoi: 10.1021/jacs.6b10169
issn: 0002-7863
e-issn: 1520-5126
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