Platinum species in the pores of NaX, NaY and NaA zeolites studied using EPR, XAS and FTIR spectroscopies

The results of X-band EPR, X-ray absorption and Fourier transform infrared spectroscopy on Pt(NH(3))(4)(2+) exchanged NaX, NaY and NaA zeolites reveal after oxygen calcination at 573 K that diamagnetic Pt(2+) is not the only product. Calcination provides Pt(3+) cations, but depending on the heating...

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Vydáno v:Physical chemistry chemical physics : PCCP Ročník 10; číslo 20; s. 2952
Hlavní autoři: Akdogan, Yasar, Vogt, Christina, Bauer, Matthias, Bertagnolli, Helmut, Giurgiu, Liviu, Roduner, Emil
Médium: Journal Article
Jazyk:angličtina
Vydáno: England 01.01.2008
Témata:
Adsorption
Carbon Monoxide - chemistry
Electron Spin Resonance Spectroscopy - methods
Hydrogen - chemistry
Models, Molecular
Platinum Compounds - chemistry
Sensitivity and Specificity
Sodium Compounds - chemistry
Spectroscopy, Fourier Transform Infrared - methods
Spectrum Analysis - methods
Surface Properties
X-Rays
Zeolites - chemistry
ISSN:1463-9076
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Shrnutí:The results of X-band EPR, X-ray absorption and Fourier transform infrared spectroscopy on Pt(NH(3))(4)(2+) exchanged NaX, NaY and NaA zeolites reveal after oxygen calcination at 573 K that diamagnetic Pt(2+) is not the only product. Calcination provides Pt(3+) cations, but depending on the heating rate, the decomposition of amino groups during calcination also produces hydrogen that reduces Pt(3+) to Pt(2+) and Pt(+). NaX (Si/Al = 1.23) has a more negative framework charge than NaY (Si/Al = 2.31), so Pt(3+) can be stabilized only in NaX, whereas lower oxidation states of Pt such as Pt(+) can be stabilized in both, NaX and NaY, and neither of the paramagnetic Pt cations are stabilized in NaUSY (Si/Al = 3). The autoreduction process allows controlling the number of Pt(3+) and Pt(+) in the NaX zeolite by changing the calcination heating rate: a heating rate of 1.25 K min(-1) gives only Pt(+), but 0.5 K min(-1) gives a Pt(3+)/Pt(+) ratio close to 1. The structure of the support is also important for the synthesis of Pt species. While isolated paramagnetic Pt ions were stabilized in faujasite zeolites (NaX and NaY), a paramagnetic Pt dimer was obtained in a Linde type A zeolite (LTA, Si/Al = 1) by applying the same preparation methods. The fraction of paramagnetic Pt species which were characterized by X-band EPR spectroscopy amounts to 2-18% of the total Pt in the zeolites, the remaining Pt must be diamagnetic.
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ISSN:1463-9076
DOI:10.1039/b718932j