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Mechanistic study of propane selective oxidation with H2 and O2 on Au/TS-1

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Abstract.
The selective oxidation of propane to acetone and 2-propanol with H2 and O2 was studied on Au/TS-1 by
kinetic and spectroscopic analysis. A kinetic study using a factorial design at conditions where the catalyst
was stable and gave propane conversions of 90%, resulted
in a power-rate law expression of the form roxyg. = koxyg.(H2)0.74(O2)0.36(C3H8)0.29. In situ Au L3-edge
X-ray absorption near-edge spectroscopy (XANES) measurements showed activation of O2 on Au, whereas
in situ ultraviolet–visible (UV–vis) spectroscopy evidenced the presence of Ti-hydroperoxo species. The
role of the Ti-hydroperoxo species was probed by a transient technique in which changes in Ti K-edge
XANES spectra were used to determine the evolution of coverage with time (dθ/dt). It was shown that
the rate of reaction by XANES (6.7×10−4 s−1) was close to the turnover rate measured in a catalytic flow
reactor (5.6×10−4 s−1), indicating that the hydroperoxo species were true intermediates in the reaction.
A proposed reaction sequence in which H2O2 forms on Au sites and propane is partially oxidized on Ti
centers accounts for the spectroscopic results and the reaction orders obtained experimentally for the
power-rate law expression.

Keywords:
Gold
TS-1
Propane
Acetone
2-Propanol
Kinetics
Ultraviolet–visible spectroscopy
X-ray absorption near edge spectroscopy
True intermediate
Oxidation

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Informasi Detail

Judul Seri

Journal of Catalysis

No. Panggil

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Penerbit

London : Elsevier Inc.., 2008

Deskripsi Fisik

Journal of Catalysis 257 (2008) 32–42

Bahasa

English

ISBN/ISSN

00219517

Klasifikasi

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Tipe Isi

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Tipe Media

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Tipe Pembawa

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Edisi

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Subjek

KIMIA

Info Detail Spesifik

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Pernyataan Tanggungjawab

agus

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