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- W2008256766 abstract "In situ ultraviolet−visible (UV−vis) diffuse reflectance spectroscopy was used in combination with in situ Ti K-edge X-ray absorption near-edge structure (XANES) to study the formation of Ti-hydroperoxo species during the gas-phase epoxidation of propylene with H2 and O2 at reaction conditions over a Au−Ba/Ti−SiO2 (Ti−TUD) catalyst. The in situ UV−vis measurements showed growth of a signal due to Ti-hydroperoxo species when the catalyst was put in contact with H2/O2/Ar (1/1/8) and C3H6/H2/O2/Ar (1/1/1/7) gas mixtures at 423 K and 0.1 MPa. Changes in the area of the pre-edge peak centered at 4968.9 eV present in the Ti K-edge XANES spectra of the catalyst were used to estimate the Ti-hydroperoxo species coverages (θ) under operating conditions. Transient Ti K-edge XANES experiments with H2/O2/Ar (1/1/8) and C3H6/H2/O2/Ar (1/1/1/7) gas mixtures allowed the estimation of the net epoxidation rate by a novel method involving the determination of dθ/dt. It is shown that the Ti-hydroperoxo species are true intermediates because their initial rate of reaction measured from the in situ transient XANES data (3.4 × 10-4 s-1) has the same order of magnitude as the steady-state turnover frequency for propylene epoxidation based on the total Ti (2.5 × 10-4 s-1) measured in a catalytic flow reactor. This is the first use of XANES to measure the turnover rate of a catalyzed reaction." @default.
- W2008256766 created "2016-06-24" @default.
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- W2008256766 date "2008-01-01" @default.
- W2008256766 modified "2023-10-18" @default.
- W2008256766 title "Transient Technique for Identification of True Reaction Intermediates: Hydroperoxide Species in Propylene Epoxidation on Gold/Titanosilicate Catalysts by X-ray Absorption Fine Structure Spectroscopy" @default.
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- W2008256766 doi "https://doi.org/10.1021/jp077501s" @default.
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