Journal
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Volume 47, Issue 21, Pages 8011-8015Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ie800245r
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Funding
- Repsol-YPF (Spain)
- Spanish Ministry of Science and Education [PSE-3 10200-2006-2, FIT-320100-2006-88]
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In previous papers, we showed that (i) neutral solutions of hydrogen peroxide can be safely obtained by the direct reaction of H-2 and O-2 gas mixtures in the presence of Pd-loaded sulfonic acid resins and (ii) low molecular weight olefins can be successfully epoxidized using aqueous solutions of H2O2 in the presence of amorphous Ti/SiO2 catalysts. Against this background, this paper seeks to go one step further in our on-site H2O2 strategy by combining the direct synthesis of nonacidic H2O2 solutions with the catalyzed epoxidation of alkenes with hydrogen peroxide. In a first step, we optimized the reaction conditions for the direct synthesis of H2O2 working in a semibatch reactor Aqueous solutions of 9 wt % H2O2 were then used in the epoxidation of oct-1-ene on a Ti-loaded amorphous silica catalyst, and reaction conditions were optimized. Finally, the propene epoxidation reaction was conducted in a continuous mode under the optimum reaction conditions selected (343 K, H2O4 catalyst ratio = 1:4, propene/catalyst ratio = 25, residence time 45 min). At steady-state, the conversion level of H2O2 reached 96% with a selectivity of hydrogen peroxide to propene oxide of 95%. After 135 h of reaction time, a slight decrease in the selectivity of H2O2 to epoxide was observed, with a decrease of H2O2 conversion from 96 to 80%. This catalyst deactivation is reversible, as original activity is fully recovered upon regeneration in air at 873 K.
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