24.02.2013 Views

Heterogeneously Catalyzed Oxidation Reactions Using ... - CHEC

Heterogeneously Catalyzed Oxidation Reactions Using ... - CHEC

Heterogeneously Catalyzed Oxidation Reactions Using ... - CHEC

SHOW MORE
SHOW LESS

You also want an ePaper? Increase the reach of your titles

YUMPU automatically turns print PDFs into web optimized ePapers that Google loves.

5.3 Results<br />

Figure 5‐7: <strong>Oxidation</strong> of benzyl alcohol at a molar flow of 0.118 mol/min; conditions: 80 °C, 1.25 g<br />

0.5%Pd/Al2O3 in a fixed bed reactor; feed composition: 0.9 mol‐% benzyl alcohol, 0.45 mol‐% O2, rest CO2; (●)<br />

conversion, (○) benzaldehyde selectivity, (□) toluene selectivity, (∆) selectivity to overoxidation products.<br />

visual inspection of the feed mixture in the inter‐connectable view cell of the setup. Thus, for the<br />

feed mixture consisting of 0.9 mol‐% benzyl alcohol (Figure 5‐6b), clearly two phases were<br />

observable at 150 bar, while only one was existing at 170 bar. At an intermediate pressure of 160 bar<br />

no clear conclusion on the number of phases could be drawn from simple phase monitoring under<br />

flow conditions. Decreasing the overall molar flow showed that the pressure at which the decrease in<br />

reaction rate occurred remained almost the same (Figure 5‐7) matching again well with the<br />

experimental data and the CPA predictions. Compared to the previously described experiments, the<br />

selectivity was always higher than 90 %. A significant increase in conversion was found between 140<br />

and 150 bar which was also reported under similar conditions [7]. Again, at both pressures the<br />

system exists as two phases by visual inspection. Thus, the observed increase in reaction rate is not<br />

due to a phase transition. The increased toluene selectivity indicates a faster transport of<br />

benzaldehyde to the catalyst surface compared to O2. When changing from two phase conditions to<br />

single phase conditions, the time until a steady‐state was reached was very long and a continuous<br />

decrease in catalytic activity occurred. Note that in this study a steady‐state was assumed when the<br />

141

Hooray! Your file is uploaded and ready to be published.

Saved successfully!

Ooh no, something went wrong!