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catalyst—being less able to reduce the kinetic barrier—this decrease in activity is partially compensated for by an increase in the pre-exponential factor, which increases from 1 × 103 for TS-1, to 2 × 105 for TS-1B. These changes may indicate a modification to the rate-limiting step, and potentially some modifications to the Catalyesptso2x0id1a5t,i5on pathway. 2312 Catalysts 2015, 5 2312 Figure 1. Time online analysis of allyl alcohol epoxidation with TS-1. Reaction conditions: Figure 1. Time online analysis of allyl alcohol epoxidation with TS-1. Reaction conditions: Figure 1. Time online analysis of allyl alcohol epoxidation with TS-1. Reaction conditions: [allyl alcohol] = 0.5 M, [H O ] = 0.25 M, mass TS-1 = 50 mg, various temperatures. 22 [allyl alcohol] = 0.5 M, [H2O2] = 0.25 M, mass TS-1 = 50 mg, various temperatures. [allyl alcohol] = 0.5 M, [H2O2] = 0.25 M, mass TS-1 = 50 mg, various temperatures. FigurFeig2u.Treim2.eToinmlieneonalnianleysainsaolyfsailslyolfaalclloyhloalceophooxlideaptoioxnidwatiitohnTwS-i1thBT.RS-e1aBc.tiRoenacotinodnitions: Figure 2. Time online analysis of allyl alcohol epoxidation with TS-1B. Reaction conditions: [allylcaolncdoihtoiol]ns=: [0al.l5ylMal,co[Hho2Ol]2=]0=.50M.2,5[HM2O, 2m]a=ss0.2T5SM-1,Bm=ass50TSm-1gB,=va5r0iomugs,tveamripoeursatures. [allyl alcohol] = 0.5 M, [H2O2] = 0.25 M, mass TS-1B = 50 mg, various temperatures. temperatures. Conversion is calculated according to the initial concentration of Conversion is calculated according to the initial concentration of H2O2 (see Conversion is calculated according to the initial concentration of H2O2 (see H O (see experimental section ). 22 experimental section). experimental section). Further changes in catalytic performance may also be observed from the conversion versus selectivity Further changes in catalytic performance may also be observed from the conversion versus selectivity plots in Figure 4, determined at maximum levels of conversion. Although both catalysts are almost plots in Figure 4, determined at maximum levels of conversion. Although both catalysts are almost exclusively selective to the main product, glycidol, up to a peroxide conversion level of 80%, exclusively selective to the main product, glycidol, up to a peroxide conversion level of 80%, it is clear that TS-1B is able to maintain excellent glycidol selectivity even at substantially higher levels it is clear that TS-1B is able to maintain excellent glycidol selectivity even at substantially higher levels of peroxide conversion. Indeed, whilst glycidol selectivity decreases rapidly to ±85% at 95% conversion of peroxide conversion. Indeed, whilst glycidol selectivity decreases rapidly to ±85% at 95% conversion 103 with TS-1, glycidol selectivity remains well above 90% throughout the conversion range for TS-1B.PDF Image | Zeolite Catalysis
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