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ctors (see above) strongly suggest that these factors are related. We consider there to be two potenti ays that the extraction of framework Ti could lead to such pronounced changes. The first possibility at NH4HF2 treatment removes a particularly non-selective framework [Ti(OSi)4] site, responsible f oth epoxidation and undesirable decomposition. Alternatively, the extraction of framework Ti coul result in the formation of active, extra-framework Ti complexes, which may provide sult in the formation of active, extra-framework Ti complexes, which may provide an alternati an alternative pathway for H2O2 activation. In light of the in situ UV-Raman analysis (Figure 10), we favour the latter. Given the narrow FWHM observed in athway for H2O2 activation. In light of the in situ UV-Raman analysis (Figure 10), we favour the latte the UV-Vis spectrum of TS-1B (ESI Figure S2), and the generation of only one new iven the narrow FWHM observed in the UV-Vis spectrum of TS-1B (ESI Figure S2), and t Raman active mode, we hypothesise that any extra-framework complex must be eneration of only one new Raman active mode, we hypothesise that any extra-framework complex mu either mononuclear, or of low nuclearity (cf. dimeric). Although reports suggest e either monmoonuocnluecalre,aro,rexotrfa-lforawmenwucolrekaTrittyob(cefi.nadcitmiverfiocr).epAolxtihdoautigohn[r2e6p],osretsvesraulgrgeecesnttmononuclea tra-framework Ti to be inactive for epoxidation [26], several recent reports have highlighted t reports have highlighted the potential for two concerted Ti sites to catalyse epoxidation reactions: Kortz et al. demonstrated that a polyoxometallate containing a unique otential for two concerted Ti sites to catalyse epoxidation reactions: Kortz et al. demonstrated that di-titanium centre ([Ti2(OH)2As2W19O67(H2O)] [8]) is able to activate H2O2 for olyoxometallate containing a unique di-titanium centre ([Ti2(OH)2As2W19O67(H2O)] [8]) is able t epoxidation catalysis [27], and the barrier calculated for H2O2 activation over a model −1 tivate H2O2Tfoi-rdeimpoerxicdoamtipolnexcwataslyfosiusn[d2t7o],baen5d3.t5hkeJ·bmarorlierbcyalLcunladtiendetfoalr. H[228O] T2haicstvivaalutieoins over a mod especially close to the experimental barrier of TS-1B. Definitive identification of the i-dimer complex was found to be 53.5 kJ·mol−1 by Lundin et al. [28] This value is especially close to t new active sites, and their potential role in the epoxidation/decomposition process, perimental barrier of TS-1B. Definitive identification of the new active sites, and their potential role i will require further (in situ) spectroscopic study with complimentary techniques, e epoxidation/decomposition process, will require further (in situ) spectroscopic study wit such as X-ray Absorption spectroscopy and computational methodologies. These mplimentaraydtdeictihoniaqluspese,ctsruoscchopaisc,Xco-rmaypuAtabtisonrapltaionnd kspineecttircosstcuodpieys raenmdacinomthpeufotactuisonofaloumrethodologie hese additional spectroscopic, computational and kinetic studies remain the focus of our on-going work. Figure 10. In situ UV-Raman (325 nm) spectra of (red) TS-1B and (purple) TS-1B igure 10. In situ UV-Raman (325 nm) spectra of (red) TS-1B and (purple) TS-1B treated with H2O2 on-going work. treated with H2O2. . Experimental Section .1. Catalyst Synthesis and Pre-Treatment TS-1 was prepared according to a method descr1i1b2ed elsewhere [29]. TS-1B was prepared as follow S-1 (4 g) was suspended in an aqueous solution (80 mL) containing NH4HF2 (120 mg) and H2 aa wi ho ev Gh s xh ce Th x h os T F s TOPDF Image | Zeolite Catalysis
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