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2 −1 1ar5eanmof b69et5wmeeng th(eTcaoblre 1a)n. dAtlhl ethsehselrle.sTulhtse dFeTm-oIRnstarnadtedUtVha-tVwise swpercetraabl(eFtiogusurecc4eAss,fBul)lyalpsroepraerveeal that th m between the core and the shell. The FT-IR and UV-Vis spectra (Figure 4A,B) also reveal that the TS-1-based nanocomposite consisted of a TS-1 core and a mSiO2 shell as well as a void space of around nature and coordination of Ti species keeps identical with pristine TS-1. e and coordination of Ti species keeps identical with pristine TS-1. 15 nm between the core and the shell. The FT-IR and UV-Vis spectra (Figure 4A,B) also reveal that the nature and coordination of Ti species keeps identical with pristine TS-1. Figure 5. (a) TEM image of TS-1@RF@mSiO2; (b–d) TEM images and SEM image of Figure 5. (a) TEM image of TS-1@RF@mSiO2; (b–d) TEM images and SEM image of FigurFeig5u.r(ea)5.T(EaM)TEimMagimeaogfeToSf-T1S@-1R@FR@F@mSiiO2;(b–d))TEEMMimimagaegsesanadndSESMEMimaimgeageof 2 YS-TS-1@mSiO2; (e) N2 sorption isotherms of pristine TS-1 (●), TS-1@RF (●) and YS-TS-1@mYSi-OT2So;f-1Y(@eS)-mTSNS-1i2O@ms;oSr(ipeO)t2io;N(ne)isNso2rtpshtoierorpnmtiosisnooitshfoethrpmerrismtiosnfoefpprTirsiSstti-in1nee(T●S)-,-11(T(S)●,-)T1,S@-T1SR@-RF1F@(●R)Faan(n●dd) and 22 YS-TYS-T1S@-1m@mSSiOiO2 (▲);;(f()fR)eRlevlaenvtaDnFtTDpFoTrepsiozeredisitzriebudtisotnricbuurvtieoonfYcuS-rTvSe-1o@fmYSSiO-T.S-1@mSiO2. 22 YS-TS-1@mYSi-OT2S-(1▲@)m; (Sfi)OR2 e(▲lev);a(nft) DReFlTevpanotreDsFiTzepdoriestsrizbeudtiiosntricburtivoen ocfurYveS-oTf SY-S1-@TSm-1S@iOm2S. iO2. 2.3. Catalytic Performance of CS/YS-TS-1@mSiO2 in Hydroxylation of Phenol Table 2 summarizes the catalytic results of various TS-1 catalysts in the hydroxylation of phenol using H2O2 as the oxidant and water as the solvent. The pristine TS-1 material (Entry 3) showed similar activity and selectivity with previous reports [12,13]. Notably, our prepared composites CS-TS-1@mSiO2 (Entry 6) and YS-TS-1@mSiO2 (Entry 9) gave a higher phenol conversion of 25.2% and 27.6% than that of pristine TS-1 (23.7%), respectively. The turnover frequency (TOF) of YS-TS-1@mSiO2 (34.4) was even higher than some other hierarchical nanoporous TS-1 zeolite materials [18]. The enhanced activities should be attributed to the effect of external mesosilica layer that can effectively capture the large phenol molecules like a pump from the reaction solution due to the large specific surface area of mesopores. This “capture” effect was also reported for enhanced catalytic cracking reactions in previous publication [25]. Moreover, the void space between the mSiO2 shell and the TS-1 core reinforced this positive “capture” effect for further enhancing the catalytic activity of material. In addition, we were aware that the selectivity of side product benzoquinone was slightly increased from 3.9% to 5.5% using our composites as the catalysts, which indicated that the external mesosilica layer and the void space also adsorbed products catechol and hydroquinone when capturing substrate phenol from reaction solution, and thus led to further oxidation. Moreover, it is worth mentioning that more product hydroquinone was produced in the cases of using composites CS-TS-1@mSiO2 and YS-TS-1@mSiO2 as catalysts. These catalytic 147PDF Image | Zeolite Catalysis
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