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middle-layer RF, surfactant CTAB and structure direct agent TPA+ by calcination at 550 ◦C in air for 6 h. 3.5. Catalytic Tests In a typical catalytic reaction, desired amount of catalyst (containing 40 mg of TS-1 zeolite), 1.0 g of phenol, 0.36 mL of H2O2 and 10 mL of H2O were mixed in a 50 mL round-bottomed flask equipped with a reflux condenser and a magnetic stirrer. After reaction at 80 ◦C for 5 h, the products were collected and analyzed by GC. 3.6. Materials Characterization SEM images were taken with a JSM-6700F field-emission electron microscope (JEOL, Tokyo, Japan). TEM images were obtained from an Tecnai G2 F20s-twin D573 field emission transmission electron microscope (FEI, Hillsboro, FL, USA) at an accelerating voltage of 200kV. Powder XRD patterns were obtained by using a 2550 diffractometer (Rigaku, Tokyo, Japan) with Cu Ka radiation (λ = 1.5418 Å). N2 adsorption-desorption isotherms were obtained at −196 ◦C on a ASAP 2010 sorptometer (Micromeritics, Shanghai, China). Samples were degassed at 120 ◦C for a minimum of 12 h prior to analysis. BET surface areas were calculated from the linear part of the BET plot. Pore size distribution was estimated from the adsorption branch of the isotherm by the BJH method. The total pore volume was estimated from the adsorbed amount of nitrogen at P/P0 = 0.995. 4. Conclusions In summary, we have prepared two kinds of TS-1-based nanocomposites, namely, core-shell structured TS-1@mesosilica and yolk-shell structured TS-1@mesosilica. These nanocomposites showed highly uniform morphology and structure, high BET surface area, and hierarchical pore structures from oriented mesochannels to zeolite micropores. When used as catalysts in the hydroxylation of phenol with H2O2 as the oxidant, they exhibited enhanced activity and unique selectivity. We found that the external mesosilica shell and the void space between the mesosilica shell and the TS-1 core not only captured phenol molecules like a pump for enhanced activity but also posed diffusion resistance for negative selectivity. Moreover, these nanocomposites presented higher selectivity of the para-product. The current work is expected to offer some insights into designing of multifunctional zeolites-based nanocomposites for enhanced oxidation reactions. Acknowledgments: This work was supported by National Natural Science Foundation of China (21390394), the National Basic Research Program of China (2012CB821700, 2011CB808703), NSFC (21261130584, 91022030), “111” project (B07016), Award Project of KAUST (CRG-1-2012-LAI-009) and Ministry of Education, Science and Technology Development Center Project (20120061130012). 150PDF Image | Zeolite Catalysis
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