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chemical works, Beijing, China. All chemicals were used as received without any further purification. 3.2. Synthesis of Pristine TS-1 Zeolite In a typical synthesis, 8.0 mL of TPAOH, 5.0 mL of TEOS and 5.0 mL of water were mixed and stirred at room temperature for 24 h to form solution A; 0.2 mL of TBOT was added into 10.0 mL of 30% H2O2 aqueous to form solution B. The solution B was added dropwise into solution A under stirring, and a clear sol was obtained after 24 h. The obtained sol was taken in a Teflon container and placed in a stainless steel autoclave. The sol was hydrothermally treated at 100 ◦C for 24 h. The TS-1 zeolites were collected through centrifugation and then washed several times with water and ethanol. 3.3. Synthesis of Core-Shell TS-1@mesosilica Composites The core-shell TS-1@mesosilica composite was prepared via a uniform coating process, according to our previous reports [29,30]. In a typical synthesis, 100 mg of the as-prepared TS-1 zeolite was homogeneously dispersed in a mixture containing 22 mL of water and 11 mL of ethanol by ultrasonication for 30 min. The resultant mixture was stirred at room temperature for 30 min followed by sequential addition of 0.12 g of CTAB, 0.25 mL of ammonium aqueous solution (25%–28%), and 0.15 mL of TEOS. The as-obtained white mixture was further stirred at room temperature for 6 h. The core-shell structured TS-1@mesosilica composites were collected by centrifugation and then washed with water and ethanol several times. Finally, the organic structure directing agent TPA+ and the surfactant CTAB were removed by calcination at 550 ◦C in air for 6 h. 3.4. Synthesis of Yolk-Shell TS-1@Mesosilica Composites The yolk-shell structured TS-1@mesosilica composite was prepared using an RF middle-layer as the sacrificial template. In a typical synthesis, 200 mg of the as-prepared TS-1 zeolite was homogeneously dispersed in a mixture containing 17.5 mL of water and 11 mL of ethanol by ultrasonication for 30 min. To the above solution were added 0.575 g of CTAB, 0.025 mL of ammonium aqueous solution (25%–28%) and 0.12 g of resorcinol sequentially and the resultant mixture was stirred at 35 ◦C for 30 min. Then, 0.3 mL of formalin solution was added to the dispersion under stirring maintaining 35 ◦ C for 6 h. The mixture was cooled to room temperature after 6 h, and then aged at room temperature overnight without stirring. The product (designated as TS-1@RF) was collected by centrifugation and then washed with water and ethanol several times. Next, a uniform mesosilica layer was coated on the surface of TS-1@RF similarly like TS-1@mesosilica to form TS-1@RF@mesosilica. Finally, the yolk-shell structured TS-1@mesosilica composite was obtained after removal of the 149PDF Image | Zeolite Catalysis
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