The combination of titanium silicalite-1 (TS-1) zeolite and HO oxidant provides an excellent alternative to many highly toxic and polluting olefin oxidation processes due to the by-product being water-only and without deep oxidation. However, the diffusion of bulky reactants and products suffers from the inherent micropores of conventional TS-1 zeolites. Herein, we designed a reticulated ordered macroporous carbon material with uniform and coherent mesopores, and successfully synthesized ordered hierarchical TS-1 zeolites containing intracrystalline macroporous-mesoporous-microporous by dry gel method. The fully interconnected intracrystalline macroporous-mesoporous-microporous hierarchical TS-1 improves the accessibility of the active site and the diffusion efficiency of bulky compounds. It showed excellent catalytic performance during the epoxidation reaction of chloropropene, and its epichlorohydrin yield and HO effective utilization were 70.11% and 77.05%, which were 2.2 and 1.9 times of the catalytic performance of commercial TS-1 zeolites, respectively, and significantly better than the ultrafine TS-1 synthesized by conventional methods. The high catalytic performance was maintained after three cycles of use. This offers a good opportunity for the design and synthesis of efficient zeolite catalysts in the future.

中文翻译：

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用有序大孔-介孔碳模板制备分级TS-1沸石用于高效氯丙烯环氧化

钛硅沸石-1 (TS-1) 沸石和 H2O 氧化剂的组合为许多高毒性和污染性的烯烃氧化工艺提供了极好的替代方案，因为其副产物仅是水且无需深度氧化。然而，大体积反应物和产物的扩散受到传统 TS-1 沸石固有微孔的影响。在此，我们设计了一种具有均匀、连贯介孔的网状有序大孔碳材料，并通过干凝胶法成功合成了含有晶内大孔-介孔-微孔的有序分级TS-1沸石。完全互连的晶内大孔-介孔-微孔分级TS-1提高了活性位点的可及性和大体积化合物的扩散效率。在氯丙烯环氧化反应中表现出优异的催化性能，其环氧氯丙烷收率和H2O有效利用率分别为70.11%和77.05%，分别是商用TS-1沸石催化性能的2.2和1.9倍，显着优于商用TS-1沸石。采用常规方法合成的超细TS-1。经过三个循环使用后仍保持较高的催化性能。这为未来高效沸石催化剂的设计和合成提供了良好的机会。