Preparation of hierarchical TS-1 zeolites from ordered macroporous-mesoporous carbon templates for efficient chloropropene epoxidation

The combination of titanium silicalite-1 (TS-1) zeolite and H 2 O 2 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 H 2 O 2 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.