Development of a titanium silicalite-1(TS-1)catalyst with good crystallinity and a four-coordinate Ti framework is critical for efficient catalytic oxidation reaction under mild conditions.Herein,a size-controlled TS-...Development of a titanium silicalite-1(TS-1)catalyst with good crystallinity and a four-coordinate Ti framework is critical for efficient catalytic oxidation reaction under mild conditions.Herein,a size-controlled TS-1 zeolite(TS-10.1ACh(acetylcholine))was synthesized via steam-assisted crystallization by introducing acetylcholine as a crystal growth modifier in the preparation process,and TS-10.1ACh was also employed in epoxidations of different substrates containing C=C double bonds.The crystalline sizes of the as-synthesized TS-10.1ACh catalysts were controlled with the acetylcholine content,and characterization results showed that the particle sizes of highly crystalline TS-10.1ACh zeolite reached 3.0μm with a good Ti framework.Throughout the synthetic process,the growth rate of the crystals was accelerated by electrostatic interactions between the connected hydroxyl groups of the acetylcholine modifier and the negatively charged skeleton of the pre-zeolites.Furthermore,the TS-10.1ACh catalyst demonstrated maximum catalytic activity,good selectivity and high stability during epoxidation of allyl chloride.Importantly,the TS-10.1ACh catalyst was also highly versatile and effective with different unsaturated substrates.These findings may provide novel,easily separable and large TS-1 catalysts for efficient and clean industrial epoxidations of C=C double bonds.展开更多
基金supported by the financial support from the National Natural Science Foundation of China(Grant Nos.21802055 and 32160537)Jiangxi Provincial Natural Science Foundation(Grant No.20202BABL205013)Jiangxi Provincial Department of Education Foundation(Grant No.GJJ190179).
文摘Development of a titanium silicalite-1(TS-1)catalyst with good crystallinity and a four-coordinate Ti framework is critical for efficient catalytic oxidation reaction under mild conditions.Herein,a size-controlled TS-1 zeolite(TS-10.1ACh(acetylcholine))was synthesized via steam-assisted crystallization by introducing acetylcholine as a crystal growth modifier in the preparation process,and TS-10.1ACh was also employed in epoxidations of different substrates containing C=C double bonds.The crystalline sizes of the as-synthesized TS-10.1ACh catalysts were controlled with the acetylcholine content,and characterization results showed that the particle sizes of highly crystalline TS-10.1ACh zeolite reached 3.0μm with a good Ti framework.Throughout the synthetic process,the growth rate of the crystals was accelerated by electrostatic interactions between the connected hydroxyl groups of the acetylcholine modifier and the negatively charged skeleton of the pre-zeolites.Furthermore,the TS-10.1ACh catalyst demonstrated maximum catalytic activity,good selectivity and high stability during epoxidation of allyl chloride.Importantly,the TS-10.1ACh catalyst was also highly versatile and effective with different unsaturated substrates.These findings may provide novel,easily separable and large TS-1 catalysts for efficient and clean industrial epoxidations of C=C double bonds.
