Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method us...Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method usually required a large amount of aqueous solution of organic template,leading to unfavorable polluted waste,low production efficiency,and high manufacture cost.Here,a facile and environmental friendly strategy was proposed for the post-synthesis of hollow TS-1 zeolite with a solventfree method utilizing NH4HCO3 and tetrapropylammounium bromide as selective etching agents,which reduced the usage of organic template and avoided the liquid waste.The high crystallinity,the microporous structure,and the active Ti sites were preserved at a high product yield(>93%).The formation mechanism of hollow structure was also investigated by exploring effects of different reactants and experimental parameters.Meanwhile,the obtained hollow TS-1 showed an outstanding performance in the epoxidation of 1-hexene in comparison to the parent zeolite.展开更多
基金This work was supported by the National Natural Science Foundation of China(Nos.21875140,21835002,21522105,and 51861145313)the Shanghai Science and Technology Plan(No.21DZ2260400)+4 种基金the China Ministry of Science and Technology(No.2021YFA1501401)The authors thank the support from Analytical Instrumentation Center(No.SPSTAIC10112914)SPST,ShanghaiTech UniversityThe authors also thank Prof.Osamu Terasaki and CħEM SPST,ShanghaiTech University(No.EM02161943)for scientific and characterization support.Y.F.thanks Junyan Li(Jilin University)for his assistance in 3D tomographic data collection.
文摘Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method usually required a large amount of aqueous solution of organic template,leading to unfavorable polluted waste,low production efficiency,and high manufacture cost.Here,a facile and environmental friendly strategy was proposed for the post-synthesis of hollow TS-1 zeolite with a solventfree method utilizing NH4HCO3 and tetrapropylammounium bromide as selective etching agents,which reduced the usage of organic template and avoided the liquid waste.The high crystallinity,the microporous structure,and the active Ti sites were preserved at a high product yield(>93%).The formation mechanism of hollow structure was also investigated by exploring effects of different reactants and experimental parameters.Meanwhile,the obtained hollow TS-1 showed an outstanding performance in the epoxidation of 1-hexene in comparison to the parent zeolite.
