4.7 Article

Single-crystalline hierarchically-porous TS-1 zeolite catalysts via a solid-phase transformation mechanism

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出版社

ELSEVIER
DOI: 10.1016/j.micromeso.2020.110828

关键词

Hierarchal zeolites; Single-crystalline; Crystallization mechanism; TS-1; Carbon dioxide; Heterogeneous catalysis

资金

  1. National Natural Science Foundation of China [51602164, 21776143, 21801144]
  2. Youth Innovative Talents Recruitment and Cultivation Program of Shandong Higher Education
  3. Program for Scientific Research Innovation Team in Colleges and Universities of Shandong Province

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Hierarchically porous zeolites are a type of catalyst with improved catalytic performances compared to conventional microporous-only zeolites, due to enhanced mass transportation among meso/macropores. The strategy of controlling growth/crystallization in a solidified hydrogel system allows for the synthesis of TS-1 zeolites with hierarchical porosity, single-crystalline structure, and high catalytic performance in alkene oxidations. This method offers a cost-effective alternative to traditional synthetic methods.
Hierarchically porous zeolites are a type of very hot catalyst with improved catalytic performances as compared with conventional microporous-only zeolites due to the improved mass transportation among the hierarchical meso/macropores, which are expected to be the next-generation catalysts for conversion of bulky molecules and/ or polymers. Moreover, hierarchical zeolites with the single crystalline structure that is an identical registry of micropores within the entire particle identified the less pore blockage and less diffusion limitation compared to an aggregated structure of nano-zeolites. The developed synthetic methods were mostly conducted in a liquidphase system and usually required expensive additives, such as silanes or mesoporogons, etc. Finding facile and cost-effective synthetic methods have been still challenging. Here, a facile and cost-effective strategy by controlling the growth/crystallization in a solidified hydrogel system was reported for the synthesis of Ticontaining MFI-type zeolites (TS-1) to simultaneously achieve hierarchical porosity, single-crystalline structure, and high catalytic performance in alkene oxidations. The synthesized zeolites were characterized by XRD, SEM, TEM, Nitrogen adsorption analysis, DRUV spectroscopy, IR spectroscopy, etc. The growth processes were also tracked and well-characterized. It was found that the solid-phase transformation mechanism was dominated for forming the hierarchical structure. This strategy could directly produce TS-1 with abundant intracrystalline continuous mesopores and large amounts of active framework titanium species, contributing to higher activity for epoxidation of alkenes compared to the traditional microporous-only TS-1 zeolites.

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