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Nano Research 2023, 16(1): 1740-1747 https://doi.org/10.1007/s12274-022-4789-1
Research Article | Issue | Published: 15 August 2022

Post-synthesis and structural evolution of hollow titanium silicalite-1 with solvent-free method

Show Author's Information Yaqi Fan1,2,§,  Xianchen Gong3,§,  Xiaomeng Si1,2,  Changjiu Xia4,  Peng Wu3,5( ),  Yanhang Ma1,2( )
Shanghai Key Laboratory of High-resolution Electron Microscopy, ShanghaiTech University, Shanghai 201210, China
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China
State Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China
Institute of Eco-Chongming, Shanghai 202162, China

§ Yaqi Fan and Xianchen Gong contributed equally to this work.

Keywords:
structural evolution, hollow structure zeolite, post synthesis method, solvent-free, TS-1
Topics:
Physicochemical properties
Cite this article:
Fan Y, Gong X, Si X, et al. Post-synthesis and structural evolution of hollow titanium silicalite-1 with solvent-free method. Nano Research, 2023, 16(1): 1740-1747. https://doi.org/10.1007/s12274-022-4789-1
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Abstract Full text Electronic supplementary material About this article

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 solvent-free 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.


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Electronic supplementary material
About this article

Post-synthesis and structural evolution of hollow titanium silicalite-1 with solvent-free method

Show Author's information Yaqi Fan1,2,§, Xianchen Gong3,§, Xiaomeng Si1,2, Changjiu Xia4, Peng Wu3,5( ), Yanhang Ma1,2( )
Shanghai Key Laboratory of High-resolution Electron Microscopy, ShanghaiTech University, Shanghai 201210, China
School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China
State Key Laboratory of Catalytic Materials and Reaction Engineering, Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China
Institute of Eco-Chongming, Shanghai 202162, China

§ Yaqi Fan and Xianchen Gong contributed equally to this work.

Abstract

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 solvent-free 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.

Keywords: structural evolution, hollow structure zeolite, post synthesis method, solvent-free, TS-1

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Acknowledgements

Publication history

Received: 04 June 2022
Revised: 12 July 2022
Accepted: 17 July 2022
Published: 15 August 2022
Issue date: January 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

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), and the China Ministry of Science and Technology (No. 2021YFA1501401). The authors thank the support from Analytical Instrumentation Center (No. SPST-AIC10112914), SPST, ShanghaiTech University. The 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.

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