Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation

Developing efficient heterogeneous catalysts for cyclic olefins epoxidation is highly attractive for meeting the growing need for various cyclic epoxides. Herein, hierarchical TS-1 zeolite with relatively abundant mesopores and less amount of surface hydroxyl groups was obtained by hydrothermal modi...

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Main Authors: Xin-Yu Chang, Yu-Ting Sun, Xiao-Jing Song, Xiao-Tong Yang, Yu-Qing Wu, Ming-Jun Jia
Format: Article
Language:English
Published: MDPI AG 2022-10-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/12/10/1241
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author Xin-Yu Chang
Yu-Ting Sun
Xiao-Jing Song
Xiao-Tong Yang
Yu-Qing Wu
Ming-Jun Jia
author_facet Xin-Yu Chang
Yu-Ting Sun
Xiao-Jing Song
Xiao-Tong Yang
Yu-Qing Wu
Ming-Jun Jia
author_sort Xin-Yu Chang
collection DOAJ
description Developing efficient heterogeneous catalysts for cyclic olefins epoxidation is highly attractive for meeting the growing need for various cyclic epoxides. Herein, hierarchical TS-1 zeolite with relatively abundant mesopores and less amount of surface hydroxyl groups was obtained by hydrothermal modification of an as-synthesized TS-1 zeolite with a mixed solution of ammonia, tetrapropylammonium bromide (TPABr) and KCl. The post-modified TS-1 zeolite exhibited much higher catalytic activity (52% conversion) and epoxide selectivity (98%) for the epoxidation of cyclopentene than the conventional TS-1 zeolites. The excellent catalytic activity of the hierarchical TS-1 could be mainly assigned to the enhancement of the mass transport ability and the accessibility of the active Ti species, while the improvement of epoxidation selectivity may be mainly related to the introduction of a certain amount of K<sup>+</sup> that can effectively modulate the coordination environment of Ti species as well as the polarity of the zeolite. This work demonstrated that a highly active and selective catalyst for the H<sub>2</sub>O<sub>2</sub>-mediated cyclopentene epoxidation could be obtained by concurrently generating mesopore and extinguishing the unfavorable defective hydroxyl groups through the simple hydrothermal treatment of the conventional TS-1 zeolite with a mixed base/salt solution.
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spelling doaj.art-fda8c4a04fc6477b84d49000b93b90a82023-11-23T23:26:01ZengMDPI AGCatalysts2073-43442022-10-011210124110.3390/catal12101241Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene EpoxidationXin-Yu Chang0Yu-Ting Sun1Xiao-Jing Song2Xiao-Tong Yang3Yu-Qing Wu4Ming-Jun Jia5Key Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, ChinaKey Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, ChinaKey Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, ChinaKey Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, ChinaState Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical Chemistry, College of Chemistry, Jilin University, Changchun 130012, ChinaKey Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130012, ChinaDeveloping efficient heterogeneous catalysts for cyclic olefins epoxidation is highly attractive for meeting the growing need for various cyclic epoxides. Herein, hierarchical TS-1 zeolite with relatively abundant mesopores and less amount of surface hydroxyl groups was obtained by hydrothermal modification of an as-synthesized TS-1 zeolite with a mixed solution of ammonia, tetrapropylammonium bromide (TPABr) and KCl. The post-modified TS-1 zeolite exhibited much higher catalytic activity (52% conversion) and epoxide selectivity (98%) for the epoxidation of cyclopentene than the conventional TS-1 zeolites. The excellent catalytic activity of the hierarchical TS-1 could be mainly assigned to the enhancement of the mass transport ability and the accessibility of the active Ti species, while the improvement of epoxidation selectivity may be mainly related to the introduction of a certain amount of K<sup>+</sup> that can effectively modulate the coordination environment of Ti species as well as the polarity of the zeolite. This work demonstrated that a highly active and selective catalyst for the H<sub>2</sub>O<sub>2</sub>-mediated cyclopentene epoxidation could be obtained by concurrently generating mesopore and extinguishing the unfavorable defective hydroxyl groups through the simple hydrothermal treatment of the conventional TS-1 zeolite with a mixed base/salt solution.https://www.mdpi.com/2073-4344/12/10/1241hierarchical TS-1 zeolitecyclopentene epoxidationbasic solution modificationhydrothermal treatmenthydrophobicity
spellingShingle Xin-Yu Chang
Yu-Ting Sun
Xiao-Jing Song
Xiao-Tong Yang
Yu-Qing Wu
Ming-Jun Jia
Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
Catalysts
hierarchical TS-1 zeolite
cyclopentene epoxidation
basic solution modification
hydrothermal treatment
hydrophobicity
title Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
title_full Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
title_fullStr Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
title_full_unstemmed Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
title_short Hydrothermal Modification of TS-1 Zeolites with Organic Amines and Salts to Construct Highly Selective Catalysts for Cyclopentene Epoxidation
title_sort hydrothermal modification of ts 1 zeolites with organic amines and salts to construct highly selective catalysts for cyclopentene epoxidation
topic hierarchical TS-1 zeolite
cyclopentene epoxidation
basic solution modification
hydrothermal treatment
hydrophobicity
url https://www.mdpi.com/2073-4344/12/10/1241
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