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...
Main Authors: | , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
MDPI AG
2022-10-01
|
Series: | Catalysts |
Subjects: | |
Online Access: | https://www.mdpi.com/2073-4344/12/10/1241 |
_version_ | 1797474412474138624 |
---|---|
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. |
first_indexed | 2024-03-09T20:30:41Z |
format | Article |
id | doaj.art-fda8c4a04fc6477b84d49000b93b90a8 |
institution | Directory Open Access Journal |
issn | 2073-4344 |
language | English |
last_indexed | 2024-03-09T20:30:41Z |
publishDate | 2022-10-01 |
publisher | MDPI AG |
record_format | Article |
series | Catalysts |
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 |
work_keys_str_mv | AT xinyuchang hydrothermalmodificationofts1zeoliteswithorganicaminesandsaltstoconstructhighlyselectivecatalystsforcyclopenteneepoxidation AT yutingsun hydrothermalmodificationofts1zeoliteswithorganicaminesandsaltstoconstructhighlyselectivecatalystsforcyclopenteneepoxidation AT xiaojingsong hydrothermalmodificationofts1zeoliteswithorganicaminesandsaltstoconstructhighlyselectivecatalystsforcyclopenteneepoxidation AT xiaotongyang hydrothermalmodificationofts1zeoliteswithorganicaminesandsaltstoconstructhighlyselectivecatalystsforcyclopenteneepoxidation AT yuqingwu hydrothermalmodificationofts1zeoliteswithorganicaminesandsaltstoconstructhighlyselectivecatalystsforcyclopenteneepoxidation AT mingjunjia hydrothermalmodificationofts1zeoliteswithorganicaminesandsaltstoconstructhighlyselectivecatalystsforcyclopenteneepoxidation |