Regulating the coordination mode of Ti atoms in the beta zeolite framework to enhance the 1-Hexene Epoxidation

Deng, Xuliang, Xu, Yang, Liu, Jincheng, Lin, Dong, Zong, Ze, Yuan, Juncong, Li, Zhiyang, Zhao, Guanghui, Zhang, Yongjun, Liu, Yibin, Chen, Xiaobo, Feng, Xiang, Chen, De, Yang, Chaohe and Shan, Honghong 2024. Regulating the coordination mode of Ti atoms in the beta zeolite framework to enhance the 1-Hexene Epoxidation. Industrial & Engineering Chemistry Research 63 (9) , pp. 3817-3826. 10.1021/acs.iecr.3c03543

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Abstract

Regulating the Ti active sites in titanosilicates with different coordination modes is of prime scientific and industrial significance to the rational design of efficient catalysts for olefin epoxidation. In this study, the Ti species in Ti-beta zeolite catalysts (open/closed tetra-coordinated Ti sites, hexa-coordinated Ti species, and TiO2) were keenly controlled via the dealumination-metallization approach. By multiple characterizations, kinetics study, and multivariate model analysis, it is found that the open tetra-coordinated framework Ti(OH)(OSi)3 species contribute more to the catalytic performance for 1-hexene epoxidation with H2O2. Moreover, the Ti-beta with rich open tetra-coordinated Ti(OH)(OSi)3 species showed significantly improved reaction performance (TON: 401, conversion: 64%, selectivity: 98%, H2O2 efficiency: 97%) with lower apparent activation energy. This study not only opens up new prospects for the design of efficient titanosilicates by modifying Ti microenvironments but also proposes the strategy to improve the content of open tetra-coordinated Ti sites.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	American Chemical Society
ISSN:	0888-5885
Funders:	National Natural Science Foundation of China
Date of First Compliant Deposit:	26 February 2024
Date of Acceptance:	13 February 2024
Last Modified:	15 Apr 2024 13:09
URI:	https://orca.cardiff.ac.uk/id/eprint/166554

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