Regulating the Coordination Mode of Ti Atoms in the Beta Zeolite Framework to Enhance the 1-Hexene Epoxidation

被引：5

作者：

Deng, Xuliang ^{[1
,2
]}

Xu, Yang ^{[1
]}

Liu, Jincheng ^{[2
]}

Lin, Dong ^{[4
]}

Zong, Ze ^{[1
]}

Yuan, Juncong ^{[1
]}

Li, Zhiyang ^{[1
]}

Zhao, Guanghui ^{[2
]}

Zhang, Yongjun ^{[2
]}

Liu, Yibin ^{[1
]}

Chen, Xiaobo ^{[1
]}

Feng, Xiang ^{[1
]}

Chen, De ^{[1
,3
]}

Yang, Chaohe ^{[1
]}

Shan, Honghong ^{[1
]}

机构：

[1] China Univ Petr, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China

[2] CNPC, PetroChina Petrochem Res Inst, Daqing Chem Res Ctr, Daqing City 163000, Peoples R China

[3] Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

[4] Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Max Planck Cardiff Ctr Fundamentals Heterogeneous, Cardiff CF103AT, Wales

来源：

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH | 2024年 / 63卷 / 09期

关键词：

D O I：

10.1021/acs.iecr.3c03543

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

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.

引用

页码：3817 / 3826

页数：10

共 26 条

[1] 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
Shan, Honghong
Industrial and Engineering Chemistry Research, 2024, 63 (09): : 3817 - 3826
[2] Zeolite structure descriptor for guiding the synthesis of efficient titanosilicalites through matching Ti sites and framework topologies for 1-Hexene epoxidation
Deng, Xuliang
Lin, Dong
Xu, Yang
Feng, Xiang
Chen, De
Yang, Chaohe
Shan, Honghong
CHEMICAL ENGINEERING JOURNAL, 2024, 487
[3] Synthesis of Ti-MWW Zeolite by Refluxing and Implanting Titanium Method and Further Application in 1-Hexene Epoxidation
Chu, Jidong
Ge, Zhijin
Peng, Jiahui
Hu, Hui
Guo, Shujuan
Chen, Xiaohui
CATALYSIS LETTERS, 2023, 153 (02) : 348 - 363
[4] Synthesis of Ti-MWW Zeolite by Refluxing and Implanting Titanium Method and Further Application in 1-Hexene Epoxidation
Jidong Chu
Zhijin Ge
Jiahui Peng
Hui Hu
Shujuan Guo
Xiaohui Chen
Catalysis Letters, 2023, 153 : 348 - 363
[5] Ammonia-regulated dynamic evolution of Ti precursor incorporating into dealuminized beta for efficient 1-Hexene epoxidation
Xu, Yang
Lin, Dong
Zong, Ze
He, Qiuming
Ma, Zhe
Deng, Xuliang
Chen, De
Yang, Chaohe
Feng, Xiang
CHEMICAL ENGINEERING SCIENCE, 2024, 300
[6] Epoxidation of 1-hexene with hydrogen peroxide over nitrogen-incorporated TS-1 zeolite
Li, Hao
Xu, Bo
Deng, Bangwei
Yan, Xuemin
Zheng, Yancheng
CATALYSIS COMMUNICATIONS, 2014, 46 : 224 - 227
[7] Lysine-assisted synthesis of plate-like TS-1 zeolite for 1-hexene epoxidation
Dai, Weijiong
Zhao, Jing
Liu, Zongqiang
Zheng, Jiajun
Li, Ruifeng
MATERIALS TODAY SUSTAINABILITY, 2024, 27
[8] Alkylation of anisole with 1-hexene and 1-hexanol over zeolite H-beta
P. V. Surse
S. Wagholikar
S. Mayadevi
S. Sivasanker
Reaction Kinetics, Mechanisms and Catalysis, 2011, 103 : 481 - 491
[9] Alkylation of anisole with 1-hexene and 1-hexanol over zeolite H-beta
Surse, P. V.
Wagholikar, S.
Mayadevi, S.
Sivasanker, S.
REACTION KINETICS MECHANISMS AND CATALYSIS, 2011, 103 (02) : 481 - 491
[10] Synthesis of Sheet-like Zeolite TS-1 with Short b-Axis for Epoxidation of 1-Hexene
Zhang, Min
Ren, Shenyong
Guo, Qiaoxia
Shen, Baojian
CHEMISTRYSELECT, 2023, 8 (10):

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