UV resonance Raman spectroscopic insight into titanium species and structure-performance relationship in boron-free Ti-MWW zeolite

被引:38
作者
Jin, Shaoqing [1 ]
Wang, Zhendong [1 ]
Tao, Guiju [1 ]
Zhang, Shilin [1 ,2 ]
Liu, Wei [1 ]
Fu, Wenhua [1 ]
Zhang, Bin [1 ]
Sun, Hongmin [1 ]
Wang, Yangdong [1 ]
Yang, Weimin [1 ,2 ]
机构
[1] SINOPEC Shanghai Res Inst Petrochem Technol, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 201208, Peoples R China
[2] East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
Boron-free Ti-MWW zeolite; Titanium species; UV resonance Raman; Acid treatment; Structure-performance relationship; TS-1; ZEOLITE; EXTRAFRAMEWORK TITANIUM; HYDROTHERMAL SYNTHESIS; CATALYTIC PERFORMANCE; TITANOSILICATE; EPOXIDATION; OXIDATION; SILICALITE-1; PROPYLENE; FRAMEWORK;
D O I
10.1016/j.jcat.2017.07.032
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The titanium species and structure-performance relationship in boron-free Ti-MWW zeolite have been thoroughly studied by 244 nm excited UV resonance Raman spectroscopy for the first time. It was surprisingly found out that acid treatment not only removed a part of the dominant non-framework TiOm (m = 5, 6) species but also made most of them transformed into TiO4 species, which has never been reported before. Interestingly, acid treatment of as-synthesized and directly calcined Ti-MWW resulted in the formation of active framework TiO4 species and inactive TiO4 species in amorphous SiO2 matrix, respectively. Only the samples obtained from acid treatment of as-synthesized Ti-MWW and subsequent calcination showed catalytic activity in 1-hexene epoxidation. Importantly, despite higher Si/Ti ratio, framework Ti(OSi)(4) species-dominant Ti-MWW showed better catalytic performance than the relatively hydrophilic framework Ti(OSi)(3)OH species-dominant one. These understandings would be beneficial for further study of Ti-MWW and development of highly efficient titanosilicate zeolites. (C) 2017 Elsevier Inc. All rights reserved.
引用
收藏
页码:305 / 314
页数:10
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