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Role of pentahedrally coordinated titanium in titanium silicalite-1 in propene epoxidation

发表时间:2019-03-09
点击次数:
论文类型:
期刊论文
第一作者:
Zuo, Yi
通讯作者:
Guo, XW (reprint author), Dalian Univ Technol, State Key Lab Fine Chem, PSU DUT Joint Ctr Energy Res, Sch Chem Engn, Dalian 116024, Peoples R China.
合写作者:
Fischer, Daniel,Liu, Min,Zhang, Ting,Hong, Luwei,Guo, Xinwen,Song, Chunshan,Chen, Yongsheng,Zhu, Pengyu,Jaye, Cherno
发表时间:
2015-01-01
发表刊物:
RSC ADVANCES
收录刊物:
SCIE、EI、Scopus
文献类型:
J
卷号:
5
期号:
23
页面范围:
17897-17904
ISSN号:
2046-2069
摘要:
Two titanium silicalite-1 samples with different crystal sizes were synthesized in the tetrapropylammonium bromide (TPABr) and tetrapropylammonium hydroxide (TPAOH) hydrothermal systems. The small-crystal TS-1 with a size of 600 nm was then treated with different organic bases. These TS-1 samples were evaluated in the epoxidation of propene, and characterized by ultraviolet-visible diffuse reflectance (UV-vis), X-ray absorption near edge structure (XANES) and Raman spectroscopies. The Ti L-edge absorption spectra show that a new Ti species, pentahedrally coordinated Ti, appears in some of the samples. This pentahedrally coordinated Ti species is correlated with the catalytic oxidation activity of TS-1, closely. Tetrahedrally coordinated Ti in TS-1 is the primary active center for selective oxidation reactions, but the existence of a small amount of pentahedrally coordinated Ti can further improve the catalytic activity. A high molar ratio of Si/Ti (n(Si/Ti)) in the synthesis process (n(Si/Ti) = 92.78) was beneficial for the generation of pentahedrally coordinated Ti. The improved catalytic activity of the TPAOH treated TS-1 is mainly due to the increasing amount of pentahedrally coordinated Ti, besides the elimination of diffusion limitation. Slowing down the crystallization rate can also increase the content of pentahedrally coordinated Ti.
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