| 薛晓璐,高鹏飞,张磊,赵永祥.微波法合成氟改性TS-1及其催化环己酮氨肟化性能[J].分子催化,2019,33(1):27-40 |
| 微波法合成氟改性TS-1及其催化环己酮氨肟化性能 |
Fluorinated TS-1 Prepared by Microwave Irradiation and Its
Catalytic Performance on Ammoximation of Cyclohexanone |
| 投稿时间：2018-12-09 修订日期：2019-01-07 |
| DOI： |
| 中文关键词: 氟改性TS-1 微波辐射 路易斯酸 疏水性 氨肟化 |
| 英文关键词:fluorinated TS-1 microwave irradiation lewis acidity hydrophobicity ammoximation |
| 基金项目:The financial supports from the National Natural Science Foundation of China (Project NO. 21403135), and Shanxi provincial key research and development plan project (NO. 201603D121018-1) are gratefully acknowledged. |
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| 中文摘要: |
| 通过微波辅助法制备了含氟的TS-1（F-TS-1-M），并与传统方法制备的氟改性TS-1（F-TS-1-T），微波处理的TS-1（TS-1-M）和未改性TS-1进行比较.XRD、DR UV-Vis、XPS表明F-TS-1-M和TS-1-M分子筛上的部分非骨架钛转变为骨架钛，这是由于微波的选择性效应可以不同程度地活化Ti—O和Si—O键；19F MAS NMR证实了F-TS-1-M分子筛中氟元素是以Si-F和SiF62-的形式存在；29Si MAS NMR表明F-TS-1-M分子筛的骨架缺陷位和表面羟基减少，Py-FT-IR结果表明F-TS-1-M的Lewis酸性和疏水性高于F-TS-1-T、TS-1-M和TS-1.在环己酮氨肟化的反应中表现出优异的催化性能. |
| 英文摘要: |
| Fluorinated TS-1 (F-TS-1-M) were prepared by treating TS-1 in dimethyl sulfoxide solution of sodium fluoride under the assistance of microwave in this work. The characterization results showed that F-TS-1-M presented increased amount of tetrahedral framework Ti thanks to the selective effect of microwave irradiation on activating M-O bonds with different dipole moments which could lead to the transformation of non-framework Ti4+ to framework Ti4+. In addition, F-TS-1-M exhibited stronger Lewis acidity and hydrophobicity due to the reduced skeleton defects and surface hydroxyls. As a result, F-TS-1-M showed enhanced catalytic activity in the ammoximation of cyclohexanone. |
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