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新型两亲性HZSM-5沸石催化剂对环己烯水合相界面反应的催化研究

Amphiphilic HZSM-5 Zeolite Catalyst for Hydration of Cyclohexene on Phase-boundary Interface

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【作者】 马丙丽淳远周炜潘剑须沁华董家騄

【Author】 MA Bing-Li, CHUN Yuan*, ZHOU Wei, PAN Jian, XU Qin-Hua, DONG Jia-Lu(Key Laboratory of Mesoscopic Materials of Ministry of Education, Department of Chemistry, Nanjing University, Nanjing 210093, China)

【机构】 南京大学化学系介观材料教育部重点实验室介观材料教育部重点实验室 南京210093南京210093南京210093

【摘要】 采用三甲基氯硅烷对HZSM-5沸石样品进行外表面修饰,制得两亲性沸石样品,该类两亲性沸石能分布于水、油两相界面处.改性后样品的红外光谱中末端硅羟基峰的强度明显降低,并出现CH3基团的C_H伸缩振动吸收峰,证实部分亲水性表面硅羟基被亲油性硅烷基团取代.这类两亲性样品在不加共溶剂及静置条件下,对环己烯水合相界面催化反应的催化活性远远高于改性前的HZSM-5沸石.由于该相界面反应是以孔道内为主的反应,三甲基氯硅烷经改性制备出的亲油性HZSM-5沸石也呈现出较高的活性.

【Abstract】 Amphiphilic HZSM-5 zeolite particles were prepared by a partial modification of the external surface of HZSM-5 zeolite with trimethylchlorosilane. These amphiphilic zeolite particles were oriented at the water-organic boundary when they were added to the mixture of cyclohexene and water or water with CCl4. IR spectra indicated that the intensity of the band for the terminal silanols decreased significantly and the band for the methyl groups(CH stretching vibration) emerged after modification, which gave a direct evidence that partial hydrophilic silanol groups on the surface of the zeolite were replaced by the hydrophobic alkylsilyl groups. This amphiphilic HZSM-5 zeolite exhibited a much higher catalytic activity than the parent HZSM-5 zeolite in the hydration of cyclohexene phase-boundary reaction without adding co-solvents and stirring. Because this phase-boundary reaction was proceeding through a channel-reaction mechanism, the hydrophobic HZSM-5 particles modified by trimethylchlorosilane also showed the better catalytic performance than the parent zeolite.

【基金】 国家自然科学基金青年基金(批准号:20203010);南京大学开放测试基金(批准号:0205001330)资助.
  • 【文献出处】 高等学校化学学报 ,Chemical Research In Chinese Universities , 编辑部邮箱 ,2005年04期
  • 【分类号】O643
  • 【被引频次】52
  • 【下载频次】477
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