Sn掺杂MCM-41介孔分子筛的制备、表征及催化性能研究

doi:10.3724/SP.J.1077.2010.01041

无机材料学报 ›› 2010, Vol. 25 ›› Issue (10): 1041-1046.DOI: 10.3724/SP.J.1077.2010.01041 CSTR: 32189.14.SP.J.1077.2010.01041

Sn掺杂MCM-41介孔分子筛的制备、表征及催化性能研究

李圭, 钟玲, 袁霞, 吴剑, 罗和安

(湘潭大学化工学院, 湘潭 411105)

收稿日期:2010-02-04 修回日期:2010-04-07 出版日期:2010-10-20 网络出版日期:2010-09-26
基金资助:
国家自然科学基金和中国石油化工股份有限公司联合资助重点项目(20736009); 湖南省教育厅优秀青年基金(06B093)

Preparation, Characterization and Catalytic Properties of Sn-Containing MCM-41

LI Gui, ZHONG Ling, YUAN Xia, WU Jian, LUO He-An

(School of Chemical Engineering, Xiangtan University, Xiangtan 411105, China)

Received:2010-02-04 Revised:2010-04-07 Published:2010-10-20 Online:2010-09-26
Supported by:
National Nature Science Foundation of China and Sinopec (20736009); Scientific Research Fund of Hunan Provincial Education Department (06B093)

摘要/Abstract

摘要： 在低模板剂浓度和弱碱介质中合成催化材料Si-MCM-41、Sn-MCM-41, 并用XRD、N₂物理吸附-脱附、FT-IR、ICP-AES和TEM等手段对催化材料进行了表征. 研究了合成方法对制备Sn掺杂MCM-41介孔分子筛的影响, 结果表明: 水热晶化法(DHT)合成的Sn-MCM-41, Sn物种主要进入分子筛的骨架中; 而模板离子交换法(TIE)合成的Sn-MCM-41, Sn物种主要位于分子筛的表面. Sn-MCM-41介孔分子筛催化环己酮Baeyer-Villiger氧化反应结果表明, n(H₂O₂):n(酮)＝3:1, 30g1,4-二氧六环为溶剂, H₂O₂为氧源, 70℃反应6 h, 环己酮的转化率可达40.02%, ε-己内酯的选择性为45.69%.

关键词: 水热晶化, 模板离子交换, Si-MCM-41, Sn-MCM-41, Baeyer-Villiger氧化

Abstract: The molecular sieve catalysis material of Si-MCM-41, Sn-MCM-41 were preparaed under the condition of low template concentration in weak base and the samples were characterized by XRD, N₂ adsorption-desorption, FT-IR, ICP-AES and TEM techniques. Effect of the synthesis methods on the Sn-containing MCM-41 were studied. The results showed that Sn species were mainly incorporated into the framework of MCM-41 molecular sieves prepared by direct hydrothermal synthesis method (DHT), while Sn species were mainly existed on the wall surface of Sn-MCM-41 molecular sieves prepared by template-ion exchange method (TIE). The catalytic properties of Sn containing MCM-41 molecular sieves in Baeyer-Villiger oxidation of cyclohexanone were investigated. Catalytic activity results show that under the reaction condition of n(H₂O₂):n(Cyclohexanone)＝3:1, 30 g dioxane, at 70℃ for 6 h, the conversion of cyclohexanone and the selectivity of ε-caprolactone reach 40.02% and 45.69%, respectively.

Key words: direct hydrothermal synthesis, template-ion exchange, Si-MCM-41, Sn-MCM-41, Baeyer-Villiger oxidation

中图分类号:

O643

李圭, 钟玲, 袁霞, 吴剑, 罗和安. Sn掺杂MCM-41介孔分子筛的制备、表征及催化性能研究[J]. 无机材料学报, 2010, 25(10): 1041-1046.

LI Gui, ZHONG Ling, YUAN Xia, WU Jian, LUO He-An. Preparation, Characterization and Catalytic Properties of Sn-Containing MCM-41[J]. Journal of Inorganic Materials, 2010, 25(10): 1041-1046.

参考文献

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Sn掺杂MCM-41介孔分子筛的制备、表征及催化性能研究

Preparation, Characterization and Catalytic Properties of Sn-Containing MCM-41

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