物理化学学报 >> 2005, Vol. 21 >> Issue (02): 146-150.doi: 10.3866/PKU.WHXB20050207

研究论文 上一篇    下一篇

四甲基锡在MCM-41分子筛表面的接枝反应及产物性能

郑瑛;王绪绪;付贤智;魏可镁   

  1. 福州大学化肥催化剂国家工程研究中心,福州 350002;福建师范大学化学与材料学院,福州 350007
  • 收稿日期:2004-07-09 修回日期:2004-09-01 发布日期:2005-02-15
  • 通讯作者: 王绪绪 E-mail:xwang@fzu.edu.cn

Grafting Reaction of SnMe4 on MCM-41 Mesoporous Molecular Sieves Surface

ZHENG Ying;WANG Xu-Xu;FU Xian-Zhi;WEI Ke-Mei   

  1. National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002; College of Chemistry and Materials Science, Fujian Normal University, Fuzhou 350007
  • Received:2004-07-09 Revised:2004-09-01 Published:2005-02-15
  • Contact: WANG Xu-Xu E-mail:xwang@fzu.edu.cn

摘要: 研究了真空条件下SnMe4在MCM-41分子筛表面的接枝反应,并用元素分析、ICP、GC-MS、XRD、FTIR、DRS、13C及119Sn MAS NMR、XPS、BET、TPD、TPR等方法对产物的组成、结构和性质进行了表征.结果表明, 两者可以定量地进行化学反应,将确定数目的甲基锡基团接枝在分子筛表面, 形成SnMe3/MCM-41物种;接枝反应发生在分子筛表面上, 不破坏MCM-41分子筛骨架结构;改性分子筛的BET比表面积有所降低,孔体积变小, 表面性质发生变化.四甲基锡在MCM-41上接枝反应的温度为343 K,比它与HY沸石的反应温度(193 K)高得多,并且产物SnMe3/MCM-41的热稳定性也高于SnMe3/HY.

关键词: 表面金属有机化学, 四甲基锡, MCM-41, 接枝反应

Abstract: The reaction of MCM-41 with tetramethyl tin was studied under high vacuum condition, and the composition, structure and properties of the resulted solid were characterized by element analysis, gas volumetry analysis, ICP, XRD, FTIR, DRS(diffuse reflectance spectroscopy), 13C and 119Sn MAS NMR, XPS, BET,TPD, TPR, adsorption of nitrogen etc., respectively. The results showed that the reaction occurred on the surface without destroying the framework structure of the zeolite, leading to the formation of the monografted species (≡Si-O)SnMe3 for MCM-41 at 773 K. Grafting methyltin species on the surface resulted in decrease of the pore size and the mesoporous volume of MCM-41. The reaction temperature of MCM-41 with tetramethyl tin was 343 K which is higher than that of HY zeolite with tetramethyl tin (193 K) and SnMe3/MCM-41 is thermal stable under 673 K and its thermal stability is higher than that of SnMe3/HY.

Key words: Surface organometallic chemistry, Tetramethyl tin, MCM-41, Grafting reaction