化学学报 ›› 2004, Vol. 62 ›› Issue (5): 449-453.    下一篇

研究论文

表面金属有机化学:SnMe4在HY沸石超笼表面的接枝反应

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
  • 投稿日期:2003-08-08 修回日期:2003-11-05 发布日期:2014-02-18
  • 通讯作者: 王绪绪,E-mail:xwang@fzu.edu.cn E-mail:xwang@fzu.edu.cn
  • 基金资助:
    国家自然科学基金(No.20173009)和福建省自然科学基金(No.E0210008)资助项目.

Surface Organometallic Chemistry:Grafting Reaction of SnMe4 on HY Zeolite Supercage 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
  • Received:2003-08-08 Revised:2003-11-05 Published:2014-02-18

研究了高真空条件下SnMe4在HY沸石超笼的接枝反应,并用元素分析,ICP, GC, XRD, FTIR, DTG, DTA, UV-vis, DRS, N2吸附等方法对产物的组成、结构和性质进行了详细表征.研究结果表明,两者可以定量地、有选择性地进行化学反应,将确定数目的三甲基锡基团接枝在沸石的超笼中.反应可以在非常低的温度下快速进行,表观活化能为10.4 kJ·mol-1.经SnMe4改性后的HY沸石分子筛BET比表面积降低,孔体积变小,对不同尺寸的烃分子表现出明显的吸附择形性.

关键词: 表面金属有机化学, 四甲基锡, Y沸石, 接枝

The grafting reaction of SnMe4 onto the supercages of HY zeolite was studied under high vacuum conditionand the chemical composition and structure of resulting solid were characterized by in situ FT-IR,XRD,UV-Vis,DRS,DTG,DTA,N2 adsorption,ICP,elemental analysis,and gas chromatography.The reaction could occur rapidly and quantitatively at low temperature down to 188 K(apparent active energy was 1014 kJ·mol-1),resulting in the grafting of well-defined—Sn(CH3)3 fragments onto the surface of zeolite supercages.The grafted Y zeolite is quite different from the starting HY zeolite in adsorption properties,and showed obvious size-selectivity for hydrocarbons.

Key words: surface organometallic chemistry, tetramethyltin, Y zeolite, grafting reaction