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不同硅烷对HMS介孔分子筛甲基接枝的对比研究

Comparison study on the methyl-grafting modification of HMS mesoporous molecular sieve with different silanes

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【作者】 李学峰张立科高焕新陈庆龄

【Author】 LI Xue-feng1,ZHANG Li-ke1,GAO Huan-xin2,CHEN Qing-ling2(1.School of Chemistry and Chemical Engineering,Xuchang University,Xuchang,461000,China; 2.Shanghai Research Institute of Petrochemical Technology,Shanghai,201208,China)

【机构】 许昌学院化学化工学院中石化上海石油化工研究院

【摘要】 通过气相沉积法,分别用三甲基氯硅烷(TMCS)和六甲基二硅氮烷(HMDSZ)对HMS介孔分子筛表面进行甲基接枝改性;分别采用XRD、N2-吸附、FTIR2、9Si NMR和TG等手段对样品进行表征,并测定了样品的亲水性能。结果表明,两种硅烷都可以在HMS表面接枝,接枝后分子筛的介孔结构依然保持;但是,HMDSZ的接枝效果要明显优于TMCS,前者能接枝引入更多的甲基;拟定的接枝反应机理可以合理解释上述结果:Si-OH被TMCS直接氯化形成羟基硅烷和Si-Cl,羟基硅烷的挥发降低了TMCS的利用率,Si-Cl的水解(形成Si-OH)间接保留了HMS表面的硅羟基(Si-OH)。

【Abstract】 HMS mesoporous molecular sieve was methyl-grafted by the chemical vapor deposition(CVD) method using trimethylchlorosilane(TMCS) and hexamethyldisilazane(HMDSZ),respectively.The samples were characterized by XRD,N2-adsorpton,FTIR,29Si NMR and TG,respectively,and the hydrophilicity of samples was measured.The results show that the mesoporous characteristics of all samples are still kept after the methyl-grafting treatment using TMCS and HMDSZ while HMDSZ performs more effectively than TMCS because HMDSZ can graft more methyl-groups.The experiment results can be reasonably explained by the proposed grafting reaction mechanism.Si-OH was directly chlorinated by TMCS to form OH-containing silane and Si-Cl group.The volatilization of OH-containing silane decreased the grafting efficiency of TMCS and the hydrolysis of Si-Cl to form Si-OH indirectly retained the surface Si-OH of HMS.

【基金】 河南省科技攻关计划(重点项目)(092102210221)资助;省教育厅自然科学研究计划(2009B150025)资助
  • 【文献出处】 化学研究与应用 ,Chemical Research and Application , 编辑部邮箱 ,2011年02期
  • 【分类号】O643.36
  • 【被引频次】2
  • 【下载频次】178
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