Pt/介孔SiO_(2)催化剂上烯丙基聚氧乙烯烷基醚的硅氢加成反应  

Hydrosilylation of polyoxyethylene alkyl allyl ethers over Pt/Meso-SiO_(2) catalyst

作　　者：刘其海[1,2,3] 谢婉婷 贾振宇 朱小花[2] 王荣辉 Liu Qihai;Xie Wanting;Jia Zhenyu;Zhu Xiaohua;Wang Ronghui(College of Chemistry and Chemical Engineering,Zhongkai University of Agriculture and Engineering, Guangzhou 510225,Guangdong,China;Zhanjiang Botai Bio-Chemical Technology Industrial Co. , Ltd. , Zhanjiang 524051,Guangdong,China;Guangdong Weiqian Technology Co., Ltd., Foshan 528216,Guangdong,China)

机构地区：[1]仲恺农业工程学院化学化工学院,广东广州510225 [2]湛江博泰生物化工科技实业有限公司,广东湛江524051 [3]广东维芊科技有限公司,广东佛山528216

出　　处：《工业催化》2021年第6期35-39,共5页Industrial Catalysis

基　　金：广东省省级科技计划项目(2016A010105022,2017A010103024,2020B121202014);广东省促进经济发展专项资金(粤自然资源合[2019]016号);湛江市海洋经济创新发展示范市建设项目(湛海创2017C4A);湛江市科技发展专项资金竞争性分配项目(2016A02010);佛山市科技创新项目(2019,FS0AA-KJ919-4402-0057)。

摘　　要：以十二烷基胺为结构导向剂,正硅酸乙酯为硅源制备了介孔SiO_(2)(Meso-SiO_(2)),并在制备Meso-SiO_(2)过程中加入氯铂酸,制备了Pt负载量为(8.5~22.1)×10^(-6)的Pt/Meso-SiO_(2)催化剂。考察了Pt/Meso-SiO_(2)催化剂对七甲基三硅氧烷(MDHM)和烯丙基聚氧乙烯烷基烯丙基醚(HDE)的硅氢加成反应的催化性能。采用傅里叶变换光谱学(IR)、X射线小角衍射(XRD)、紫外-可见光谱(UV-Vis)和电子显微镜(SEM)对催化剂进行了表征。结果显示,在Pt负载量为17.2×10^(-6)的催化剂上,HDE∶MDHM物质的量比为1∶1时,可获得高达93.7%的MDHM转化率。催化剂重复试验结果显示,催化剂重复使用7次,催化活性无明显下降,可推断Pt活性粒子在介孔SiO_(2)载体的分散性是稳定的,这可能归因于TEOS水解过程中,Pt粒子被硅-氧-硅骨架嵌入,从而使其维持良好的催化稳定性。Mesoporous SiO_(2)(Meso-SiO_(2))were synthesized by the method of one pot hydrolysis of tetrathoxysilane(TEOS)using dodecyl amine(DDA)as structure-directing agent.Catalysts(Pt/Meso-SiO_(2))with Pt loading of(8.5-22.1)×10^(-6) were prepared by adding chloroplatinic acid during preparing of Meso-SiO_(2).The catalytic performance of the Pt/Meso-SiO_(2) catalysts for hydrosilylation of heptamethyltrisiloxane(MDHM)and polyoxyethylene alkyl allyl ethers(HDE)were investigated.The catalysts were characterized by Fourier transform infrared spectroscopy(IR),X-ray small angle diffraction(XRD),ultraviolet-visible spectroscopy(UV-Vis)and electron microscopy(SEM).Results show that when n(HDE)∶n(MDHM)=1∶1,as high as 93.7%of MDHM conversion can be achieved over catalyst(16Pt/Meso-SiO_(2))with Pt loading of 17.2×10^(-6).The catalyst could be reused at least seven times without obvious catalytic activity decrease.The performance of the catalysts may attribute to the well dispersion of Pt particles over the surface of Meso-SiO_(2).Additionally,Pt particles were inlayed and embedded by the skeleton of Si—O—Si in the process of TEOS hydrolysis,which played an important role in maintaining the catalytic stability.

关 键 词：催化化学 介孔SiO_(2) PT催化剂 硅氢加成 七甲基三硅氧烷 聚氧乙烯烷基烯丙基醚 

分 类 号：O643.36[理学—物理化学] TQ426.6[理学—化学]