用于选择性硅氢加成反应的可磁分离高性能铂催化剂
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- 英文论文题名：High efficient and magnetic Pt catalysts for hydrosilylation reactions
- 论文作者：赵建波 ; 孙雨安 ; 王国庆 ; 刘应凡
- 英文论文作者：Jianbo Zhao ; Yu'an Sun ; Guoqing Wang ; Yingfan Liu ; School of Material & Chemistry Engieering ; Zhengzhou University of Light Industry
- 年：2016
- 作者机构：郑州轻工业学院;
- 论文关键词：硅氢加成 ; 铂催化剂 ; 磁性分离
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第十五分会：表界面结构调控与催化
- 语种：中文
- 分类号：O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十五分会 ; 表界面结构调控与催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：300k
- 原文格式：D
- 会议级别：全国
摘要
选择性硅氢加成反应是合成功能性有机硅化合物和有机硅偶联剂的最重要途径。工业上,该类反应大多在氯铂酸等均相催化剂下作用完成。尽管该催化体系具有催化活性高、反应条件温和等优点,但存在一些缺陷,例如,贵金属铂催化剂与产物溶液分离困难,难以循环利用等[1]。由于贵金属资源的稀缺性、不可替代性和不可再生性,实现贵金属的节约和高效利用,是有机硅工业领域必须解决的关键问题。本文以Fe_3O_4@SiO_2磁性核壳结构为载体,对其表面用3-氨丙基三乙氧基硅烷(APTS)修饰,再与氯铂酸配位,制得多相催化剂Fe_3O_4@SiO_2-APTS-Pt。该催化剂在三乙氧基硅烷和1-辛烯的硅氢加成反应中显示出极佳的性能,且比经典Speier’s催化剂的活性更高。60℃时,Pt的摩尔量仅为底物的0.00067%,三乙氧基硅烷的转化率可达98%,β-加成反应选择性99%以上。Fe_3O_4@SiO_2-APTS-Pt通过外磁场与反应液分离,且重复使用三次时其活性没有明显的下降。结合XPS、FT-IR和TEM等表征结果,Fe_3O_4@SiO_2-APTS-Pt的优异性能与其结构相关(如Pt与N的配位等)。
Generally,hydrosilylation is homogeneously catalyzed which means that after completion of the reaction the catalyst either remains within the product or has to be expensively removed.Fe_3O_4@SiO_2-APTS-Pt complex was prepared and then characterized by TEM,XPS,FT-IR and ICP-AES,respectively.The catalyst exhibited excellent catalytic activity and remarkable regioselectivity in the hydrosilylation reaction of 1-octene with triethoxysilane.The conversion of triethoxysilane is 98%,while the regioselectivity for the β-addition product achieves above 99% under mild reaction conditions.It can be recovered by external magnetic field and can be used for three times with no significant loss of activity.Its excellent performances are related to the structure of the catalyst.
Generally,hydrosilylation is homogeneously catalyzed which means that after completion of the reaction the catalyst either remains within the product or has to be expensively removed.Fe_3O_4@SiO_2-APTS-Pt complex was prepared and then characterized by TEM,XPS,FT-IR and ICP-AES,respectively.The catalyst exhibited excellent catalytic activity and remarkable regioselectivity in the hydrosilylation reaction of 1-octene with triethoxysilane.The conversion of triethoxysilane is 98%,while the regioselectivity for the β-addition product achieves above 99% under mild reaction conditions.It can be recovered by external magnetic field and can be used for three times with no significant loss of activity.Its excellent performances are related to the structure of the catalyst.
引文
[1]Zhao,J;Xie,B;Wang,G;Song,S;Sun,Y.REACT KINET CATAL L 2009,96:101-108.