炭载铂配位化合物结构对催化烯烃硅氢加成性能的影响  

Effect of carbon loaded platinum coordination compounds structure on catalytic performance of hydrosilylation of alkenes

作　　者：朱锦华 张仕鹏 谢小艳 王榕[1,2] ZHU Jinhua;ZHANG Shipeng;XIE Xiaoyan;WANG Rong(School of Chemistry and Chemical Engineering,Nanchang University,Nanchang 330031,China;Key Laboratory of Poyang Lake Environment and Resource Utilization,Ministry of Education,Nanchang University,Nanchang 330031,China)

机构地区：[1]南昌大学化学化工学院,江西南昌330031 [2]南昌大学鄱阳湖环境与资源利用教育部重点实验室,江西南昌330031

出　　处：《南昌大学学报(工科版)》2025年第1期14-24,共11页Journal of Nanchang University(Engineering & Technology)

基　　金：国家自然科学基金资助项目(21968018)。

摘　　要：为弄清催化剂表面金属活性组分的存在形态与结构对催化端位烯烃与叔硅烷的硅氢加成反应性能的影响,使用氧化处理的水稻秸秆活性炭(RSOC)为载体,分别引入乙烯基三乙氧基硅烷和氨丙基三乙氧基硅烷作为配体化合物,进而分别获得水稻秸秆活性炭负载的铂乙烯基配位催化剂(Pt-VTES-RSOC)与铂氨基配位催化剂(Pt-ATES-RSOC)。基于2种催化剂的表征结果及其催化1-辛烯与三乙氧基硅烷的性能差异和Chalk-Harrod机理,分别构筑了Pt-VTES-RSOC与Pt-ATES-RSOC的结构模型及催化1-辛烯与三乙氧基硅烷的反应模型,使用理论计算在结构优化基础上对催化机理进行对比研究,深入了解活性组分存在形态与结构对催化性能的影响。To understand the influence of the morphology and structure of the metal active components on catalyst surface on the catalytic performance of hydrosilylation of terminal alkenes with tertiary silanes, oxidized carbon derived from waste rice straw was used as the support, vinyl triethoxysilane and aminopropyl triethoxysilane were introduced as ligand compounds to acquire oxidized carbon with Pt(Ⅱ)-vinyl complex(Pt-VTES-RSOC) and Pt(Ⅱ)-amino complex(Pt-ATES-RSOC), respectively. Based on characterization results of the two catalysts and their difference in catalytic performance for hydrosilylation of 1-octene and triethoxysilane(TES), as well as the Chalk Harrod mechanism, the structural models of Pt-VTES-RSOC and Pt-ATES-RSOC and the catalytic reaction model of 1-octene and TES were reasonably constructed. And a comprehensive understanding of the influence of morphology and structure of active components on catalytic performance could be gained by comparing the difference in catalytic mechanisms of two catalyst with different coordinate structures.

关 键 词：硅氢加成 多相催化 配位结构 密度泛函理论 催化机理 

分 类 号：O643.3[理学—物理化学]