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周期有序双连续介孔结构Pd (II)有机金属催化剂用于水介质Sonogashira反应的研究
杨迪迪, 朱凤霞, 李和兴, 张 昉
上海师范大学
摘要:
以1,4-双(三乙氧基硅基)苯和苯基膦钯有机金属硅烷为混合硅源,在表面活性剂导向组装下共缩聚制得Pd(Ⅱ)-PMO-KIT-6非均相催化剂,并利用NMR、XPS、XRD、TEM和氮气吸附等手段对催化剂进行了表征.考察了该催化剂在水介质Sonogashira反应中的催化性能,结果表明:所制备的Pd(Ⅱ)-PMO-KIT-6具有优异的催化活性和选择性,这主要归因于催化剂的高比表面积、双连续介孔结构有利于提高Pd(Ⅱ)活性位分散度,减少传质阻力;同时苯基桥联PMO构建形成的微环境增强表面疏水性,有利于反应底物的吸附和扩散.此外,催化剂还可以重复使用多次后活性没有明显降低.
关键词:  非均相催化  双连续介孔结构  有机金属固载化  水介质清洁有机合成
DOI:
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基金项目:
Preparation of recyclable Pd(Ⅱ) organometal catalyst with bicontinuous cubic Ia3d mesostructure for water-medium organic reaction
YANG Didi, ZHU Fengxia, LI Hexing, ZHANG Fang
College of Life and Environment Sciences,Shanghai Normal University
Abstract:
A heterogenous Pd(Ⅱ) organometal catalyst with bicontinuous cubic Ia3d mesostructure was synthesized by surfactant-directed co-condensation of Pd[PPh2(CH2)2Si(OCH2CH3)32Cl2 and (CH3CH2O)3SiPhSi(OCH2CH3)3.In water-medium Sonogashira reaction,the as-prepared Pd(Ⅱ)-PMO-KIT-6 exhibited higher catalytic activity than reference catalyst Pd(Ⅱ)-KIT-6 and could be used repetitively for more than 4 times,which could reduce the cost and even diminish the environmental pollution from heavy metallic ions,showing a good potential in industrial applications.
Key words:  recyclable catalyst  I mmobilization of Pd(Ⅱ) organometal  bicontinuous cubic mesostructure  water-medium organic reactions