Gradient Copolymer Prepared from Alternating Ring-Opening Metathesis of Three Monomers.
Gradient Copolymer Prepared from Alternating Ring-Opening Metathesis of Three Monomers.
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DOI：
10.1039/d1py00690h
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发表时间：
2021-10-21
影响因子：
4.6
通讯作者：
中科院分区：
文献类型：
--
作者：
双环[4.2.0]辛-6-烯-7-甲酰胺是一种结构简单但高度紧张的烯烃单体，在N-杂环卡宾-钌催化剂存在下与环己烯形成交替共聚物。与催化剂的钌中心螯合的在C7上具有庞大取代基的[4.2.0]部分比不能螯合的单体增长更慢。因此，N-丙基双环[4.2.0]辛-6-烯-7-甲酰胺与环己烯的竞聚率显著高于N-（2-（2-乙氧基乙氧基）乙烷）-双环[4.2.0]辛-6-烯-7-甲酰胺与环己烯的竞聚率。三种单体以1：1：2（丙基：乙二醇：环己烯）的摩尔比共聚，在一锅反应中形成梯度共聚物。梯度共聚物的表面疏水性、拓扑结构和热性质类似于通过在每个微嵌段中交替使用相同的两个双环[4.2.0]辛-6-烯-7-甲酰胺通过多步合成制备的由六个微嵌段组成的共聚物。梯度共聚物的性质不同于由基于相同双环[4.2.0]辛-6-烯-7-甲酰胺的两个较大嵌段组成的共聚物。
Bicyclo[4.2.0]oct-6-ene-7-carboxamide is a simple but highly strained olefin monomer which forms an alternating copolymer with cyclohexene in the presence of N-heterocyclic carbene-ruthenium catalyst. [4.2.0] moiety with bulky substituent on C7 that chelate with the ruthenium center of the catalyst propagate more slowly than monomers that cannot chelate. Accordingly, the reactivity ratio of N-propylbicyclo[4.2.0]oct-6-ene-7-carboxamide with cyclohexene is significantly higher than that of N-(2-(2-ethoxyethoxy)ethan)-bicyclo[4.2.0]oct-6-ene-7-carboxamide with cyclohexene. A copolymerization involving the three monomers in a 1:1:2 (propyl:ethylene glycol:cyclohexene) molar ratio formed a gradient copolymer in a one-pot reaction. Surface hydrophobicity, topology, and thermal properties of the gradient copolymer were similar to those of a copolymer comprised of six microblocks prepared through multistep synthesis by alternately employing the same two bicyclo[4.2.0]oct-6-ene-7-carboxamides in each microblock. The properties of the gradient copolymer were distinct from a copolymer comprised of two larger blocks based on the same bicyclo[4.2.0]oct-6-ene-7-carboxamides.
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