Multifunctional Vesicles from a Self-assembled Cluster-Containing Diblock Copolymer,Journal of the American Chemical Society

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Multifunctional Vesicles from a Self-assembled Cluster-Containing Diblock Copolymer
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-04-12 , DOI: 10.1021/jacs.8b02041
Anastasia Voevodin ₁ , Luis M. Campos ₁ , Xavier Roy ₁

Affiliation

We describe a new diblock copolymer composed of two segments with complementary functionalities. One block contains pendent photo-cross-linkable cinnamoyl groups, and the other contains molecular clusters, Co6Se8, capable of multielectron redox processes. This multifunctional macromolecule is synthesized by sequential ring-opening metathesis polymerization of monomers constructed using norbornene moieties. Remarkably, the tethered molecular cluster gives access to three different charge states in N, N-dimethylformamide: neutral, +1, and +2. In tetrahydrofuran, by contrast, the charged copolymer self-assembles into vesicles that inhibit the redox reactions. The wall of these vesicles can be cross-linked by exploiting the photoinduced 2 + 2 cycloaddition of the cinnamoyls to form cyclobutane dimers. Moreover, these vesicles can be loaded with molecular cargo and used as cross-linkable containers; we demonstrate this feature by encapsulating the molecular dye methylene blue into the capsules. Our work is the first report of a well-defined block copolymer containing a metal chalcogenide molecular cluster; more generally, it opens the door to new applications of metal-containing polymers.

中文翻译：

自组装含簇二嵌段共聚物的多功能囊泡

我们描述了一种由具有互补功能的两个链段组成的新型二嵌段共聚物。一个块包含悬垂的可光交联肉桂酰基，另一个包含分子簇 Co6Se8，能够进行多电子氧化还原过程。这种多功能大分子是通过使用降冰片烯部分构建的单体的顺序开环复分解聚合合成的。值得注意的是，系留分子簇可以访问 N, N-二甲基甲酰胺中的三种不同电荷状态：中性、+1 和 +2。相比之下，在四氢呋喃中，带电共聚物会自组装成抑制氧化还原反应的囊泡。这些囊泡的壁可以通过利用肉桂酰基的光诱导 2 + 2 环加成形成环丁烷二聚体来交联。而且，这些囊泡可以装载分子货物并用作可交联的容器；我们通过将分子染料亚甲蓝封装到胶囊中来证明这一特性。我们的工作是第一份关于包含金属硫属化物分子簇的明确定义的嵌段共聚物的报告；更一般地说，它为含金属聚合物的新应用打开了大门。

更新日期：2018-04-12

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