Overcoming the Necessity of a Lateral Aggregation in the Formation of Supramolecular Polymer Bottlebrushes in Water,Macromolecular Rapid Communications

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Overcoming the Necessity of a Lateral Aggregation in the Formation of Supramolecular Polymer Bottlebrushes in Water
Macromolecular Rapid Communications ( IF 4.2 ) Pub Date : 2020-12-04 , DOI: 10.1002/marc.202000585
Tobias Klein _{1,

2} , Hans F Ulrich _{1,

2} , Franka V Gruschwitz _{1,

2} , Maren T Kuchenbrod _{1,

2} , Rintaro Takahashi ₃ , Stephanie Hoeppener _{1,

2} , Ivo Nischang _{1,

2} , Kazuo Sakurai ₃ , Johannes C Brendel _{1,

2}

Affiliation

The assembly of supramolecular polymer bottlebrushes in aqueous systems is, in most cases, associated with a lateral aggregation of the supramolecular building blocks in addition to their axial stacking. Here, it is demonstrated that this limitation can be overcome by attaching three polymer chains to a central supramolecular unit that possesses a sufficiently high number of hydrogen bonding units to compensate for the increased steric strain. Therefore, a 1,3,5‐benzenetrisurea‐polyethylene oxide conjugate is modified with different peptide units located next to the urea groups which should facilitate self‐assembly in water. For a single amino acid per arm, spherical micelles are obtained for all three tested amino acids (alanine, leucine, and phenylalanine) featuring different hydrophobicities. Only a slight increase in size and solution stability of spherical micelles is observed with increasing hydrophobicity of amino acid unit. In contrast, introducing two amino acid units per arm and thus increasing the number of hydrogen bonds per unimer molecule results in the formation of cylindrical structures, that is, supramolecular polymer bottlebrushes, despite a suppressed lateral aggregation. Consequently, it can be concluded that the number of hydrogen bonds has a more profound impact on the resulting solution morphology than the hydrophobicity of the amino acid unit.

中文翻译：

克服水中超分子聚合物牙刷形成过程中横向聚集的必要性

在大多数情况下，水性系统中的超分子聚合物牙刷的组装除轴向堆叠外，还与超分子构件的侧向聚集有关。在此证明，可以通过将三个聚合物链连接到一个中心超分子单元上来克服这一限制，该中心超分子单元具有足够高数量的氢键合单元以补偿增加的空间应变。因此，用位于尿素基团旁边的不同肽单元修饰了1,3,5-苯三氮杂-聚环氧乙烷共轭物，这应有助于在水中自组装。对于每臂一个氨基酸，针对具有不同疏水性的所有三个测试氨基酸（丙氨酸，亮氨酸和苯丙氨酸）获得球形胶束。随着氨基酸单位疏水性的增加，球形胶束的尺寸和溶液稳定性仅略有增加。相反，尽管抑制了横向聚集，但是每臂引入两个氨基酸单元并因此增加每个单聚体分子的氢键数目导致形成圆柱结构，即超分子聚合物刷。因此，可以得出结论，与氨基酸单元的疏水性相比，氢键的数目对所得溶液的形态具有更深远的影响。尽管抑制了横向聚集，但仍使用超分子聚合物牙刷。因此，可以得出结论，与氨基酸单元的疏水性相比，氢键的数目对所得溶液的形态具有更深远的影响。尽管抑制了横向聚集，但仍使用超分子聚合物牙刷。因此，可以得出结论，与氨基酸单元的疏水性相比，氢键的数目对所得溶液的形态具有更深远的影响。

更新日期：2020-12-04

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