Anisotropic, Degradable Polymer Assemblies Driven by a Rigid Hydrogen-Bonding Motif That Induce Shape-Specific Cell Responses

Anisotropic, Degradable Polymer Assemblies Driven by a Rigid Hydrogen-Bonding Motif That Induce Shape-Specific Cell Responses
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DOI:
10.1021/acs.macromol.1c01894
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发表时间:
2021-12-20
期刊:
影响因子:
5.5
通讯作者:
Tanaka, Masaru
Tanaka, Masaru
中科院分区:
化学1区
文献类型:
--
作者:
Fukushima, Kazuki;Matsuzaki, Kodai;Tanaka, Masaru

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聚乙二醇共轭两亲性嵌段共聚物含有通过刚性氢键键合基序(RHM)连接的可降解疏水性嵌段,可以以与疏水性嵌段的结晶性质无关的方式产生各向异性纳米组装体。全原子和粗粒分子动力学模拟表明,嵌段共聚物的各向异性排列可归因于 RHM 的 pi-pi 相互作用,而可结晶疏水嵌段有助于维持排列结构。聚合物组装体的光散射分析表明,含 RHM 的嵌段共聚物与无定形疏水嵌段形成非球形组装体;这表明 RHM 对嵌段共聚物的定向组装有很大贡献,这与结晶驱动的自组装不同。在存在纵横比大于12或长度大于310nm的各向异性聚合物组装体的情况下,在含有正常人成纤维细胞的细胞培养物中观察到增强的细胞增殖。
Poly(ethylene glycol)-conjugated amphiphilic block copolymers, which contain degradable hydrophobic blocks connected by a rigid hydrogen-bonding motif (RHM), are developed to yield anisotropic nanoassemblies in a manner independent of the crystalline nature of the hydrophobic block. The all-atom and coarse-grained molecular dynamics simulations suggest that the anisotropic alignment of the block copolymers can be attributed to the pi-pi interactions of the RHM and the crystallizable hydrophobic blocks help maintain the aligned structure. Light scattering analysis of the polymer assemblies demonstrates the formation of nonspherical assemblies by the RHM-containing block copolymers with an amorphous hydrophobic block; this indicates the strong contribution of the RHM to the directed assembly of the block copolymers, unlike crystallization-driven self-assembly. Enhanced cell proliferation is observed in cell cultures containing normal human fibroblasts in the presence of the anisotropic polymer assemblies with aspect ratios greater than 12 or lengths greater than 310 nm.