Hierarchical Self-Assembly of a Biomimetic Diblock Copolypeptoid into Homochiral Superhelices
Hierarchical Self-Assembly of a Biomimetic Diblock Copolypeptoid into Homochiral Superhelices
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DOI：
10.1021/ja106340f
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发表时间：
2010-11-17
影响因子：
15
通讯作者：
Zuckermann, Ronald N.
中科院分区：
文献类型：
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作者：
Murnen, Hannah K.;Rosales, Adrianne M.;Zuckermann, Ronald N.
序列特异性仿生肽二嵌段共聚物的水性自组装成单分散超螺旋被证明是分层过程的结果，强烈依赖于分子的电荷水平。部分带电的两亲性二嵌段共聚肽 30 聚体，[N-(2-苯乙基)甘氨酸](15)-[N-(2-羧乙基)甘氨酸](15)，以高产率形成超螺旋，直径为 624 +/- 69 nm，长度为 2 至 20 μm。化学类似物与模型化合物的 X 射线散射和晶体学相结合已被用来开发自组装的分层模型。层状堆叠卷起形成超分子双螺旋结构，堆叠的内部排序由疏水嵌段内的结晶芳族侧链侧链相互作用介导。还研究了亲水嵌段中静电和氢键相互作用的作用，发现其在自组装过程中很重要。
The aqueous self-assembly of a sequence-specific bioinspired peptoid diblock copolymer into monodisperse superhelices is demonstrated to be the result of a hierarchical process, strongly dependent on the charging level of the molecule. The partially charged amphiphilic diblock copolypeptoid 30-mer, [N-(2-phenethyl)glycine](15)-[N-(2-carboxyethyl)glycine](15), forms superhelices in high yields, with diameters of 624 +/- 69 nm and lengths ranging from 2 to 20 mu m. Chemical analogs coupled with X-ray scattering and crystallography of a model compound have been used to develop a hierarchical model of self-assembly. Lamellar stacks roll up to form a supramolecular double helical structure with the internal ordering of the stacks being mediated by crystalline aromatic side chain-side chain interactions within the hydrophobic block. The role of electrostatic and hydrogen bonding interactions in the hydrophilic block is also investigated and found to be important in the self-assembly process.