Control over Conformational Landscapes of Polypeptoids by Monomer Sequence Patterning

Control over Conformational Landscapes of Polypeptoids by Monomer Sequence Patterning
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通过单体序列图案控制多肽的构象景观

DOI:
10.1021/acs.macromol.3c02338
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发表时间:
2024
期刊:
影响因子:
5.5
通讯作者:
Segalman, Rachel A.
Segalman, Rachel A.
中科院分区:
化学1区
文献类型:
--
作者:
DeStefano, Audra J.;Mengel, Shawn D.;Bates, Morgan W.;Jiao, Sally;Shell, M. Scott;Han, Songi;Segalman, Rachel A.

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通过控制合成聚合物的单体序列来编程链构象和结构的能力对于下一代材料设计具有广泛的意义。虽然蛋白质折叠和设计的相关问题已经产生了三维(3D)折叠链结构的准确预测,但由于需要大型结构数据库和聚合物构建块的内在无序性质,合成聚合物的推广仍然很难。在这项工作中,拟多肽,一类拟肽合成聚合物,被用来建立一个通用的工作流程,在溶液中的单体序列和动态三维链结构之间的关系的研究。这项工作演示了如何控制单体序列可以改变合成聚合物的构象景观显着偏离经典的链统计。具体而言,端到端的距离的分布,如通过双电子-电子共振光谱法在稀溶剂中测量的,系统地偏向于较短的距离与疏水物的数量的增加,并进一步细化疏水物的安排在两亲性类多肽链。
The ability to program chain conformation and structure through control over the monomer sequence of synthetic polymers has broad implications for next-generation material design. While related problems of protein folding andde novodesign have generated accurate predictions of three-dimensional (3D) folded chain structures, generalization to synthetic polymers remains intractable due to the requirement of large structural databases and the intrinsically disordered nature of polymer building blocks. In this work, polypeptoids, a class of peptidomimetic synthetic polymers, are utilized to build a general workflow for the study of relationships between the monomer sequence and dynamic 3D chain structure in solution. This work demonstrates how control over the monomer sequence can alter the conformational landscape of synthetic polymers to deviate dramatically from classical chain statistics. Specifically, the distribution of end-to-end distances, as measured by double electron–electron resonance spectroscopy in dilute solvent, is systematically skewed toward shorter distances with an increasing number of hydrophobes and further refined by hydrophobe arrangement in amphiphilic polypeptoid chains.
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