Sequence and entropy-based control of complex coacervates.
Sequence and entropy-based control of complex coacervates.
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DOI：
10.1038/s41467-017-01249-1
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发表时间：
2017-11-02
影响因子：
16.6
通讯作者：
Perry SL
中科院分区：
文献类型：
--
作者：
Chang LW;Lytle TK;Radhakrishna M;Madinya JJ;Vélez J;Sing CE;Perry SL
生物大分子依赖于单体的精确定位来编码结构、功能和生理信息。通过合成控制聚合物中的化学序列来模拟这种复杂性的努力正在取得成功；然而，对于如何将单体序列转化为物理材料性质的理解很少。在这里，我们建立了在被称为复杂凝聚体的材料中实现这种顺序控制的设计规则。这些材料是由相反带电的聚电解质形成的缔合相分离成聚电解质稠密(凝聚)和聚电解质稀释(上清液)相。我们证明，电荷模式可以深刻地影响驱动这一过程的电荷-电荷关联。此外，我们建立了这种依赖于图案的相互作用的物理起源：在致密凝聚相中存在结构变化的微妙组合，以及由于上清相中沿聚合物的图案而产生的反离子的一维限制。单体序列是一种新兴的工具，可以将信息(从而结构和功能)精确编码到聚合物系统中。在这里，作者使用复杂凝聚体中的序列控制来理解单体序列如何转化为物理材料属性。
Biomacromolecules rely on the precise placement of monomers to encode information for structure, function, and physiology. Efforts to emulate this complexity via the synthetic control of chemical sequence in polymers are finding success; however, there is little understanding of how to translate monomer sequence to physical material properties. Here we establish design rules for implementing this sequence-control in materials known as complex coacervates. These materials are formed by the associative phase separation of oppositely charged polyelectrolytes into polyelectrolyte dense (coacervate) and polyelectrolyte dilute (supernatant) phases. We demonstrate that patterns of charges can profoundly affect the charge–charge associations that drive this process. Furthermore, we establish the physical origin of this pattern-dependent interaction: there is a nuanced combination of structural changes in the dense coacervate phase and a 1D confinement of counterions due to patterns along polymers in the supernatant phase. Monomer sequence is an emerging tool to precisely encode information (and thus structure and function) into polymer systems. Here the authors use sequence-control in complex coacervates to understand how monomer sequence translates to physical material properties.
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