Molecular crystallization directed by polymer size and overlap under dilute and crowded macromolecular conditions

Molecular crystallization directed by polymer size and overlap under dilute and crowded macromolecular conditions
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DOI:
10.1038/s41428-021-00461-7
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发表时间:
2021-02-08
期刊:
影响因子:
2.8
通讯作者:
Sakai, Takamasa
Sakai, Takamasa
中科院分区:
化学3区
文献类型:
--
作者:
Hata, Yuuki;Li, Xiang;Sakai, Takamasa

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溶解聚合物在稀相和拥挤相条件下指导分子结晶行为。较大的聚乙二醇(PEG)加速咖啡因晶体的形成在稀释制度的PEG溶液中,这是由于耗尽吸引力,促进咖啡因簇聚集成晶核。在半稀释状态下,晶体形成速率对PEG的分子量不敏感。这一观察结果是一致的聚合物滴的属性,其中管理耗尽吸引力,并保持在一个给定的聚合物浓度恒定的大小,无论分子量在semidilute regiment.We表明,溶解的聚合物可以直接在稀释和拥挤的条件下的分子结晶行为。较大的聚乙二醇(PEG)加速咖啡因晶体的形成在稀释制度的PEG溶液中,这是由于耗尽吸引力,促进咖啡因簇聚集成晶核。或者,在半稀释方案中,咖啡因晶体形成速率对PEG的分子量(MW)不敏感。具有各种MW的PEG似乎诱导耗尽吸引力的程度类似的性质的聚合物溶液中的半稀释液的制度所描述的斑点,这是恒定的大小,在给定的聚合物浓度,无论MW。这项研究突出了体外聚合物溶液和拥挤的细胞内环境组成的折叠生物大分子之间的差异,并有助于开发使用体外大分子拥挤的控制分子自组装。
Dissolved polymers directed molecular crystallization behavior under dilute and crowding conditions. Larger poly(ethylene glycol)s (PEGs) accelerated caffeine crystal formation in the dilute regime of PEG solutions, which was attributed to the depletion attraction that promoted caffeine cluster aggregation into crystal nuclei. In the semidilute regime, the crystal formation rate was insensitive to the molecular weight of PEGs. This observation was consistent with polymer blob properties, which govern depletion attraction and maintain a constant size at a given polymer concentration, irrespective of molecular weight in the semidilute regime.We demonstrate that dissolved polymers can direct molecular crystallization behavior under dilute and crowded conditions. Larger poly(ethylene glycol)s (PEGs) accelerated caffeine crystal formation in the dilute regime of PEG solutions, which was attributed to the depletion attraction that promoted caffeine cluster aggregation into crystal nuclei. Alternatively, in the semidilute regime, the caffeine crystal formation rate was insensitive to the molecular weight (MW) of PEGs. PEGs with various MWs appeared to induce depletion attraction to a similar extent as the properties of polymer solutions in the semidilute regime described by blobs, which are constant in size at a given polymer concentration irrespective of MW. This study highlights differences between in vitro polymer solutions and crowded intracellular environments composed of folded biomacromolecules and contributes to developing the use of in vitro macromolecular crowding for the control of molecular self-assembly.