Structural Insights into the Mechanism of Heat-Set Gel Formation of Polyisocyanopeptide Polymers.,Macromolecular Rapid Communications

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Structural Insights into the Mechanism of Heat-Set Gel Formation of Polyisocyanopeptide Polymers.
Macromolecular Rapid Communications ( IF 4.2 ) Pub Date : 2020-08-06 , DOI: 10.1002/marc.202000304
Mikhail Gavrilov ₁ , Elliot P Gilbert _{2,

3} , Alan E Rowan ₁ , Jan Lauko ₁ , Gleb E Yakubov _{4,

5}

Affiliation

One of the key factors influencing the mechanical properties of natural and synthetic extracellular matrices (ECM) is how large‐scale 3D gel‐like structures emerge from the molecular self‐assembly of individual polymers. Here, structural characterization using small‐angle neutron scattering (SANS) of ECM‐mimicking polyisocyanopeptide (PIC) hydrogels are reported as a function of background ions across the Hofmeister series. More specifically, the process of polymer assembly is examined by probing the structural features of the heat‐set gels and correlating them with their rheological and micro‐mechanical properties. The molecular parameters obtained from SANS clearly show changes in polymer conformation which map onto the temperature‐induced changes in rheological and micro‐mechanical behavior. The formation of larger structures are linked to the formation of cross‐links (or bundles), whilst the onset of their detection in the SANS is putatively linked to their concentration in the gel. These insights provide support for the ‘hot‐spot’ gelation mechanism of PIC heat‐set gels. Finally, it is found that formation of cross‐links and heat‐set gelling properties can be strongly influenced by ions in accordance with Hofmeister series. In practice, these results have significance since ions are inherently present in high concentration during cell culture studies; this may therefore influence the structure of synthetic ECM networks.

中文翻译：

聚异氰基肽聚合物热定型凝胶形成机理的结构见解。

影响天然和合成细胞外基质（ECM）力学性能的关键因素之一是大型3D凝胶状结构如何从单个聚合物的分子自组装中出现。在此，据报道，在整个Hofmeister系列中，使用ECM模拟聚异氰基肽（PIC）水凝胶的小角度中子散射（SANS）进行结构表征是背景离子的作用。更具体地说，通过探测热固性凝胶的结构特征并将其与流变学和微机械性能相关联，来检查聚合物的组装过程。从SANS获得的分子参数清楚地显示出聚合物构象的变化，这些变化映射到温度引起的流变和微机械行为的变化。较大结构的形成与交联（或束）的形成有关，而在SANS中检测到它们的开始则与它们在凝胶中的浓度有关。这些见解为PIC热固性凝胶的“热点”胶凝机制提供了支持。最后，发现根据Hofmeister系列，离子会强烈影响交联的形成和热定型胶凝性能。实际上，这些结果具有重要意义，因为在细胞培养研究中，离子固有地以高浓度存在。因此，这可能会影响合成ECM网络的结构。这些见解为PIC热固性凝胶的“热点”胶凝机制提供了支持。最后，发现根据Hofmeister系列，离子会强烈影响交联的形成和热定型胶凝性能。实际上，这些结果具有重要意义，因为在细胞培养研究中，离子固有地以高浓度存在。因此，这可能会影响合成ECM网络的结构。这些见解为PIC热固性凝胶的“热点”胶凝机制提供了支持。最后，发现根据Hofmeister系列，离子会强烈影响交联的形成和热定型胶凝性能。实际上，这些结果具有重要意义，因为在细胞培养研究中，离子固有地以高浓度存在。因此，这可能会影响合成ECM网络的结构。

更新日期：2020-09-22

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