Quantifying Thermoswitchable Carbohydrate-Mediated Interactions via Soft Colloidal Probe Adhesion Studies.
Quantifying Thermoswitchable Carbohydrate-Mediated Interactions via Soft Colloidal Probe Adhesion Studies.
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DOI：
10.1002/mabi.202000186
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发表时间：
2020-08
影响因子：
4.6
通讯作者：
A. K. Strzelczyk;T. Paul;Stephan Schmidt
中科院分区：
文献类型：
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作者：
A. K. Strzelczyk;T. Paul;Stephan Schmidt
热敏聚合物可以实现外部可控的生物分子相互作用，但滞后效应阻碍了这些材料的可逆性和重复使用。为了量化依赖于温度的相互作用和滞后效应，使用了基于结合刀豆蛋白A表面甘露糖的聚乙二醇微胶体(软胶体探针，SCP)的光学结合分析。合成了一系列不同碳水化合物类型、密度和连接物类型的热响应性糖共聚物，然后将其接枝到SCP上。碳水化合物介导的粘附力受糖配体密度的影响，并在糖共聚物的较低临界溶液温度(LCST)以上增加。重要的是，观察到了一个强烈的滞后现象，即冷却回到LCST以下并不会将附着力降低到加热前的初始值。对于疏水连接体和低碳水化合物官能化程度，滞后更强，这表明由于疏水相互作用，聚合物没有充分的再溶胀。通过研究大肠杆菌与SCP的粘附性，证实了这一结果，在LCST上方观察到细菌的增强捕获，而冷却时不可能分离。总体而言，关于特定结合聚合物的可切换粘附性的定量数据可能为下一代交互生物材料的设计提供潜在的途径。
Thermosensitive polymers enable externally controllable biomolecular interactions but hysteresis effects hamper the reversibility and repeated use of these materials. To quantify the temperature-dependent interactions and hysteresis effects, an optical adhesion assay based on poly(ethylene glycol) microgels (soft colloidal probes, SCPs) with mannose binding concanavalin A surfaces is used. A series of thermoresponsive glycopolymers is synthesized varying the carbohydrate type, their density, and linker type, and then grafted to the SCPs. The carbohydrate-mediated adhesion is influenced by the density of sugar ligands and increased above the lower critical solution temperature (LCST) of the glycopolymer. Importantly, a strong hysteresis is observed, i.e., cooling back below the LCST does not reduce the adhesion back to the initial value before heating. The hysteresis is stronger for hydrophobic linkers and for low carbohydrate functionalization degrees suggesting insufficient reswelling of the polymers due to hydrophobic interactions. The results are confirmed by studying the adhesion of Escherichia coli to the SCPs, where an enhanced capture of the bacteria is observed above the LCST while the detachment upon cooling is not possible. Overall, the quantitative data on the switchable adhesion of specifically binding polymers may provide potential avenues for the design of the next-generation interactive biomaterials.