Boronic acid and diol-containing polymers: how to choose the correct couple to form “strong” hydrogels at physiological pH,Soft Matter

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Boronic acid and diol-containing polymers: how to choose the correct couple to form “strong” hydrogels at physiological pH
Soft Matter ( IF 2.9 ) Pub Date : 2020-03-19 , DOI: 10.1039/d0sm00178c
Tamiris Figueiredo _{1,

2,

3,

4} , Vanina Cosenza _{1,

2,

3,

4} , Yu Ogawa _{1,

2,

3,

4} , Isabelle Jeacomine _{1,

2,

3,

4} , Alicia Vallet _{1,

5,

6,

7,

8} , Sonia Ortega _{1,

2,

3,

4} , Raphael Michel _{1,

2,

3,

4} , Johan D. M. Olsson _{9,

10,

11} , Thibaud Gerfaud _{4,

9,

12} , Jean-Guy Boiteau _{4,

9,

12} , Jing Jing _{4,

9,

12} , Craig Harris _{4,

9,

12} , Rachel Auzély-Velty _{1,

2,

3,

4}

Affiliation

Dynamic covalent hydrogels crosslinked by boronate ester bonds are promising materials for biomedical applications. However, little is known about the impact of the crosslink structure on the mechanical behaviour of the resulting network. Herein, we provide a mechanistic study on boronate ester crosslinking upon mixing hyaluronic acid (HA) backbones modified, on the one hand, with two different arylboronic acids, and on the other hand, with three different saccharide units. Combining rheology, NMR and computational analysis, we demonstrate that carefully selecting the arylboronic-polyol couple allows for tuning the thermodynamics and molecular exchange kinetics of the boronate ester bond, thereby controlling the rheological properties of the gel. In particular, we report the formation of “strong” gels (i.e. featuring slow relaxation dynamics) through the formation of original complex structures (tridentate or bidentate complexes). These findings offer new prospects for the rational design of hydrogel scaffolds with tailored mechanical response.

中文翻译：

含硼酸和含二醇的聚合物：如何选择正确的对在生理pH下形成“强”水凝胶

通过硼酸酯键交联的动态共价水凝胶是用于生物医学应用的有前途的材料。然而，关于交联结构对所得网络的机械性能的影响知之甚少。在本文中，我们提供了将一方面与两种不同的芳基硼酸修饰的透明质酸（HA）主链混合，另一方面与三种不同的糖基单元修饰的硼酸酯交联的机理研究。结合流变学，核磁共振和计算分析，我们证明了仔细选择芳基硼酸酯-多元醇对可以调节硼酸酯键的热力学和分子交换动力学，从而控制凝胶的流变性。特别是，我们报告了“强”凝胶的形成（即通过形成原始的复杂结构（三齿或二齿复合物）而具有缓慢的松弛动力学）。这些发现为合理设计具有适当机械响应的水凝胶支架提供了新的前景。

更新日期：2020-04-24

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