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Highly stretchable hydrogels from complex coacervation of natural polyelectrolytes
Soft Matter ( IF 2.9 ) Pub Date : 2017-09-14 00:00:00 , DOI: 10.1039/c7sm01215b Gautier Lalevée 1, 2, 3, 4, 5 , Laurent David 1, 2, 3, 4, 5 , Alexandra Montembault 1, 2, 3, 4, 5 , Kevin Blanchard 1, 2, 3, 4, 5 , John Meadows 5, 6, 7, 8 , Sébastien Malaise 5, 6, 7, 8 , Agnès Crépet 1, 2, 3, 4, 5 , Isabelle Grillo 5, 9, 10 , Isabelle Morfin 5, 11, 12, 13, 14 , Thierry Delair 1, 2, 3, 4, 5 , Guillaume Sudre 1, 2, 3, 4, 5
Soft Matter ( IF 2.9 ) Pub Date : 2017-09-14 00:00:00 , DOI: 10.1039/c7sm01215b Gautier Lalevée 1, 2, 3, 4, 5 , Laurent David 1, 2, 3, 4, 5 , Alexandra Montembault 1, 2, 3, 4, 5 , Kevin Blanchard 1, 2, 3, 4, 5 , John Meadows 5, 6, 7, 8 , Sébastien Malaise 5, 6, 7, 8 , Agnès Crépet 1, 2, 3, 4, 5 , Isabelle Grillo 5, 9, 10 , Isabelle Morfin 5, 11, 12, 13, 14 , Thierry Delair 1, 2, 3, 4, 5 , Guillaume Sudre 1, 2, 3, 4, 5
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The controlled complex coacervation of oppositely charged hyaluronic acid (Mw ≈ 800–1000 kg mol−1) and chitosan (Mw ≈ 160 kg mol−1, degree of acetylation = 15%) led to hydrogels with controllable properties in terms of elasticity and strength. In this work, we performed desalting by dialysis of high ionic strength solutions of mixed polyelectrolytes and showed that the control of the pH during the polyelectrolyte assembly greatly impacts the mechanical properties of the hydrogel. First, for pHs from 5.5 to 7.5, a slight coacervation was observed due to low chitosan protonation and poor polyelectrolyte associations. Then, for pHs from 3.0 to 5.5, coacervation and syneresis led to free-standing and easy to handle hydrogels. Finally, for pHs from 2.0 to 3.0 (close to the pKa of the hyaluronic acid), we observed the unusual stretchability of these hydrogels that could arise from the pre-folding of hyaluronic acid chains while physical crosslinking was achieved by hyaluronic acid/chitosan polyelectrolyte complexation.
中文翻译：
天然聚电解质复杂凝聚产生的高度可拉伸水凝胶
带相反电荷的透明质酸的控制复合凝聚（中号瓦特≈800-1000公斤摩尔-1）和脱乙酰壳多糖（中号瓦特≈160公斤摩尔-1，乙酰化度= 15％）导致水凝胶在弹性和强度方面具有可控的特性。在这项工作中，我们通过透析高离子强度的混合聚电解质溶液进行脱盐，结果表明在聚电解质组装过程中对pH值的控制极大地影响了水凝胶的机械性能。首先，对于5.5至7.5的pH值，由于壳聚糖的质子化程度低和聚电解质缔合性差，因此观察到了轻微的凝聚。然后，对于pH值从3.0到5.5，凝聚和脱水收缩会导致自立且易于处理的水凝胶。最后，对于2.0到3.0的pH值（接近p K a 透明质酸），我们观察到这些水凝胶的异常拉伸性可能来自透明质酸链的预折叠，而通过透明质酸/壳聚糖聚电解质络合实现了物理交联。
更新日期：2017-09-14
中文翻译：
天然聚电解质复杂凝聚产生的高度可拉伸水凝胶
带相反电荷的透明质酸的控制复合凝聚（中号瓦特≈800-1000公斤摩尔-1）和脱乙酰壳多糖（中号瓦特≈160公斤摩尔-1，乙酰化度= 15％）导致水凝胶在弹性和强度方面具有可控的特性。在这项工作中，我们通过透析高离子强度的混合聚电解质溶液进行脱盐，结果表明在聚电解质组装过程中对pH值的控制极大地影响了水凝胶的机械性能。首先，对于5.5至7.5的pH值，由于壳聚糖的质子化程度低和聚电解质缔合性差，因此观察到了轻微的凝聚。然后，对于pH值从3.0到5.5，凝聚和脱水收缩会导致自立且易于处理的水凝胶。最后，对于2.0到3.0的pH值（接近p K a 透明质酸），我们观察到这些水凝胶的异常拉伸性可能来自透明质酸链的预折叠，而通过透明质酸/壳聚糖聚电解质络合实现了物理交联。
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