Polyelectrolyte complex scaffoldings for photocrosslinked hydrogels
Polyelectrolyte complex scaffoldings for photocrosslinked hydrogels
复制标题
用于光交联水凝胶的聚电解质复合支架
DOI：
10.1039/d2me00171c
复制
发表时间：
2023
影响因子：
3.6
通讯作者：
Srivastava, Samanvaya
中科院分区：
文献类型：
--
作者：
Li, Defu;Ghovvati, Mahsa;Annabi, Nasim;Srivastava, Samanvaya
可光交联的前体(小分子或聚合物)在光照射下发生快速交联，形成共价交联的水凝胶。这种可以在原位实现的时空可控的交联性，鼓励了光交联水凝胶作为生物粘合剂、生物印刷油墨和细胞外基质模拟物在生物医学中的应用。然而，前驱体溶液的低粘度导致不必要的流动和稀释，导致操作困难和光交联水凝胶的强度降低。在这里，我们引入带相反电荷的三嵌段聚电解质作为前驱体溶液的添加剂，将其转化为具有更高剪切强度和粘度的自组装聚电解质复合体(PEC)水凝胶，提供临时保护，防止前驱体稀释并缓解二次流动。PEC网络还增强了光交联水凝胶的性质。先驱体在光照射下的交联会导致与PEC和共价连接网络形成互穿聚合物网络水凝胶，其剪切模数超过组成网络模数的线性组合，并克服了限制共价连接水凝胶性能的拉伸强度-延伸性权衡。增强方法被证明与四种类型的光交联前驱体兼容，不需要对前驱体进行任何修改，并且引入了最少的处理步骤，为生物医学应用的光交联性材料的更广泛的平移铺平了道路。
Photocrosslinkable precursors (small molecules or polymers) undergo rapid crosslinking upon photoirradiation, forming covalently crosslinked hydrogels. The spatiotemporally controlled crosslinking, which can be achieved in situ, encourages the utility of photocrosslinked hydrogels in biomedicine as bioadhesives, bioprinting inks, and extracellular matrix mimics. However, the low viscosity of the precursor solutions results in unwanted flows and dilution, leading to handling difficulties and compromised strength of the photocrosslinked hydrogels. Here, we introduce oppositely charged triblock polyelectrolytes as additives for precursor solutions that transform them into self-assembled polyelectrolyte complex (PEC) hydrogels with enhanced shear strength and viscosity, providing interim protection against precursor dilution and mitigating secondary flows. The PEC network also augments the properties of the photocrosslinked hydrogels. Crosslinking of the precursors upon photoirradiation results in the formation of interpenetrating polymer network hydrogels with PEC and covalently-linked networks that exhibit shear moduli exceeding the linear combination of the moduli of the constituent networks and overcome the tensile strength–extensibility tradeoff that restricts the performance of covalently-linked hydrogels. The reinforcement approach is shown to be compatible with four types of photocrosslinkable precursors, does not require any modification of the precursors, and introduces minimal processing steps, paving the way for a broader translation of photocrosslinkable materials for biomedical applications.