A Shear-thinning electrostatic hydrogel with antibacterial activity by nanoengineering of polyelectrolytes

A Shear-thinning electrostatic hydrogel with antibacterial activity by nanoengineering of polyelectrolytes
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通过聚电解质纳米工程制备具有抗菌活性的剪切稀化静电水凝胶

DOI:
10.1039/c9bm01386e
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发表时间:
--
影响因子:
6.6
通讯作者:
Zhu Weipu
Zhu Weipu
中科院分区:
工程技术2区
文献类型:
--
作者:
Zhu Yanhui;Luo Qiaojie;Zhang Hongjie;Cai Qiuquan;Li Xiaodong;Shen Zhiquan;Zhu Weipu

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通过亲水性聚合物之间的非共价相互作用可以制备可注射剪切减薄水凝胶。虽然静电力是一种典型的非共价相互作用,但两种带相反电荷的聚电解质的直接混合通常会产生复杂的凝聚体,而不是可注射的水凝胶。本文提出了一种利用聚电解质纳米工程制备剪切减薄水凝胶的简便方法。将甲氧基聚乙二醇-嵌段聚(ε-己内酯)和聚(ε-己内酯)-嵌段聚(六亚甲基胍)-聚(ε-己内酯)在水溶液中混合制备了具有电中性壳层的纳米阳离子胶束。在胶束溶液中加入羧甲基纤维素钠,混合胶束外层的聚乙二醇壳层阻止了聚六亚甲基胍盐酸盐片段与羧甲基纤维素钠之间的瞬间静电相互作用,形成均匀的剪切减薄静电(STES)水凝胶。由于阳离子聚(六亚甲基胍)盐酸段,这种水凝胶对革兰氏阳性和革兰氏阴性细菌都具有很强的抗菌活性。此外,混合胶束的聚(ε-己内酯)核可以有效地包封疏水药物。本研究将该方法制备的姜黄素负载STES水凝胶作为伤口敷料,通过释放姜黄素进一步减少细菌感染,即使在感染的伤口也能促进伤口愈合。本研究为利用聚电解质制备剪切减薄抗菌水凝胶提供了一种简便的方法,具有很大的生物医学应用潜力。
Injectable shear-thinning hydrogels can be prepared by the non-covalent interactions between hydrophilic polymers. Although electrostatic force is a typical non-covalent interaction, direct mixing of two oppositely charged polyelectrolytes usually leads to a complex coacervate rather than an injectable hydrogel. Herein, a facile approach is proposed to prepare a shear-thinning hydrogel by nanoengineering of polyelectrolytes. Nanosized cationic micelles with electroneutral shells were prepared by mixing methoxyl poly(ethylene glycol)-block-poly(ε-caprolactone) and poly(ε-caprolactone)-block-poly(hexamethylene guanidine) hydrochloride-block-poly(ε-caprolactone) in an aqueous solution. When sodium carboxymethyl cellulose was added into the micellar solution, the outer poly(ethylene glycol) shell of mixed micelles prevented the instant electrostatic interaction between poly(hexamethylene guanidine) hydrochloride segments and sodium carboxymethyl cellulose, resulting in a homogenous shear-thinning electrostatic (STES) hydrogel. Because of the cationic poly(hexamethylene guanidine) hydrochloride segments, this hydrogel exhibits strong antibacterial activity against both Gram-positive and Gram-negative bacteria. Furthermore, the poly(ε-caprolactone) core of the mixed micelles can efficiently encapsulate a hydrophobic drug. In this work, curcumin-loaded STES hydrogel prepared by this method was used as wound dressing material that can promote wound healing even in infected wounds by further reducing bacterial infection via releasing curcumin. The present study provides a facile strategy to prepare shear-thinning antibacterial hydrogels from polyelectrolytes, which has great potential in biomedical application.