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用于免疫调节性骨膜再生的鞣花酸接枝羧甲基壳聚糖/氧化石墨烯包覆纳米纤维膜

Ellagic acid-grafted carboxymethyl chitosan/graphene oxide-coated nanofibrous membrane for immunomodulatory periosteal regeneration.

作者信息

Zhang Xue, Luo Chunyi, Liu Na, Liu Siyu, Jiang Zhouquan, Zhou Jinjun, Shao Lishu, Luo Weihua

机构信息

College of Materials Science and Engineering, Central South University of Forestry and Technology, Changsha 410004, PR China.

College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China.

出版信息

Carbohydr Polym. 2025 Oct 15;366:123826. doi: 10.1016/j.carbpol.2025.123826. Epub 2025 May 29.

DOI:10.1016/j.carbpol.2025.123826
PMID:40733780
Abstract

To enhance the clinical value of carboxymethyl chitosan (CMCS) as an osteogenic material, improving its bioactivity and mechanical strength is crucial. Meanwhile, ellagic acid (EA) has strong bioactivities but low bioavailability due to its hydrophobicity. In this study, by introducing EA units into CMCS molecules, a near-infrared (NIR) light-mediated nanofiber membrane based on polycaprolactone (PCL)/EA-CMCS blended nanofibers coated with an EA-CMCS/graphene oxide (GO) layer (PCL/EA-CMCS@EA-CMCS/GO) was designed. The bioactivity of CMCS and bioavailability of EA could be significantly improved by covalent coupling of EA with CMCS. Blending EA-CMCS with PCL significantly enhanced the mechanical properties of nanofiber membranes. The coated nanofibrous membrane featured a multi-level structure of coating and blending. By leveraging the photothermal conversion effect of GO, it enabled the programmed and sustained release of EA-CMCS from both the coating and the nanofibers. Moreover, the membrane exhibited excellent biomineralization and antioxidant capabilities. It effectively regulated macrophage polarization and promoted the adhesion, proliferation, and osteogenic differentiation of MC3T3-E1 osteoblasts. These properties enabled the membrane to regulate the harsh osteogenic immune microenvironment and promote bone regeneration. This biomimetic periosteum holds great potential as a substitute for periosteal grafts and offers a novel strategy for developing artificial periosteum.

摘要

为提高羧甲基壳聚糖(CMCS)作为成骨材料的临床价值,改善其生物活性和机械强度至关重要。同时,鞣花酸(EA)具有很强的生物活性,但由于其疏水性导致生物利用度较低。在本研究中,通过将EA单元引入CMCS分子中,设计了一种基于聚己内酯(PCL)/EA-CMCS混合纳米纤维并涂覆有EA-CMCS/氧化石墨烯(GO)层的近红外(NIR)光介导纳米纤维膜(PCL/EA-CMCS@EA-CMCS/GO)。通过EA与CMCS的共价偶联,可显著提高CMCS的生物活性和EA的生物利用度。将EA-CMCS与PCL混合可显著增强纳米纤维膜的机械性能。涂覆的纳米纤维膜具有涂层和混合的多级结构。通过利用GO的光热转换效应,它能够使EA-CMCS从涂层和纳米纤维中实现程序性和持续释放。此外,该膜表现出优异的生物矿化和抗氧化能力。它有效地调节巨噬细胞极化,并促进MC3T3-E1成骨细胞的粘附、增殖和成骨分化。这些特性使该膜能够调节恶劣的成骨免疫微环境并促进骨再生。这种仿生骨膜作为骨膜移植替代品具有巨大潜力,并为开发人工骨膜提供了一种新策略。

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