Casillas-Popova Sofia Nieves, Lokuge Nishadi Dilkushi, Singh Prerna, Cirillo Arianna, Thinphang-Nga Anna, Skinner Cameron D, Vuckovic Dajana, Findlay Brandon L, Oh Jung Kwon
Department of Chemistry and Biochemistry, Concordia University, Montreal, Quebec, H4B 1R6, Canada.
Department of Biology, Concordia University, Montreal, Quebec, H4B 1R6, Canada.
J Mater Chem B. 2025 Jul 16;13(28):8419-8433. doi: 10.1039/d5tb00738k.
Owing to their high aspect ratio of length to diameter, large surface area, large pore size, and high molecular orientation, electro-spun (e-spun) nanofibrous mats have been explored as effective nanomaterials for various applications, including wound dressings and healing materials. Of particular interest are poly(vinyl alcohol) (PVA) e-spun nanofibers that are required to be crosslinked with covalent organic bonds to retain their structural integrity in wound environments. However, conventionally crosslinked PVA nanofibers present critical drawbacks, typically including the uncontrolled release of encapsulated drug molecules. Herein, we report a robust approach that centers on the integration of boronic ester (BE) chemistry into the design of PVA e-spun nanofibers crosslinked through the formation of degradable BE crosslinks. A new phenyldiboronic acid with an ethylene spacer, which is biocompatible and has a lower p value, is proved to be an effective crosslinker to fabricate BE-crosslinked PVA e-spun nanofibrous materials. In response to multiple stimuli such as reactive oxygen species, alkaline pH, and glucose (common features of wounds), the fibers degrade through the cleavage of BE bonds or transesterification, confirmed by our model spectroscopic study with a small molecular boronic ester. Such wound-induced degradation ensures the controlled/enhanced release of antibiotics active against both Gram-positive and Gram-negative bacteria. These results, combined with their non-hemolysis and non-cytotoxicity properties, demonstrate that the approach is versatile for the fabrication of well-defined BE-crosslinked PVA e-spun nanofibers that are dimensionally stable but degrade to release antibiotics in wounds, thus exhibiting a great promise as smart wound dressing materials.
由于其长径比高、表面积大、孔径大以及分子取向性高，电纺纳米纤维垫已被探索作为用于各种应用的有效纳米材料，包括伤口敷料和愈合材料。特别令人感兴趣的是聚（乙烯醇）（PVA）电纺纳米纤维，其需要通过共价有机键交联以在伤口环境中保持其结构完整性。然而，传统交联的PVA纳米纤维存在关键缺点，通常包括封装药物分子的不受控制释放。在此，我们报告了一种稳健的方法，该方法以将硼酸酯（BE）化学整合到通过形成可降解BE交联来交联的PVA电纺纳米纤维的设计中为核心。一种具有乙烯间隔基的新型苯基二硼酸，其具有生物相容性且p值较低，被证明是制备BE交联的PVA电纺纳米纤维材料的有效交联剂。响应于多种刺激，如活性氧、碱性pH和葡萄糖（伤口的常见特征），纤维通过BE键的裂解或酯交换反应而降解，这通过我们对小分子硼酸酯的模型光谱研究得到证实。这种伤口诱导的降解确保了对革兰氏阳性和革兰氏阴性细菌均有活性的抗生素的可控/增强释放。这些结果，结合其非溶血和非细胞毒性特性，表明该方法对于制备定义明确的BE交联的PVA电纺纳米纤维具有通用性，这些纳米纤维尺寸稳定但在伤口中降解以释放抗生素，因此作为智能伤口敷料材料展现出巨大的前景。
