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Synthesis of Poly(ε-caprolactone) Diacrylate for Micelle-Cross-Linked Sodium AMPS Hydrogel for Use as Controlled Drug Delivery Wound Dressing
Biomacromolecules ( IF 5.5 ) Pub Date : 2021-08-11 , DOI: 10.1021/acs.biomac.1c00683
Amlika Rungrod 1 , Apichaya Kapanya 1 , Winita Punyodom 1, 2 , Robert Molloy 2, 3 , Jomkhwan Meerak 4 , Runglawan Somsunan 1, 2
Affiliation  

This study focuses on the synthesis of poly(ε-caprolactone) diacrylate (PCLDA) for the fabrication of micelle-cross-linked sodium AMPS wound dressing hydrogels. The novel synthetic approach of PCLDA is functionalizing a PCL diol with acrylic acid. The influences of varying the PCL diol/AA molar ratio and temperature on the suitable conditions for the synthesis of PCLDA are discussed. The hydrogel was synthesized through micellar copolymerization of sodium 2-acrylamido-2-methylpropane sulfonate (Na-AMPS) as a basic monomer and PCLDA as a hydrophobic association monomer. In this study, an attempt was made to develop new hydrogel wound dressings meant for the release of antibacterial drugs (ciprofloxacin and silver sulfadiazine). The chemical structures, morphology, porosity, and water interaction of the hydrogels were characterized. The hydrogels’ swelling ratio and water vapor transmission rate (WVTR) showed a high swelling capacity (4688–10753%) and good WVTR (approximately 2000 g·m–2·day–1), which can be controlled through variation of the PCLDA concentration. The mechanical property results confirmed that PCLDA improved the mechanical properties of the hydrogel; the stress increased from 37 to 68 kPa, and the strain increased from 198 to 360% with increasing PCLDA (0–30% wt of Na-AMPS). These hydrogels presented no cytotoxicity based on over 70% cell viability responses (L929 fibroblasts) using an in vitro 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide (MTT) assay. Additionally, the drug release mechanism, kinetic models, and antibacterial activity were determined. The results demonstrated that antibiotics were released from the hydrogel with a Fickian diffusion mechanism and antibacterial activity against Gram-negative bacteria (Escherichia coli and Pseudomonas aeruginosa) and Gram-positive bacteria (Staphylococcus aureus). Based on the results obtained, and bearing in mind that further progress still needs to be made, the fabricated hydrogels show considerable potential for meeting the stringent property requirements of hydrogel wound dressings.

中文翻译:

聚(ε-己内酯)二丙烯酸酯的合成用于胶束交联的 AMPS 钠水凝胶作为受控药物递送伤口敷料

本研究的重点是合成聚(ε-己内酯)二丙烯酸酯(PCLDA),用于制备胶束交联的钠 AMPS 伤口敷料水凝胶。PCLDA 的新合成方法是用丙烯酸对 PCL 二醇进行功能化。讨论了改变 PCL 二醇/AA 摩尔比和温度对合成 PCLDA 的合适条件的影响。该水凝胶是通过 2-丙烯酰胺基-2-甲基丙烷磺酸钠 (Na-AMPS) 作为基本单体和 PCLDA 作为疏水缔合单体的胶束共聚反应合成的。在这项研究中,尝试开发用于释放抗菌药物(环丙沙星和磺胺嘧啶银)的新型水凝胶伤口敷料。表征了水凝胶的化学结构、形态、孔隙率和水相互作用。–2 ·天–1 ),可以通过改变 PCLDA 浓度来控制。力学性能结果证实PCLDA提高了水凝胶的力学性能;随着 PCLDA(Na-AMPS 的 0-30% wt)的增加,应力从 37 kPa 增加到 68 kPa,应变从 198% 增加到 360%。基于使用体外3-(4,5-二甲基噻唑-2-基)-2,5-二苯基溴化四唑 (MTT) 测定的超过 70% 的细胞活力反应(L929 成纤维细胞),这些水凝胶没有表现出细胞毒性。此外,还确定了药物释放机制、动力学模型和抗菌活性。结果表明,抗生素从水凝胶中释放出来,具有 Fickian 扩散机制和对革兰氏阴性菌的抗菌活性。大肠杆菌铜绿假单胞菌)和革兰氏阳性菌(金黄色葡萄球菌)。基于所获得的结果,并记住仍需取得进一步进展,所制造的水凝胶显示出满足水凝胶伤口敷料严格性能要求的巨大潜力。
更新日期:2021-09-13
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