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在作为溶致液晶模板的十六烷基三甲基溴化铵存在下通过自由基聚合制备的抗菌聚(-[3-(二甲基氨基丙基)]甲基丙烯酰胺)水凝胶的机械性能得到改善。

Improved mechanical properties of antimicrobial poly(-[3-(dimethylaminopropyl)] methacrylamide) hydrogels prepared by free radical polymerization in the presence of cetyltrimethylammonium bromide as a lyotropic liquid crystal template.

机构信息

Chemistry Department, Istanbul Technical University, Maslak, Istanbul 34469, Turkey.

Department of Molecular Biology and Genetics, Faculty of Engineering and Natural Sciences, Bahcesehir University, Besiktas, Istanbul 34353, Turkey.

出版信息

Soft Matter. 2022 Jun 1;18(21):4156-4166. doi: 10.1039/d2sm00186a.

Abstract

The poor mechanical strength of the poly(-[3-(dimethylamino)propyl] methacrylamide) (PDMAPMAAm) hydrogel limits its application as a drug delivery system and antimicrobial agent. In this study, both its morphology and antibacterial effectiveness were controlled through free radical solution polymerization in the presence of cetyltrimethylammonium bromide (CTAB; cationic nonreactive surfactant), forming lyotropic liquid crystal (LLC) mesophases. All the templated reactions proceeded in four different CTAB concentrations with three different concentrations of DMAPMAAm (2.0, 3.0 and 4.0 mol L), which were carried out in distilled-deionized water (DDW) using potassium persulfate (KPS) and ,'-methylenebisacrylamide (BIS) as the initiator and crosslinker, respectively. The pH-dependent phase transition temperature (34 °C at pH 14), compression moduli, antibacterial and diffusion properties, and the effect of the LLC mesophases of CTAB on the hydrogel properties were investigated by mechanical measurements, image analysis, inhibition zone tests, X-ray diffractograms and polarized optical microscopy (POM). It was found that the compression moduli of the templated (T)-PDMAPMAAm hydrogels increased by nearly ten times (from ∼3.0 to 30.0 kPa) compared to that of the isotropic (I) ones. The POM and XRD results before the removal of CTAB exhibited the formation of lamellar and hexagonal mesophases. Further, the inhibition zones showed the ability of the I-PDMAPMAAm hydrogels to reduce the activity of even in the absence of CTAB, gentamicin (GS) and ciprofloxacin (CF). This was because the quaternary ammonium (QA) groups on the DMAPMAAm units could interact with the bacterial membrane.

摘要

聚([3-(二甲氨基)丙基]甲基丙烯酰胺)(PDMAPMAAm)水凝胶的机械强度较差,限制了其作为药物输送系统和抗菌剂的应用。在这项研究中,通过在十六烷基三甲基溴化铵(CTAB;阳离子非反应性表面活性剂)存在下的自由基溶液聚合,控制其形态和抗菌效果,形成溶致液晶(LLC)中间相。所有模板反应都在四种不同的 CTAB 浓度下进行,使用过硫酸钾(KPS)和亚甲基双丙烯酰胺(BIS)分别作为引发剂和交联剂,在去离子水中(DDW)进行了三种不同浓度的 DMAPMAAm(2.0、3.0 和 4.0 mol/L)的反应。通过机械测量、图像分析、抑菌圈试验、X 射线衍射图谱和偏光显微镜(POM)研究了 pH 依赖性的相转变温度(pH 14 时为 34°C)、压缩模量、抗菌和扩散性能以及 CTAB 的 LLC 中间相对水凝胶性能的影响。结果发现,与各向同性(I)水凝胶相比,模板(T)-PDMAPMAAm 水凝胶的压缩模量增加了近十倍(从约 3.0 增加到 30.0 kPa)。在去除 CTAB 之前,POM 和 XRD 结果显示形成了层状和六方中间相。此外,抑菌圈结果表明,即使在没有 CTAB、庆大霉素(GS)和环丙沙星(CF)的情况下,I-PDMAPMAAm 水凝胶也能够降低的活性。这是因为 DMAPMAAm 单元上的季铵(QA)基团可以与细菌膜相互作用。

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