罗静,戴苗,刘晓亚,李小杰.pH响应性聚合物抗菌涂层的制备及性能研究[J].表面技术,2021,50(10):194-204, 278.
LUO Jing,DAI Miao,LIU Xiao-ya,LI Xiao-jie.Preparation of pH-responsive Polymer Antibacterial Coating and Its Performance[J].Surface Technology,2021,50(10):194-204, 278
pH响应性聚合物抗菌涂层的制备及性能研究
Preparation of pH-responsive Polymer Antibacterial Coating and Its Performance
投稿时间:2021-01-19  修订日期:2021-04-08
DOI:10.16490/j.cnki.issn.1001-3660.2021.10.018
中文关键词:  防污杀菌  聚合物涂层  pH响应  席夫碱  聚乙二醇(PEG)  不锈钢316L
英文关键词:antifouling coating  antibacterial coating  schiff base  polyethylene glycol (PEG)  pH response
基金项目:江南大学研究生科研与实践创新计划项目(JNKY19_046)
作者单位
罗静 江南大学 合成与生物胶体教育部重点实验室,江苏 无锡 214122;江南大学化学与材料工程学院,江苏 无锡 214122 
戴苗 江南大学 合成与生物胶体教育部重点实验室,江苏 无锡 214122;江南大学化学与材料工程学院,江苏 无锡 214122 
刘晓亚 江南大学 合成与生物胶体教育部重点实验室,江苏 无锡 214122;江南大学化学与材料工程学院,江苏 无锡 214122 
李小杰 江南大学 合成与生物胶体教育部重点实验室,江苏 无锡 214122;江南大学化学与材料工程学院,江苏 无锡 214122 
AuthorInstitution
LUO Jing Key Laboratory of Synthetic and Biological Colloids, Ministry of Education,University, Wuxi 214122, China;School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China 
DAI Miao Key Laboratory of Synthetic and Biological Colloids, Ministry of Education,University, Wuxi 214122, China;School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China 
LIU Xiao-ya Key Laboratory of Synthetic and Biological Colloids, Ministry of Education,University, Wuxi 214122, China;School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China 
LI Xiao-jie Key Laboratory of Synthetic and Biological Colloids, Ministry of Education,University, Wuxi 214122, China;School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China 
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中文摘要:
      目的 制备一种具有pH响应性的智能聚合物抗菌涂层,能按需实现涂层从防污到杀菌功能的转换。方法 以季铵盐甲基丙烯酰氧乙基二甲基辛烷基溴化铵(DMAEMA-8C)、对-(2-甲基丙烯氧乙氧基)苯甲醛(MAEBA)和甲基丙烯酸异辛酯(EHA)作为共聚单体,通过自由基聚合制备了一种季铵盐聚合物PMQE-CHO,并将其利用浸涂技术在不锈钢316L(SS)表面制备季铵盐聚合物涂层SS-PMQE-CHO。随后,使用PEG-NH2对季铵盐涂层SS-PMQE-CHO表面进行接枝改性,得到pH响应性聚合物涂层SS-PMQE-PEG。对涂层的基本性能进行了表征。通过大肠杆菌和荧光素偶联的牛血清白蛋白(FITC-BSA)的附着力测试,评估涂层的防污和抗菌性能。利用抗菌实验表征涂层在不同pH条件下的抗菌效果。进行体外细胞毒性分析和溶血试验,评估涂层的生物相容性。结果 涂层结构致密规整、机械性能优异,具有良好的生物相容性和低溶血率,并且可以有效地防止BSA和大肠杆菌的粘附。在菌液里培养10 h后,涂层SS-PMQE-PEG-30和SS-PMQE-PEG-40表面的细菌与SS表面的细菌相比,分别减少了94%和96%。此时,PEG显示出有效的防污作用。在菌液里培养24 h后,菌液的pH值降低。涂层SS-PMQE-PEG-30和SS-PMQE-PEG-40的功能从防污转化为杀菌,杀菌效率分别为93%和92%。即使是在PBS中浸泡两周后,涂层仍呈现出良好的功能转化性能。结论 在正常条件下,涂层SS-PMQE-PEG中的PEG可以有效抵抗蛋白质和细菌的粘附。当涂层附近的微环境变为弱酸性时,席夫碱键发生断裂,此时涂层底部的杀菌层暴露出来,以杀死细菌并抑制感染的发生。
英文摘要:
      The work aims to prepare a smart polymer antibacterial coating with pH responsiveness, where the conversion of the coating function from antifouling to sterilization can be realized on demand. Firstly, methacryloxyethyl dimethyl octyl ammonium bromide (DMAEMA-8C), p-(2-methacryloxyethoxy) benzaldehyde (MAEBA) and methacrylic acid (EHA) were used as comonomer to prepare a quaternary ammonium salt polymer PMQE-CHO by free radical polymerization. And then the quaternary ammonium salt polymer coating SS-PMQE-CHO was prepared on the surface of stainless steel 316L (SS) through dip-dipping technique. Subsequently, PEG-NH2 was used to modify the surface of SS-PMQE-CHO to obtain SS-PMQE-PEG. After the basic performance of the coatings was characterized by SEM, XPS, WCA, etc, the adhesion test of E. coli and fluorescein-coupled bovine serum albumin (FITC-BSA) were used to evaluate the antifouling and antibacterial performance of the coatings. The antibacterial effect of the coatings were investigated through antibacterial experiments to verify the responsiveness in different pH conditions. And the biocompatibility of the coatings was evaluated by in vitro cytotoxicity analysis and hemolysis test. The results show that the coatings have compact and neat structure, excellent mechanical property, good biocompatibility, low hemolysis rate and effective prevention from the adhesion of BSA and E. coli. Compared with bare SS surface, the bacteria on the surface of SS-PMQE-PEG-30 and SS-PMQE-PEG-40 are respectively reduced by 94% and 96% after 10-hour incubation in the bacterial solution. At this time, PEG shows effective antifouling property. After the 24-hour culture, the pH value of bacterial solution decreases. Therefore, the functions of the coating SS-PMQE-PEG-30 and SS-PMQE- PEG-40 change from antifouling to sterilization, and the sterilization efficiency is 93% and 92%, respectively. Even after being soaked in PBS for two weeks, the coating still exhibits good functional transformation properties. Normally, the PEG in the coating SS-PMQE-PEG can effectively resist the adhesion.of protein and bacterial. When the microenvironment near the coating becomes weakly acidic, the schiff base bonds break. At this point, the bactericidal layer at the bottom of the coating is exposed to kill bacteria and suppress infection.
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