氧化石墨烯复合材料的制备及其吸附与抗菌性能研究

发布时间：2018-03-02 13:03

本文选题：氧化石墨烯　切入点：高分子　出处：《吉林大学》2017年博士论文　论文类型：学位论文

【摘要】：由工业发展带来的水体污染日益成为严重的环境威胁之一,水体中的污染物多种多样,包括微生物、金属离子、有机物、染料等。其中染料污染是一个严重的环境问题,因为染料污水量大、成分复杂、色泽深、毒性高。吸附法以其廉价和后处理简单的优势成为广泛采用的去除污染物的方法,因此设计吸附能力优异的新型吸附剂显得尤为重要。而微生物污染是另一个严峻的环境问题,多种细菌可引发各种感染性疾病,威胁到人类健康和经济发展。因此开发和应用高效广谱型的抗菌材料已成为科研及生产领域的热门课题之一。石墨烯,一种二维、单原子层厚度的碳材料,自被首次发现之后已被广泛研究报道。氧化石墨烯(GO)是石墨烯的一种重要衍生物,表面带大量含氧基团,如羟基、羧基和环氧基等。由于GO的这种结构特点,使其具有一些十分优异的性质。近年来,GO及多种GO的复合材料被研究应用为抗菌材料或吸附材料,然而性能更加优异的氧化石墨烯复合材料仍然亟待开发应用。本文从研究GO的性质入手,深入分析了GO的特征,进一步系统研究了GO的吸附和抗菌性能。基于GO的性质特点,用同样兼有吸附和抗菌性能的壳聚糖功能化GO,得到了具有优异的吸附性能和抗菌性能的双功能复合材料,同时针对材料回收困难的问题,引入了Fe3O4磁性纳米材料。从提高GO的抗菌性能的思路出发,用胍类高分子抗菌材料对GO进行功能化,获得了抗菌性能更加优异的复合材料。其次,从防止氧化石墨烯复合材料团聚的思路出发,分别用聚乙二醇(PEG)和壳聚糖进行修饰,获得了两种不易团聚,抗菌性能优异的氧化石墨烯复合材料。论文的主要研究内容如下:1.利用改良的Hummers方法制备了GO,并对其化学结构和形貌进行了表征。通过抗菌实验研究了接触时间和浓度对其抗菌性能的影响,结果表明:GO的抗菌活性在一定范围内随GO的浓度增加而增强,在浓度为2000μg/m L时,表现出最高效的抗菌活性;GO对E.coli和S.aureus的抑菌率随时间的增加而增加;实验进一步测定了GO对E.coli和S.aureus的最小抑菌浓度(MIC),结果显示go对e.coli的抗菌效果要优于s.aureus。通过染料吸附实验研究了go对亚甲基蓝(mb)和罗丹明b(rhb)的吸附性能,结果表明:go具有比传统吸附剂活性炭更加优异的吸附性能;go对mb和rhb的吸附与染料的初始浓度相关,在mb初始浓度为200mg/l和rhb初始浓度为300mg/l时,go的吸附容量较大;吸附动力学研究结果显示go的吸附行为符合准二级动力学模型。2.用磁性壳聚糖(mcs)对go功能化合成了go-mcs磁性复合材料,利用多种测试方法表征了其结构、形貌和性质。通过抗菌实验研究了go-mcs复合材料的抗菌性能,结果显示go-mcs复合材料对e.coli和s.aureus的抗菌活性高于单一组分go和mcs,展示出显著增强的抗菌性能。通过吸附实验研究了go-mcs复合材料的吸附性能,结果表明:go-mcs复合材料具有比go更加优异的吸附性能,对mb和rhb的吸附容量分别为258mg/g和153mg/g;go-mcs对mb和rhb吸附的最佳ph值在5附近;吸附动力学研究结果显示go-mcs的吸附行为符合准二级动力学模型,表明go-mcs对mb和rhb的吸附速率受化学吸附控制;磁性能测试结果显示go-mcs具有超顺磁性,使材料具有磁性可回收性。综上,go-mcs具有优异的吸附性能和抗菌活性,可作为一种多功能材料,既可以去除水体中的染料污染物,亦可以消灭其中的有害菌,兼具有较好的磁性可回收性。3.分别用聚乙二醇(peg)和聚六亚甲基盐酸胍(phgc)对go进行功能化,合成了go-peg-phgc复合材料,并对其结构、形貌和性质进行了表征。go-peg-phgc复合材料保持了go的片层结构,peg的引入避免了go-peg-phgc复合材料的团聚。通过抗菌实验研究了go-peg-phgc对e.coli和s.aureus两种菌的抗菌性能,结果表明分散性良好的go-peg-phgc比易团聚的go-phgc的抗菌活性更强。go-peg-phgc复合材料展示出显著增强的抗菌性能。4.用cs和phgc的复合物cs-phgc对go进行功能化,合成了go-cs-phgc复合材料,并利用多种测试方法表征了其结构、形貌和性质。go-cs-phgc保持了go的片层结构,cs的存在使go-cs-phgc复合材料不易团聚。通过抗菌实验研究了go-cs-phgc对e.coli和s.aureus两种菌的抗菌性能,抗菌实验结果显示go-cs-phgc具有较强的杀菌效力,并且go-cs-phgc的抗菌活性高于任何单一组分(GO、CS、PHGC或CS-PHGC)的抗菌活性,抗菌性能得到显著增强。实验进一步测定了GO-CS-PHGC的MIC值,GO-CS-PHGC复合材料对E.coli的MIC值为32μg/mL,明显低于GO与CS-PHGC混合物,以及GO、CS与PHGC混合物的MIC值,说明GO-CS-PHGC复合材料抗菌性能的增强不是各组分抗菌活性的简单叠加,而是各组分之间协同作用的结果。
[Abstract]:The water pollution caused by industrial development has become one of the serious environmental threat, a variety of pollutants in water, including microorganisms, metal ions, organic compounds, dyes and other dyes. The pollution is a serious environmental problem, because a large amount of dye wastewater, complex components, deep color, high toxicity to the adsorption. Cheap and simple postprocessing has become the widely used method to remove pollutants, so the design of new adsorption ability of excellent adsorption agent is particularly important. The microbial pollution is another serious environmental problems, many kinds of bacteria can cause a variety of infectious diseases, threaten human health and economic development. Therefore the development and application of antibacterial materials efficient broad-spectrum type has become one of the hot topics in the field of scientific research and production. Graphene, a two-dimensional carbon material, a single atomic layer, since it was first discovered has been widely The research reported. Graphene oxide (GO) is a kind of important graphene derivatives, with a large number of surface oxygen groups, such as hydroxyl, carboxyl and epoxy group. Because of the characteristics of the structure of GO, which has some excellent properties. In recent years, research and application of antibacterial materials or composite adsorption material GO and GO are various, however, graphene oxide composite more excellent performance still need to develop applications. The properties of GO with the in-depth analysis of the characteristics of GO system, further study the performance of GO adsorption properties and antibacterial. Based on the characteristic of GO chitosan functionalized GO has antibacterial properties with the same the adsorption and the obtained excellent adsorption properties and antibacterial properties of double functional composite materials, at the same time for material recovery difficult problem, introduced Fe3O4 magnetic nano materials. From improving the GO idea of the antibacterial Hair, with guanidine antibacterial functionalization of GO material, the composite material obtained more excellent antibacterial properties. Secondly, starting from the idea of preventing graphene oxide composite particles, respectively using polyethylene glycol (PEG) and chitosan was modified to obtain two is not easy to agglomerate, excellent antibacterial property of graphite oxide graphene composite materials. The main research contents of this paper are as follows: to prepare GO 1. using the modified Hummers method, and the chemical structure and morphology were studied. Through the experimental study on antibacterial effect, contact time and concentration on the antimicrobial properties of the results showed that the antibacterial activity of GO in a certain range with the concentration of GO the increase in the concentration of 2000, g/m L, showed the most potent antibacterial activity of E.coli and S.aureus; GO inhibitory rate increased with time; were determined for E.coli and S.aureus's GO Small inhibitory concentration (MIC), the results showed that go on the antibacterial activity of E.coli is better than s.aureus. by dye adsorption experiment of go of methylene blue (MB) and Luo Danming B (RHB) results showed that the adsorption properties of go with adsorption than traditional activated carbon adsorbent can more excellent adsorption and initial concentration of go; dye on MB and RHB is associated with MB, the initial concentration of 200mg/l and RHB when the initial concentration is 300mg/l, large capacity go adsorption; adsorption kinetics showed that the adsorption behavior of the go with the pseudo two order kinetics model of.2. magnetic chitosan (MCS) on the function of go go-mcs magnetic composites synthesized by several test methods for characterization of the structure, morphology and properties. The antibacterial properties of go-mcs composites was studied through experimental results show that the antibacterial, antibacterial activity of go-mcs composite materials on E.coli and S.aureus is higher than that of single component go and MCS display The antibacterial properties were significantly improved. The adsorption properties of go-mcs composites, were investigated by the adsorption experiment results show that the go-mcs composite has more excellent performance than the go adsorption, adsorption capacity of MB and RHB were 258mg/g and 153mg/g; go-mcs MB and RHB pH on the best adsorption values in the vicinity of 5; adsorption kinetics the results showed that the adsorption behavior of go-mcs with the pseudo two order kinetics model, show that the adsorption rate of MB and RHB go-mcs controlled by chemical adsorption; magnetism testing results showed that go-mcs with superparamagnetism materials with magnetic Recyclable. In conclusion, go-mcs has excellent adsorption properties and antibacterial activity, can be used as a multifunctional the material, can remove dye pollutants in water, also can eliminate the harmful bacteria, and has good magnetic Recyclable.3. respectively using polyethylene glycol (PEG) and poly six methyl hydrochloride Guanidine (phgC) function of go go-peg-phgc composites were synthesized, and their structure, morphology and properties were characterized by.Go-peg-phgc composites maintain the lamellar structure of go, peg to avoid the introduction of go-peg-phgc composites by agglomeration. Experimental study on antibacterial antibacterial properties of go-peg-phgc E.coli and S.aureus two kinds of bacteria the results showed that good dispersion of go-peg-phgc than agglomerate go-phgc stronger antibacterial activity of.Go-peg-phgc composite materials show significantly enhanced the antibacterial properties of.4. with CS and phgC compound cs-phgc functional go, go-cs-phgc composites were synthesized, and using various testing method to characterize its structure, morphology and properties of.Go-cs-phgc the lamellar structure of go, the presence of CS go-cs-phgc composite material is not easy to agglomerate. The antibacterial effect of go-cs-phgc on E.coli and S.aureus two kinds of anti bacteria The performance of bacteria, antibacterial experiment results show that go-cs-phgc has a strong bactericidal effect, and the antibacterial activity of go-cs-phgc was higher than that of any single component (GO, CS, PHGC or CS-PHGC) antibacterial activity, antibacterial performance has been significantly enhanced. The experiment to further determine the GO-CS-PHGC value of MIC, GO-CS-PHGC composite materials on E.coli MIC value is 32 g/mL that was significantly lower than that of GO and CS-PHGC mixture, and GO, CS and PHGC, the MIC value of the mixture shows a simple superposition of antibacterial properties of GO-CS-PHGC composite are not components of antibacterial activity, but the synergistic effect between the components.

【学位授予单位】：吉林大学
【学位级别】：博士
【学位授予年份】：2017
【分类号】：O647.33;TB332

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