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丝素蛋白纳微米颗粒的制备及在抗菌功能织物中的应用

Preparation and Applications of Silk Fibroin Nano-and Microparticles for Antibacterial Functional Fabrics

【作者】 陈浩;

【导师】 王晓沁;

【作者基本信息】 苏州大学 , 纺织工程(专业学位), 2021, 硕士

【摘要】 抗菌是一个十分广泛的概念,包括灭菌、防霉、消毒、抑菌、防腐等行为,一般是指通过化学或物理方法起到杀死细菌或抑制细菌增长的过程。而传统的纤维及织物通常对微生物及其代谢产物没有清除能力,在合适的温度、湿度及一定的养分条件下,微生物会迅速繁殖,因此,对织物进行抗菌整理十分重要。目前,许多织物采用抗菌剂改性,但这些抗菌剂大多存在着抗菌性不稳定及毒性高的问题。考虑到抗菌织物应同时具备强抗菌性和良好的生物安全性,将具有高抗菌能力的无机抗菌材料与绿色有机载体复合是解决上述问题的重要手段,而采用无毒绿色的可降解纳米粒子作为载体负载无机抗菌剂则更适合应用于织物抗菌。本文以蚕丝提取的丝素蛋白为材料制备纳米或微米尺寸颗粒,通过吸附搭载抗菌剂,并将此复合抗菌颗粒应用于织物,在不改变织物服用性能的同时,赋予织物稳定的抗菌性能,之后将抗菌颗粒应用于空气过滤膜布,改善了膜布的过滤效率及抗菌性。首先,采用PEG冻融法和乳化沉淀法制备了丝素蛋白纳微米颗粒,分析了丝素蛋白浓度、PEG添加量、PEG分子量对纳米颗粒粒径的影响;将纳微米颗粒作为载体搭载抗菌剂,对抗菌颗粒的粒径、Zeta电位、二级结构、抗菌性、生物安全性进行表征。结果表明,丝素蛋白浓度为3%,PEG浓度为50%,PEG分子量为600 Da时,制备的纳米颗粒粒径最小(157.6±8.8 nm)。纳微米颗粒搭载抗菌剂后,Ag-NPS的抗菌性较Ag-MPS更强,浓度为100 μg/mL时对大肠杆菌抑制率大于99.9%。Cu-NPS-150同时具备良好的生物安全性和抗菌性,浓度为100μg/mL时,24 h后的细胞活力为75.21±4.32%,抑菌率大于 99.9%。然后,与交联剂配合使用将不同浓度抗菌颗粒固定在织物样品及对照品纤维表面,并对改性前后织物的透气性、回潮率、力学性能、表面形貌、二级结构、EDS元素分析进行测试,而后利用细胞实验、细菌实验对织物的生物安全性及抗菌性进行评估,其中,利用100μg/mL Cu-NPS-150改性的织物48 h后细胞活力比空白对照高14%,说明抗菌颗粒改性后织物的生物安全性有所提高,Cu-NPS浓度为1 mg/mL时,制备的织物生物安全性与改性前相比无差异,水洗十次后,依然具有良好的抗菌性,抑菌圈宽度为2.41±0.14 mm。最后,将不同粒径的抗菌颗粒应用于空气过滤膜布,研究改性前后膜布的过滤阻力与过滤效率,分析抗菌颗粒改性前后膜布的生物安全性及抗菌性能变化。结果表明改性后膜布能够有效吸附并杀死细菌,同时在不增加过滤阻力的情况下改性膜布的过滤效率有所提升,其中,采用浓度为100 ug/mL 150 nm Cu-NPS改性的膜布过滤效率相比未改性膜布提升18%,并对大肠杆菌的生长起到完全抑制作用。综上所述,本课题研制了丝素蛋白抗菌纳微米颗粒并将其应用于织物改性。结果表明,改性后的织物具有良好的抗菌性和生物安全性,并且过滤膜布改性后过滤效率与抗菌性都有显著提升,为开发绿色环保、高效安全的织物和空气过滤膜布提供新思路和新方法。

【Abstract】 Antibacterial is a very broad concept,generally referring to the process of killing bacteria or inhibiting the growth of bacteria through chemical or physical methods including sterilization,anti-mold,disinfection,antibacterial,antiseptic and other behaviors.Traditional fibers and fabrics usually have no ability to remove microorganisms and their metabolites,and they are actually good media for nourishing microorganisms.Under suitable temperature,humidity and certain nutrient conditions,microorganisms will multiply rapidly in the porous fabric.Therefore,it is very important to carry out antibacterial finishing of fabrics.At present,many fabrics are modified with antibacterial agents,but most of these antibacterial agents have problems of unstable antibacterial properties and high toxicity.Considering that antibacterial fabrics should have both strong antibacterial properties and good biological safety,the combination of inorganic antibacterial reagents with high antibacterial ability and green organic carriers is an ideal solution for the above problems.Nano-and microparticles made from biodegradable polymers are suitable carriers for this purpose.In this paper,silk fibroin protein extracted from silkworm cocoons was used to prepare nano-and microparticles and encapsulate antibacterial reagents,and the antibacterial particles obtained were used to functionalize fabrics by immobilization on the fibers.The fabric was endowed with stable antibacterial properties without changing its wearability.Furthermore,the application of antibacterial particles to the air filtration cloth not only conferred antibacterial properties,but also improved the filtration efficiency of the cloth.First,the silk fibroin nano-and microparticles were prepared by the PEG-assisted freeze-thaw method and the emulsification precipitation method,and the effects of the silk fibroin concentration,amount of PEG added,and PEG molecular weights on the particle size were determined.The nano-/microparticles were then mixed and soaked with antibacterial agents,and the particle size,zeta potential,silk secondary structure,antibacterial properties,and biological safety of the antibacterial particles were examined.The results showed that when the concentration of silk fibroin was 3%,the concentration of PEG was 50%,and the molecular weight of PEG was 600 Da,the nanoparticles had the smallest particle size(157.6±8.8 nm).The silver ion-loaded nanoparticles(Ag-NPS)had stronger antibacterial activity than the silver ion-loaded microparticles(Ag-MPS),and the inhibition rate of E.coli was greater than 99.9%at a particle concentration of 100μg/mL.Compared to silver,copper ion loaded nanoparticle(Cu-NPS-150)showed both good biosafety and antibacterial activity,as the cell viability after 24 h was 75.21±4.32%,and the antibacterial rate was greater than 99.9%at a concentration of 100μg/mL.Then,using chemical crosslinking agents,antibacterial particles at different concentrations were immobilized on the surface of the fabric,and material properties like gas permeability,resiliency,mechanical strength,surface morphology,silk secondary structure,element components,etc.,before and after modification were analyzed.Furthermore,cytotoxicity and antibacterial activity of the functionalized fabric were assessed by culturing mammalian cells and bacteria on the fabric,respectively.The results showed that the cell viability 100μg/ml Cu-NPS-150 modified fabric was 14%higher than the blank control,indicating the biosafety of the fabric was improved after the surface modification with antibacterial particles.When the Cu-NPS concentration was 1 mg/ml,the cytotoxicity of the functionalized fabric had no difference from the blank fabric,and the antibacterial activity of the fabric remained high even after ten times washing,with the antibacterial ring width detected of 2.41±0.14 mm.Finally,the antibacterial particles with different particle sizes were immobilized on the air filtration cloth,and material properties including filtration resistance,filtration efficiency,cytotoxicity and antibacterial performance of the cloth before and after the modification were examined.The results showed that the modified cloth could effectively adsorb and kill bacteria,and the filtration efficiency of the cloth was improved without influencing the filtration resistance.The filtration efficiency of the cloth modified with 100 ug/mL 150 nm Cu-NPS increased by 18%when compared with the unmodified cloth,and it can completely inhibit the growth of E.coli attached to the cloth.In summary,silk fibroin antibacterial nano-and microparticles were successfully prepared and used to functionalize fabric in this study.The results showed that the modified fabric has good antibacterial properties and biological safety,and the filtration efficiency and antibacterial properties of the modified filter cloth were significantly improved,which provides a useful tool for the development of green,environmentally friendly,efficient and safe fabrics and air filter membranes.

  • 【网络出版投稿人】 苏州大学
  • 【网络出版年期】2023年 04期
  • 【分类号】TS195.5
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