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透明质酸钠-胶原肽荷载生育酚微乳凝胶制备与性能研究

Preparation and Properties of Microemulsion Gels with Sodium Hyaluronate-collagen Peptides and Tocopherol

【作者】 王艳;

【导师】 曾庆祝;

【作者基本信息】 广州大学 , 材料与化工(专业学位), 2024, 硕士

【摘要】 透明质酸钠(sodium hyaluronate,SH)是一种多糖,由双糖作为基本单位构成,它是公认的保水能力最强的成分,被广泛应用于化妆品、保健食品中;胶原蛋白肽(collagen peptides,CP)是胶原蛋白在酶的作用下水解后的产物,具有丰富的羟脯氨酸,有多种生物活性,如抗氧化性、保湿等多种功能;α-生育酚(α-tocopherol)作为维生素E中的一种,具有很强的抗氧化性,但是由于其易氧化与脂溶性的特点,它在各种领域的应用受到了很大的限制。将SH与CP交联后制备的凝胶性能更好,将其作为凝胶基质制备微乳凝胶并荷载α-生育酚,其透皮率、抗氧化、抗炎性、保湿性等多种活性均提高。本论文以不同分子量的CP与SH为原料制备了水凝胶,并将其作为凝胶基质制备了负载α-生育酚的微乳凝胶改善了α-生育酚易氧化的缺点,探究了水凝胶的性能与微乳凝胶的透皮率及其生物活性。研究结果如下:(1)通过酸提法从罗非鱼鱼皮中提取出胶原蛋白,将胶原蛋白在木瓜蛋白酶的作用下水解成CP,利用超滤获得了不同分子量的胶原蛋白肽(CP1、CP2、CP3、CP4)。将不同分子量的CP与改性后不同分子量的SH(GMSH1、GMSH2、GMSH3、GMSH4)在紫外光下交联形成水凝胶,结果为:与CP交联后形成的水凝胶的性能均比单独以GMSH制备成的水凝胶性能要好;GMSH4无法与CP成胶,GMSH1、GMSH2、GMSH3与CP形成的水凝胶中,GMSH分子量越大,制备成的水凝胶性能越好,而CP对水凝胶的性能影响不大。(2)微乳及微乳凝胶的制备与表征。通过观察微乳溶液离心后的分层情况及其透明度,选定了吐温-80(T-80)与蓖麻油聚氧乙烯醚(EL-40)作为研究的表面活性剂,利用伪三元相图技术,分析确定表面活性剂与助表面活性剂之间的最适配比为4:1,以保证微乳体系的稳定性;肉豆蔻酸异丙酯(IPM)作为微乳的油相与混合表面活性剂的最佳比例为1:9;对微乳测定电导率,当体系中水的体积分数小于22%时,电导率较小,在22%-60%之间时,体系的电导率直线上升,为60-67%时,电导率缓慢上升至最大值,本文制备的微乳水体积分数为70%,为O/W型微乳,并经过染色进一步确认了微乳的类型;通过对水体积分数分别为50%、60%、70%的微乳进行FT-IR测定观察了微乳中水分子的状态分别为游离水、自由水和结合水;将微乳在经过离心、冻融循环、冷热循环与室温储藏等操作后测定粒径,发现微乳粒径均在9-15nm之间,且非常稳定;将α-生育酚溶解于IPM并与混合表面活性剂混合后逐滴滴加CP与GMSH预交联后的溶液,在紫外光下成胶制备微乳凝胶。(3)测定以不同分子量GMSH与CP为凝胶基质制备的微乳凝胶中荷载的α-生育酚发现,凝胶基质中GMSH的分子量越大,其附载的α-生育酚的溶出率是越小的;通过体外透皮实验发现微乳凝胶中α-生育酚的透皮率均比微乳中α-生育酚的透皮率大,且含量为0.5%的α-生育酚的微乳(17.00%)与微乳凝胶(46.67%)的透皮率是最大的;微乳凝胶水相中CP与SH的分子量越小,透皮率越高,<3k Da的CP透皮率最高,达到56.78%,且凝胶基质中GMSH的分子量越大,CP与SH的透皮率就越大。与CP交联后微乳凝胶的抗氧化性、抗炎性、保湿性、抗菌性均提高。

【Abstract】 Sodium hyaluronate(SH)is a polysaccharide,consisting of disaccharide units.It is recognized as an ingredient with strong water retention ability,widely used in cosmetics and health foods.Collagen peptides(CP),a product of enzymatically hydrolyzed collagen,are rich in hydroxyproline and exhibit various biological activities,including antioxidant and moisturizing functions.α-Tocopherol,a form of vitamin E,has strong antioxidant properties.However,its susceptibility to oxidation and fat solubility greatly limit its application in various fields.The gel prepared by cross-linking SH and CP exhibits improved properties,such as enhanced stability and bioactivity.This gel is used as a matrix to prepare a microemulsion gel,which is then loaded with α-tocopherol.It exhibits various properties,including skin permeability,antioxidant,anti-inflammatory,and moisturizing effects.As a result,the biological activity of the gel has been improved.This paper prepared hydrogels using CP and SH of different molecular weights as raw materials and used them as a gel matrix to prepare α-tocopherol-loaded microemulsion gels.This approach improved the stability of α-tocopherol,addressing its tendency to oxidize easily,and explored the water-related properties,the transdermal penetration rate of the microemulsion gel,and its biological activity.The research results are as follows:Extract collagen from tilapia skin through acid extraction,hydrolyze the collagen into CP under the action of papain,and use ultrafiltration to obtain collagen peptides of different molecular weights(CP1,CP2,CP3,CP4).CP of different molecular weights and modified SH(GMSH1,GMSH2,GMSH3,GMSH4)of different molecular weights were cross-linked under ultraviolet light to form hydrogels.The results show that the hydrogels formed after cross-linking with CP have better properties than those prepared with GMSH alone;GMSH4cannot gel with CP.Among the hydrogels formed by GMSH1,GMSH2,GMSH3,and CP,the greater the molecular weight of GMSH,the better the performance of the hydrogel,while the molecular weight of CP has little effect on the performance of the hydrogels.(2)Preparation and characterization of microemulsions and microemulsion gels.By observing the stratification and transparency of the microemulsion solution after centrifugation,Tween-80(T-80)and castor oil polyoxyethylene ether(EL-40)were selected as the surfactants for research,using pseudo-ternary Phase diagram technology,analysis determined that the optimal ratio between surfactant and co-surfactant is 4:1 to ensure the stability of the microemulsion system;isopropyl myristate(IPM)is used as the oil phase of the microemulsion The optimal ratio to the mixed surfactant is 1:9;measure the conductivity of the microemulsion.When the volume fraction of water in the system is less than 22%,the conductivity is small.When it is between 22% and 60%,the conductivity of the system is The conductivity rises linearly.When it is 60-67%,the conductivity slowly rises to the maximum value.The water volume fraction of the microemulsion prepared in this article is 70%,which is an O/W type microemulsion.The type of microemulsion was further confirmed by dyeing.;By conducting FT-IR measurements on microemulsions with water volume fractions of 50%,60%,and 70%,the states of water molecules in the microemulsions were observed as free water,free water,and bound water;the microemulsions were centrifuged,freeze-thaw cycle,hot and cold cycle and room temperature storage,etc.,the particle size was measured and it was found that the particle size of the microemulsion was between 9-15 nm and very stable;dissolve α-tocopherol in IPM and mix it with the mixed surfactant Finally,the pre-crosslinked solution of CP and GMSH is added dropwise,and gelled under UV light to prepare a microemulsion gel.(3)The determination of α-tocopherol loaded in microemulsion gels,prepared with GMSH and CP of varying molecular weights as the gel matrix,revealed that the higher the molecular weight of GMSH in the gel matrix,the slower the dissolution rate of the associatedα-tocopherol.In vitro transdermal experiments showed that the dermal penetration rate ofα-tocopherol in the microemulsion gel was higher than that in the microemulsion alone,although the α-tocopherol content at 0.5% was slightly lower than that in the microemulsion gel.The transdermal rates of emulsions and microemulsion gels were found to be the highest;whereas,the transdermal rates of CP and SH in the aqueous phase of the microemulsion gel were lower than those of α-tocopherol in the oil phase.The lower molecular weight CP and SH exhibited higher transdermal rates,with larger GMSH molecular weights in the gel matrix increasing the transdermal rates of CP and SH.The antioxidant,anti-inflammatory,moisturizing,and antibacterial properties of the microemulsion gel were enhanced after cross-linking with CP.

  • 【网络出版投稿人】 广州大学
  • 【网络出版年期】2025年 03期
  • 【分类号】TQ427.26
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