聚N-异丙基丙烯酰胺基高强度水凝胶的制备及性能研究
发布时间：2019-04-23 19:37
【摘要】：水凝胶作为一种功能高分子材料,由于具有高吸水性、良好的生物相容性和刺激响应能力,被广泛应用于生物组织工程、药物控制释放、废水处理、化学机械器件、生活用品等领域。传统水凝胶响应速率慢、易碎等缺点严重限制了水凝胶的应用范围。因此提高水凝胶的响应速率和力学性能成为该领域的研究热点。本文以N-异丙基丙烯酰胺基水凝胶为主要研究对象,采用不同的改性手段,通过添加无机粒子、加入制孔剂、引进互穿网络结构等方式,分别合成出纳米复合凝胶、多孔结构水凝胶和互穿网络水凝胶,研究了新型水凝胶的溶胀性能和力学性能等。本论文主要研究内容如下:1.采用自由基溶液聚合法,将带C=C的笼型倍半硅氧烷(MAPOSS)加入N-异丙基丙烯酰胺(NIPAM)单体中,聚乙二醇二丙烯酸酯(PEGDA)充当交联剂的作用,制备POSS改性P(NIPAM-co-PEGDA)的纳米复合水凝胶。水凝胶的压缩强度随MAPOSS和PEGDA的增加而显著提升,当体系中MAPOSS和PEGDA的含量达到最大时,水凝胶的压缩强度达到368.32 kPa,这主要是因为MAPOSS固有的刚性笼型结构增加了聚合物分子链的硬度,PEGDA的增多能够提高体系的交联密度。此外,MAPOSS的增加和PEGDA的减少均能提升水凝胶的退溶胀率,当体系中MAPOSS含量最多、PEGDA含量最少时,水凝胶在30min内的失水率为60.7%,退溶胀速率最快。2.以聚乙二醇(PEG)为制孔剂,加入到经过无机粒子改性的P(NIPAM-coMAPOSS)水凝胶中,考察制孔剂对多孔结构水凝胶的影响。不含PEG的水凝胶几乎看不出孔洞结构;当PEG含量达到0.3g时,水凝胶的孔结构十分明显。PEG的加入有助于孔洞的产生,而且平均孔径随PEG含量的增加而增大。随着PEG的增加,水凝胶的压缩模量呈现先增大后减小的趋势,当PEG含量为0.1g时,水凝胶的力学性能最好。水凝胶的退溶胀率随PEG含量的增加而增大,这是因为除去的制孔剂为水分子的散失提供了通道,使水凝胶的退溶胀率明显提高。以5-氟尿嘧啶(5-FU)为模型药物的缓释实验表明,可以通过调整PEG的含量,控制水凝胶对药物的释放。3.通过化学交联反应和互穿网络技术,将聚乙烯吡络烷酮(PVP)引入到P(NIPAM-co-AA)水凝胶网络结构中,制备出具有温度/pH双重敏感性的P(NIPAM-co-AA)/PVP互穿网络结构水凝胶。红外光谱图和差示扫描图像证明了水凝胶中互穿网络结构的形成。与未加入PVP的水凝胶相比,PVP含量为0.1g时水凝胶的熔融温度有了小幅度提高,达到215°C。当水凝胶应变为20%时,未加入PVP的水凝胶的压缩模量为0.24 MPa,而PVP含量为0.1g的水凝胶的压缩模量提高到0.36 MPa,证明了互穿网络结构的形成有助于提高水凝胶的力学性能。以5-FU为模型药物,PVP含量为0.1g的水凝胶的持续释药时间达到9小时以上,累积释药率达到84.5%。
[Abstract]:As a kind of functional polymer material, hydrogel is widely used in biological tissue engineering, drug controlled release, wastewater treatment, chemical and mechanical devices due to its high water absorption, good biocompatibility and stimulation response. Areas such as household goods. The disadvantages of traditional hydrogels, such as slow response rate and fragility, seriously limit the application range of hydrogels. Therefore, improving the response rate and mechanical properties of hydrogels has become a hot topic in this field. In this paper, N-isopropylacrylamide hydrogel was used as the main research object, nano-composite gel was synthesized by adding inorganic particles, adding pore-making agent, introducing interpenetrating network structure and so on, by means of different modification methods, such as adding inorganic particles, adding pore-making agent, introducing interpenetrating network structure, etc. Porous hydrogels and interpenetrating network hydrogels were used to study the swelling and mechanical properties of the new hydrogels. The main contents of this thesis are as follows: 1. The cage silsesquioxane (MAPOSS) with C C was added into N-isopropylacrylamide (NIPAM) monomer by free radical solution polymerization. Polyethylene glycol diacrylate (PEGDA) was used as cross-linking agent. POSS modified P (NIPAM-co-PEGDA) nanocomposite hydrogels were prepared. The compressive strength of hydrogels increased significantly with the increase of MAPOSS and PEGDA. When the contents of MAPOSS and PEGDA reached the maximum, the compressive strength of hydrogels reached 368.32 kPa,. The main reason is that the inherent rigid cage structure of MAPOSS increases the hardness of polymer molecular chain, and the increase of PEGDA can improve the crosslinking density of the system. In addition, both the increase of MAPOSS and the decrease of PEGDA can increase the swelling ratio of hydrogel. When the content of MAPOSS is the highest and the content of PEGDA is the least, the water loss rate of hydrogel in 30min is 60.7%, and the rate of deswelling is the fastest. Polyethylene glycol (PEG) was added to P (NIPAM-coMAPOSS) hydrogel modified by inorganic particles, and the effect of pore-making agent on porous structure hydrogel was investigated. When the content of PEG is 0.3g, the pore structure of hydrogel is very obvious. The addition of PEG is helpful to the formation of pores, and the average pore size increases with the increase of PEG content. With the increase of PEG, the compressive modulus of hydrogels increases first and then decreases. When the content of PEG is 0.1g, the mechanical properties of hydrogels are the best. The swelling ratio of hydrogel increases with the increase of PEG content because the removed pore-making agent provides a channel for the loss of water molecules and increases the swelling rate of hydrogel obviously. The sustained release experiment with 5-fluorouracil (5-FU) as model drug showed that the release of 5-fluorouracil (PEG) could be controlled by adjusting the content of 5-fluorouracil (PEG). Polyvinylpyrrolidone (PVP) was introduced into the network structure of P (NIPAM-co-AA) hydrogel by chemical crosslinking reaction and interpenetrating network technique. P (NIPAM-co-AA) / pH interpenetrating hydrogels with temperature / PVP double sensitivity were prepared. Infrared spectra and differential scanning images demonstrate the formation of interpenetrating network structure in hydrogels. Compared with the hydrogels without adding PVP, the melting temperature of the hydrogels increased slightly to 215 掳C. when the content of PVP was 0.1g, the melting temperature of the hydrogels was increased to 215C. When the strain of hydrogel is 20%, the compressive modulus of hydrogel without adding PVP is 0.24 MPa, and that of hydrogel containing 0.1g PVP is 0.36 MPa,. It is proved that the formation of interpenetrating network structure is helpful to improve the mechanical properties of hydrogels. With 5-FU as model drug, the sustained release time of hydrogel with 0.1g PVP content was over 9 hours, and the cumulative release rate was 84.5%.
【学位授予单位】：吉林大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TQ427.26
本文编号：2463740
[Abstract]:As a kind of functional polymer material, hydrogel is widely used in biological tissue engineering, drug controlled release, wastewater treatment, chemical and mechanical devices due to its high water absorption, good biocompatibility and stimulation response. Areas such as household goods. The disadvantages of traditional hydrogels, such as slow response rate and fragility, seriously limit the application range of hydrogels. Therefore, improving the response rate and mechanical properties of hydrogels has become a hot topic in this field. In this paper, N-isopropylacrylamide hydrogel was used as the main research object, nano-composite gel was synthesized by adding inorganic particles, adding pore-making agent, introducing interpenetrating network structure and so on, by means of different modification methods, such as adding inorganic particles, adding pore-making agent, introducing interpenetrating network structure, etc. Porous hydrogels and interpenetrating network hydrogels were used to study the swelling and mechanical properties of the new hydrogels. The main contents of this thesis are as follows: 1. The cage silsesquioxane (MAPOSS) with C C was added into N-isopropylacrylamide (NIPAM) monomer by free radical solution polymerization. Polyethylene glycol diacrylate (PEGDA) was used as cross-linking agent. POSS modified P (NIPAM-co-PEGDA) nanocomposite hydrogels were prepared. The compressive strength of hydrogels increased significantly with the increase of MAPOSS and PEGDA. When the contents of MAPOSS and PEGDA reached the maximum, the compressive strength of hydrogels reached 368.32 kPa,. The main reason is that the inherent rigid cage structure of MAPOSS increases the hardness of polymer molecular chain, and the increase of PEGDA can improve the crosslinking density of the system. In addition, both the increase of MAPOSS and the decrease of PEGDA can increase the swelling ratio of hydrogel. When the content of MAPOSS is the highest and the content of PEGDA is the least, the water loss rate of hydrogel in 30min is 60.7%, and the rate of deswelling is the fastest. Polyethylene glycol (PEG) was added to P (NIPAM-coMAPOSS) hydrogel modified by inorganic particles, and the effect of pore-making agent on porous structure hydrogel was investigated. When the content of PEG is 0.3g, the pore structure of hydrogel is very obvious. The addition of PEG is helpful to the formation of pores, and the average pore size increases with the increase of PEG content. With the increase of PEG, the compressive modulus of hydrogels increases first and then decreases. When the content of PEG is 0.1g, the mechanical properties of hydrogels are the best. The swelling ratio of hydrogel increases with the increase of PEG content because the removed pore-making agent provides a channel for the loss of water molecules and increases the swelling rate of hydrogel obviously. The sustained release experiment with 5-fluorouracil (5-FU) as model drug showed that the release of 5-fluorouracil (PEG) could be controlled by adjusting the content of 5-fluorouracil (PEG). Polyvinylpyrrolidone (PVP) was introduced into the network structure of P (NIPAM-co-AA) hydrogel by chemical crosslinking reaction and interpenetrating network technique. P (NIPAM-co-AA) / pH interpenetrating hydrogels with temperature / PVP double sensitivity were prepared. Infrared spectra and differential scanning images demonstrate the formation of interpenetrating network structure in hydrogels. Compared with the hydrogels without adding PVP, the melting temperature of the hydrogels increased slightly to 215 掳C. when the content of PVP was 0.1g, the melting temperature of the hydrogels was increased to 215C. When the strain of hydrogel is 20%, the compressive modulus of hydrogel without adding PVP is 0.24 MPa, and that of hydrogel containing 0.1g PVP is 0.36 MPa,. It is proved that the formation of interpenetrating network structure is helpful to improve the mechanical properties of hydrogels. With 5-FU as model drug, the sustained release time of hydrogel with 0.1g PVP content was over 9 hours, and the cumulative release rate was 84.5%.
【学位授予单位】：吉林大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TQ427.26
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