聚N-異丙基丙烯酰胺基高強度水凝膠的制備及性能研究
發(fā)布時間：2019-04-23 19:37
【摘要】：水凝膠作為一種功能高分子材料,由于具有高吸水性、良好的生物相容性和刺激響應(yīng)能力,被廣泛應(yīng)用于生物組織工程、藥物控制釋放、廢水處理、化學機械器件、生活用品等領(lǐng)域。傳統(tǒng)水凝膠響應(yīng)速率慢、易碎等缺點嚴重限制了水凝膠的應(yīng)用范圍。因此提高水凝膠的響應(yīng)速率和力學性能成為該領(lǐng)域的研究熱點。本文以N-異丙基丙烯酰胺基水凝膠為主要研究對象,采用不同的改性手段,通過添加無機粒子、加入制孔劑、引進互穿網(wǎng)絡(luò)結(jié)構(gòu)等方式,分別合成出納米復(fù)合凝膠、多孔結(jié)構(gòu)水凝膠和互穿網(wǎng)絡(luò)水凝膠,研究了新型水凝膠的溶脹性能和力學性能等。本論文主要研究內(nèi)容如下:1.采用自由基溶液聚合法,將帶C=C的籠型倍半硅氧烷(MAPOSS)加入N-異丙基丙烯酰胺(NIPAM)單體中,聚乙二醇二丙烯酸酯(PEGDA)充當交聯(lián)劑的作用,制備POSS改性P(NIPAM-co-PEGDA)的納米復(fù)合水凝膠。水凝膠的壓縮強度隨MAPOSS和PEGDA的增加而顯著提升,當體系中MAPOSS和PEGDA的含量達到最大時,水凝膠的壓縮強度達到368.32 kPa,這主要是因為MAPOSS固有的剛性籠型結(jié)構(gòu)增加了聚合物分子鏈的硬度,PEGDA的增多能夠提高體系的交聯(lián)密度。此外,MAPOSS的增加和PEGDA的減少均能提升水凝膠的退溶脹率,當體系中MAPOSS含量最多、PEGDA含量最少時,水凝膠在30min內(nèi)的失水率為60.7%,退溶脹速率最快。2.以聚乙二醇(PEG)為制孔劑,加入到經(jīng)過無機粒子改性的P(NIPAM-coMAPOSS)水凝膠中,考察制孔劑對多孔結(jié)構(gòu)水凝膠的影響。不含PEG的水凝膠幾乎看不出孔洞結(jié)構(gòu);當PEG含量達到0.3g時,水凝膠的孔結(jié)構(gòu)十分明顯。PEG的加入有助于孔洞的產(chǎn)生,而且平均孔徑隨PEG含量的增加而增大。隨著PEG的增加,水凝膠的壓縮模量呈現(xiàn)先增大后減小的趨勢,當PEG含量為0.1g時,水凝膠的力學性能最好。水凝膠的退溶脹率隨PEG含量的增加而增大,這是因為除去的制孔劑為水分子的散失提供了通道,使水凝膠的退溶脹率明顯提高。以5-氟尿嘧啶(5-FU)為模型藥物的緩釋實驗表明,可以通過調(diào)整PEG的含量,控制水凝膠對藥物的釋放。3.通過化學交聯(lián)反應(yīng)和互穿網(wǎng)絡(luò)技術(shù),將聚乙烯吡絡(luò)烷酮(PVP)引入到P(NIPAM-co-AA)水凝膠網(wǎng)絡(luò)結(jié)構(gòu)中,制備出具有溫度/pH雙重敏感性的P(NIPAM-co-AA)/PVP互穿網(wǎng)絡(luò)結(jié)構(gòu)水凝膠。紅外光譜圖和差示掃描圖像證明了水凝膠中互穿網(wǎng)絡(luò)結(jié)構(gòu)的形成。與未加入PVP的水凝膠相比,PVP含量為0.1g時水凝膠的熔融溫度有了小幅度提高,達到215°C。當水凝膠應(yīng)變?yōu)?0%時,未加入PVP的水凝膠的壓縮模量為0.24 MPa,而PVP含量為0.1g的水凝膠的壓縮模量提高到0.36 MPa,證明了互穿網(wǎng)絡(luò)結(jié)構(gòu)的形成有助于提高水凝膠的力學性能。以5-FU為模型藥物,PVP含量為0.1g的水凝膠的持續(xù)釋藥時間達到9小時以上,累積釋藥率達到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 擄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%.
【學位授予單位】：吉林大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TQ427.26
本文編號：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 擄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%.
【學位授予單位】：吉林大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：TQ427.26
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