發(fā)布時(shí)間：2018-11-24 12:29

【摘要】：海藻酸是一種天然高分子,主要由褐藻提取而來,具有優(yōu)異的生物相容性、生物粘附性和生物可降解性,在藥物控制、組織工程等生物醫(yī)學(xué)工程領(lǐng)域有應(yīng)用價(jià)值。但目前關(guān)于具有自修復(fù)功能的海藻酸水凝膠的研究并不多。對(duì)海藻酸水凝膠進(jìn)行自修復(fù)功能化,有助于其在藥物控釋等領(lǐng)域的運(yùn)用。而目前的自修復(fù)水凝膠,多傾向于利用材料本身分子結(jié)構(gòu)的特點(diǎn)完成修復(fù)過程,即基于“超分子作用”的自修復(fù)。本論文擬將氫鍵、主客體相互作用這兩種超分子作用自修復(fù)機(jī)制引入到海藻酸上,制備出具有自修復(fù)功能的海藻酸水凝膠。主要研究內(nèi)容及取得的結(jié)果如下:(1)制備了不同Bis交聯(lián)劑含量的聚6-丙烯酰胺基己酸(PA6ACA)水凝膠,測(cè)試并總結(jié)了交聯(lián)劑用量對(duì)水凝膠力學(xué)及自修復(fù)性能的影響,結(jié)果表明,隨交聯(lián)劑用量增加,水凝膠拉伸強(qiáng)度與模量增加,斷裂伸長率降低,自修復(fù)率降低。從修復(fù)界面間氫鍵強(qiáng)度與水凝膠主體強(qiáng)度兩個(gè)因素分析了測(cè)試結(jié)果。挑選出自修復(fù)性能較優(yōu)的配比,并將其應(yīng)用到海藻酸水凝膠中,成功制備出具有自修復(fù)功能的PA6ACA/海藻酸半互穿網(wǎng)絡(luò)水凝膠(PA6ACA/SA Semi-IPN水凝膠),同時(shí)也測(cè)試了交聯(lián)劑用量及海藻酸鈉濃度對(duì)半互穿網(wǎng)絡(luò)水凝膠力學(xué)及自修復(fù)性能的影響。(2)通過共價(jià)接枝的方式將PA6ACA高分子鏈與海藻酸鏈相結(jié)合,成功制備出具有自修復(fù)性能的海藻酸-接枝-PA6ACA水凝膠(SA-g-PA6ACA水凝膠),并考察了交聯(lián)密度對(duì)其自修復(fù)性能的影響。結(jié)果表明,交聯(lián)密度對(duì)SA-g-PA6ACA水凝膠的自修復(fù)性能影響很大,隨交聯(lián)密度增加,自修復(fù)效果迅速下降。同時(shí),對(duì)比了SA-g-PA6ACA水凝膠與PA6ACA/SA Semi-IPN水凝膠在力學(xué)與自修復(fù)性能方面的差異,并分析了接枝與半互穿兩種網(wǎng)絡(luò)結(jié)構(gòu)對(duì)這種差異的影響。(3)通過將β環(huán)糊精(β-CD)接枝于氧化海藻酸鈉(OSA)主鏈,將雙鍵金剛烷(Ad-AAm)與丙烯酰胺共聚,制備了基于β-CD與金剛烷主客體相互作用的水凝膠——OSA-g-β-CD/PAM-Ad水凝膠。并考察了其粘彈性、力學(xué)性能及自修復(fù)性能。流變實(shí)驗(yàn)結(jié)果表明,OSA-g-β-CD/PAM-Ad水凝膠內(nèi)部具有三維網(wǎng)絡(luò)結(jié)構(gòu),即β-CD與金剛烷間存在主客體相互作用,構(gòu)成了凝膠的交聯(lián)點(diǎn),使凝膠成型。自修復(fù)實(shí)驗(yàn)結(jié)果表明,水凝膠有較好的自修復(fù)效果(自修復(fù)率Rs為72%),競(jìng)爭(zhēng)實(shí)驗(yàn)證實(shí)了這種自修復(fù)行為是凝膠切面間主客體相互作用的結(jié)果。
[Abstract]:Alginic acid is a kind of natural polymer, which is mainly extracted from brown algae. It has excellent biocompatibility, bioadhesion and biodegradability. It has application value in biomedical engineering such as drug control, tissue engineering and so on. However, there are few studies on alginate hydrogels with self-repair function. The self-repair functionalization of alginate hydrogel is helpful for its application in drug controlled release. At present, the self-repairing hydrogels tend to use the molecular structure of the materials to complete the repair process, that is, self-repair based on "supramolecular interaction". In this thesis, two supramolecular self-repairing mechanisms, hydrogen bond and host-guest interaction, are introduced to alginic acid to prepare a self-repairing alginate hydrogel. The main results are as follows: (1) Poly (6-acrylamide caproic acid (PA6ACA) hydrogels with different Bis crosslinker contents were prepared, and the effects of crosslinking agent dosage on hydrogel mechanical and self-repairing properties were tested and summarized. The results showed that the tensile strength and modulus of the hydrogel increased, the elongation at break decreased and the self-repair rate decreased with the increase of the amount of crosslinking agent. The results were analyzed from two factors, hydrogen bond strength and hydrogel main strength. The self-repairing ratio of PA6ACA/ alginate hydrogel was selected and applied to alginate hydrogel. The self-repairing PA6ACA/ alginate semi-interpenetrating network hydrogel (PA6ACA/SA Semi-IPN hydrogel) was successfully prepared. At the same time, the effects of the amount of crosslinking agent and the concentration of sodium alginate on the mechanical and self-repairing properties of semi-interpenetrating network hydrogels were also tested. (2) the PA6ACA polymer chain was combined with alginate chain by covalent grafting. Alginic acid-grafted PA6ACA hydrogels (SA-g-PA6ACA hydrogels) with self-repairing properties were successfully prepared and the effects of crosslinking density on their self-repair properties were investigated. The results showed that the crosslinking density had a great effect on the self-repair properties of SA-g-PA6ACA hydrogels, and the self-repairing effect decreased rapidly with the increase of crosslinking density. At the same time, the mechanical and self-repairing properties of SA-g-PA6ACA hydrogel and PA6ACA/SA Semi-IPN hydrogel were compared. The influence of grafted and semi-interpenetrating networks on the difference was also analyzed. (3) by grafting 尾 -cyclodextrin (尾-CD) onto the main chain of sodium alginate oxide (OSA), the double bond adamantane (Ad-AAm) was copolymerized with acrylamide. A hydrogel OSA-g- 尾-CD/PAM-Ad hydrogel based on the interaction of 尾-CD and adamantane was prepared. The viscoelastic properties, mechanical properties and self-repairing properties were also investigated. The results of rheological experiments show that the OSA-g- 尾-CD/PAM-Ad hydrogel has a three-dimensional network structure, that is, there exists a host and guest interaction between 尾-CD and adamantane, which constitutes the crosslinking point of the gel and forms the gel. The results of self-repair experiments show that hydrogels have a good self-repair effect (self-repair rate Rs is 72%). The results of competitive experiments show that the self-repair behavior is the result of the interaction between the host and the host.
【學(xué)位授予單位】：華南理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2016
【分類號(hào)】：O648.17

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