本文選題：二氧化碳刺激響應(yīng)性聚合物　切入點(diǎn)：納米球形聚電解質(zhì)刷　出處：《華東理工大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：二氧化碳作為一種新型的刺激源,不僅具有無(wú)毒易除去等特點(diǎn),還是高等有機(jī)體新陳代謝的主要產(chǎn)物之一,同時(shí)兼具很好的生物相容性,因此研究具有二氧化碳刺激響應(yīng)性的聚合物成為目前的研究熱點(diǎn)之一。納米球形聚電解質(zhì)刷是由球形聚合物乳液微粒以及接枝在其表面的線形聚電解質(zhì)鏈所組成的一種核-殼結(jié)構(gòu)的納米粒子,通過(guò)在表面接枝不同的高分子鏈,進(jìn)而可以達(dá)到球形聚電解質(zhì)刷的功能化,因此它在基礎(chǔ)研究或工業(yè)應(yīng)用方面均有著不俗的表現(xiàn)。本工作的主要內(nèi)容是制備具有pH、鹽離子濃度、溫度以及二氧化碳的多重刺激響應(yīng)性的球形聚甲基丙烯酸N,N-二甲基氨基乙酯刷(PS-DMAEMA),研究它對(duì)各種環(huán)境刺激響應(yīng)性以及它用于蛋白質(zhì)"吸附—脫附"過(guò)程的綠色可逆性。除此之外,還將PS-PDMAEMA作為對(duì)二氧化碳刺激響應(yīng)的粒子用于穩(wěn)定Pickering乳液,并使用二氧化碳調(diào)節(jié)其刺激響應(yīng)性。本文的主要工作和相應(yīng)的研究結(jié)論如下:(1)利用光乳液聚合法合成納米球形聚電解質(zhì)刷:以聚苯乙烯(PS)作為球核,接枝帶有叔胺基團(tuán)的聚甲基丙烯酸N,N-二甲基氨基乙酯(DMAEMA)鏈,研究該納米粒子PS-PDMAEMA在水相中的pH、鹽離子和溫度的多重敏感性;并且,將PS-PDMAEMA用于固載牛血清蛋白(BSA),使用動(dòng)態(tài)光散射(DLS)、zeta電位、濁度以及等溫量熱儀(ITC)進(jìn)行吸附效果的表征。研究表明PS-PDMAEMA是一種很好的蛋白質(zhì)載體,具有很強(qiáng)的吸附能力,并且可以通過(guò)pH、鹽離子和溫度調(diào)節(jié)聚合物刷的粒徑尺寸以及對(duì)蛋白質(zhì)的吸附效果。(2)在前面的工作基礎(chǔ)上,繼續(xù)研究了球刷PS-PDMAEMA對(duì)二氧化碳的刺激響應(yīng)性以及對(duì)蛋白質(zhì)的可逆"吸附-脫附"過(guò)程:在PS-PDMAMEA體系中通入二氧化碳后,可以使得PDMAEMA鏈質(zhì)子化,呈現(xiàn)舒展的狀態(tài),球刷的粒徑變大,隨后,通入惰性氣體(如氮?dú)饣蚝?后,PDAMEAM鏈去質(zhì)子化,分子鏈?zhǔn)湛s,粒徑會(huì)回復(fù)至初始狀態(tài),經(jīng)過(guò)多次可逆循環(huán)后仍能保持該性質(zhì)并且也不會(huì)給體系留下任何多余的組分,因此,以"氮?dú)?二氧化碳"作為開關(guān),可以實(shí)現(xiàn)PS-PDMAEMA對(duì)蛋白質(zhì)的可逆"吸附-脫附",結(jié)果表明該過(guò)程對(duì)蛋白質(zhì)的生物活性影響很小,也不會(huì)產(chǎn)生鹽離子濃度的積累。因此,可將其作為蛋白質(zhì)的載體,完成蛋白質(zhì)的分離和富集。(3)Pickering乳液是一類將固體顆粒作為穩(wěn)定劑吸附于油水兩個(gè)不相容的界面上并形成穩(wěn)定的乳液。PS-PDMAEMA作為Pickering乳液的一種可二氧化碳調(diào)控的乳化劑:該乳化劑(PS-PDMAEMA)可使用pH、二氧化碳/氮?dú)庹{(diào)節(jié)其乳化能力。本文分別從PS-PDMAEMA的濃度、體系的pH值探討了該乳化劑的乳化效果,在光學(xué)顯微鏡的研究表明:當(dāng)PS-PDMAEMA作為乳化劑時(shí),需要達(dá)到一定的濃度才可以得到穩(wěn)定的乳液,體系的pH會(huì)嚴(yán)重影響乳液的穩(wěn)定性,pH過(guò)低會(huì)使得乳液發(fā)生破乳現(xiàn)象。除此之外,該乳化劑還可以使用二氧化碳/氮?dú)饪赡嬲{(diào)控其乳化性能。
[Abstract]:As a new stimulant, carbon dioxide is not only nontoxic and easy to remove, but also one of the main metabolites of higher organisms, and also has good biocompatibility. Therefore, the study of carbon dioxide responsive polymers has become one of the research hotspots. Nano-spherical polyelectrolyte brushes are composed of spherical polymer emulsion particles and linear polyelectrolyte chains grafted on their surface. Of a core-shell structure, The functionalization of spherical polyelectrolyte brushes can be achieved by grafting different polymer chains on the surface, so it has a good performance in basic research and industrial application. The main content of this work is the preparation of pH, salt ion concentration, PS-DMAEMAMAA, a spherical polyN-dimethylaminoethyl methacrylate brushes with multiple stimuli response to temperature and carbon dioxide, to study its response to various environmental stimuli and its green reversibility for protein "adsorption-desorption" processes. PS-PDMAEMA was also used to stabilize the Pickering emulsion as a particle responsive to carbon dioxide stimulation. In this paper, the main work and corresponding conclusions are as follows: the photoemulsion polymerization method is used to synthesize nano-spherical polyelectrolyte brushes: PS) is used as the spherical nucleus. Grafted poly (N-dimethyl aminoethyl methacrylate) chain with tertiary amine group was used to study the pH, salt ion and temperature sensitivity of the PS-PDMAEMA nanoparticles in aqueous phase. PS-PDMAEMA was used to immobilize bovine serum protein (BSA). The adsorption effect of BSA was characterized by dynamic light scattering (DLS), turbidity and isothermal calorimeter. The results show that PS-PDMAEMA is a good protein carrier and has strong adsorption ability. In addition, the particle size of polymer brush and the adsorption effect of protein can be adjusted by pH, salt ion and temperature on the basis of the previous work. The reactivity of PS-PDMAEMA to carbon dioxide and the reversible "adsorption-desorption" process of protein were studied. When carbon dioxide was added into the PS-PDMAMEA system, the PDMAEMA chain could be protonated, showing a stretch state, and the particle size of the spheroidal brush became larger. Subsequently, the PDAMEAM chain is deprotonated with inert gas (such as nitrogen or helium), the molecular chain shrinks, the particle size returns to its initial state, and the property remains after several reversible cycles without leaving any extra components in the system. Therefore, using "nitrogen / carbon dioxide" as switch can realize the reversible "adsorption-desorption" of protein by PS-PDMAEMA. The results show that the process has little effect on the biological activity of protein and does not result in the accumulation of salt ion concentration. They can be used as carriers of proteins, Complete protein separation and enrichment. Pickering emulsion is a kind of stable emulsion. PS-PDMAEMA is a kind of Pickering emulsion which adsorbs solid particles as stabilizer on the interface of oil and water and forms stable emulsion. PS-PDMAEMA is a kind of emulsifier that can be controlled by carbon dioxide in Pickering emulsion. The emulsifier PS-PDMAEMAA can use pH, carbon dioxide / nitrogen to adjust its emulsifying ability. The emulsifying effect of the emulsifier was discussed by pH value of the system. The results of optical microscope showed that when PS-PDMAEMA was used as emulsifier, a stable emulsion could be obtained only when the emulsifier reached a certain concentration. The pH of the emulsion will seriously affect the stability of the emulsion. Too low pH will lead to the emulsion demulsification. In addition, the emulsifier can be used to control the emulsifying performance of the emulsion by using carbon dioxide / nitrogen.
【學(xué)位授予單位】：華東理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O631;TB383.1

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