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  本文選題：非共價鍵鍵合膠束　切入點：自組裝　出處：《鄭州大學》2015年碩士論文　論文類型：學位論文

【摘要】：在高分子學領域,我們采用自組裝法可以獲得形態(tài)和結構各異的兩親性高分子膠束,同時賦予它們優(yōu)良的生物相容性、親水性等特點。當這種兩親性膠束呈現空心結構時,它的內腔可以包覆大量的藥物、疏水性聚合物等,在藥物傳輸、材料改性等方面應用廣泛。目前,基于非共價鍵鍵合膠束法(NCCM)制備聚合物納米膠束的方法簡單易操作,且可通過改變交聯劑用量、聚合物摩爾比等得到不同尺寸的膠束。而在諸多的非共價鍵鍵合體系中,相較于其他驅動力,氫鍵的作用力強,方向性好,有利于形成穩(wěn)定膠束;且通過氫鍵連接的聚合物膠束,其核-殼結構無需特殊溶劑降解內核,改變溶劑狀態(tài)即可。因此基于氫鍵的自組裝體系在化學和生物體系中都占據非常重要的位置。本論文研究的主要內容是制備基于氫鍵作用的聚合物納米膠束,并探究交聯劑用量、溶劑等對膠束制備的影響。論文的具體工作可分為如下兩個部分:1、首先合成了端羧基化的聚苯乙烯(PS-COOH)和線性多嵌段聚醚胺(PEA),然后基于此構建NCCM體系,在水相中成功制備PS/PEA核-殼膠束,經甲醛交聯固定核-殼結構后,切換溶劑至二甲基甲酰胺(DMF)獲得PEA納米膠束。并進一步探究PS和PEA的滴加順序,PS和PEA的摩爾比,甲醛用量,DMF用量對膠束結構和尺寸的影響。經動態(tài)光散射(DLS)測試,交聯后的膠粒尺寸由98.40nm減小至75.85nm,證明膠束的殼結構被成功鎖住;經空穴化處理后,膠粒尺寸又增加至113.70nm。探究實驗結果分析可知,反向滴加制備的膠束尺寸為93.46nm,明顯減小;其他條件下,用量適當增有利于得到尺寸更大的膠束,但超過一定的范圍后,膠束尺寸反而減小。證明制備條件及體系各組份用量的改變會影響聚合物膠束的形狀和尺寸。2、首先合成了接枝共聚物PEO-g-P4VP,同種條件下在硝基甲烷(CH3NO2)溶液中制備PS/PEO-g-P4VP膠束,經二溴丁烷交聯固定后切換溶劑至DMF空穴化得到PEO-g-P4VP納米膠束。并進一步探究PS和PEO-g-P4VP的滴加順序,不同摩爾比的PS和PEO-g-P4VP,二溴丁烷用量,DMF用量對膠束形成或空穴化的影響。經DLS測試,我們得到尺寸為143.21nm的PEO-g-P4VP納米膠束,分散指數(PDI)為0.226,說明其具有較好的分散性。反向滴加得到117.40nm的膠束,其他條件如摩爾比、二溴丁烷及DMF用量的改變等均進一步驗證了第一個體系的結論。
[Abstract]:In the field of macromolecule science, we can obtain amphiphilic micelles with different morphology and structure by self-assembly method, and give them excellent biocompatibility and hydrophilicity, etc. When the amphiphilic micelles show hollow structure, Its inner cavity can be coated with a large number of drugs, hydrophobic polymers, etc. It is widely used in drug transport, material modification, etc. At present, the method of preparing polymer nano-micelles based on non-covalent bonding micelles is simple and easy to operate. Different sizes of micelles can be obtained by changing the amount of crosslinking agent and the molar ratio of polymer. In many non-covalent bonding systems, the hydrogen bonding force is stronger and the direction is good than other driving forces, which is conducive to the formation of stable micelles. The core-shell structure of the polymer micelles connected by hydrogen bond does not require special solvent to degrade the core. Therefore, the self-assembly system based on hydrogen bond occupies a very important position in both chemical and biological systems. The effects of crosslinking agent and solvent on the preparation of micelles were investigated. The specific work of this paper can be divided into two parts: 1. The carboxyl terminated polystyrene (PS-COOH) and linear multiblock polyether amine (PEAA) were synthesized, and then the NCCM system was constructed. PS/PEA core-shell micelles were successfully prepared in water phase. After crosslinking and fixing the core-shell structure by formaldehyde, the PEA nanomeres were obtained by switching solvent to dimethylformamide. The molar ratio of PS and PEA was further investigated. The effect of the amount of formaldehyde and DMF on the structure and size of the micelles was studied by DLSs. The size of the crosslinked micelles was reduced from 98.40 nm to 75.85 nm, which proved that the shell structure of the micelles was successfully locked up, and the structure of the micelles was treated by hole treatment. The size of micelle was increased to 113.70 nm. The results of the experiment showed that the size of micelle prepared by reverse dropping was 93.46 nm, which was obviously reduced. Under other conditions, the micelle with larger size was obtained by proper increase of dosage, but beyond a certain range. It was proved that the shape and size of polymer micelles would be affected by the changes of the preparation conditions and the amount of each component in the system. Firstly, the graft copolymer PEO-g-P4VPwas synthesized, and the PS/PEO-g-P4VP micelles were prepared in nitromethane Ch _ 3NO _ 2 solution under the same conditions. The PEO-g-P4VP nanomicelles were prepared by dibromobutane crosslinking immobilization by switching solvents to DMF cavitation. The dropping order of PS and PEO-g-P4VP was further investigated. The effects of PS, PEO-g-P4VPand dibromobutane on the micelle formation or cavitation of PS and PEO-g-P4VP at different molar ratios. By DLS, we obtained the PEO-g-P4VP nanomicelles with the size of 143.21 nm. The dispersion index (PDI) is 0.226, which indicates that it has good dispersion. The micelle of 117.40 nm is obtained by reverse dropping. The conclusion of the first system is further verified by the other conditions, such as molar ratio, dibromobutane and the change of the amount of DMF.
【學位授予單位】：鄭州大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：TB383.1;O648.1

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1 向曉曉;基于氫鍵自組裝作用的PEA和PEO-g-P4VP納米膠束的制備[D];鄭州大學;2015年

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本文編號：1632003