發(fā)布時間：2018-06-23 13:06

  本文選題：熒光納米硅球 + 反相微乳液法��； 參考：《河北大學》2017年碩士論文

【摘要】：近幾年來,環(huán)境污染愈來愈嚴重,食品安全問題愈演愈烈,人類的健康受到嚴重威脅,新增癌癥病例逐年遞增,研發(fā)有效的檢測手段和抗癌方法已刻不容緩。隨著納米技術(shù)的發(fā)展,熒光納米材料在整個生物醫(yī)學領(lǐng)域的地位日益凸顯。為了滿足醫(yī)療技術(shù)的需要,熒光納米材料逐漸向著生物相容性好、熒光信號穩(wěn)定高效、特異性強、易功能化等方向發(fā)展。鑒于酸堿度對生物體生命活動的重要調(diào)控作用,以及生命現(xiàn)象的發(fā)生和細胞內(nèi)pH值的變化密切相關(guān),在眾多功能化熒光納米材料中,具有pH響應性的熒光納米硅球以其優(yōu)良的性能脫穎而出。由于pH響應性能不僅可以來自熒光染料本身,還可以通過pH響應性功能基團修飾獲得,因此,本文制備了兩種不同的熒光納米硅球,并對其在pH傳感器和藥物釋放等方面的應用進行了初步研究。本論文以異硫氰酸類熒光染料為熒光源,選用生物相容性良好且表面易修飾的硅膠為載體制備熒光納米硅球。首先綜述了熒光納米顆粒及pH響應性材料的分類、合成方法及潛在的應用前景,闡述了本文研究意義。利用硅烷偶聯(lián)劑γ-氨丙基三乙氧基硅烷(APTES)在其氨基與異硫氰根加成生成Schiff堿的同時,還能與TEOS發(fā)生水解縮合的特點,制備鍵合異硫氰酸熒光素(FITC)的熒光納米硅球。根據(jù)FITC在微球中位置的不同,熒光硅球?qū)⒂袃煞N結(jié)構(gòu)——包覆型(c-FSNs)與表面接枝型(s-FSNs)。對其性能進行比較分析發(fā)現(xiàn):與表面接枝型型相比,包覆型熒光硅球光漂白程度低,光穩(wěn)定性良好,其中,利用反相微乳液法(W/O)包硅制備的包覆型熒光納米硅球比St?ber法粒徑更小易控,熒光信號較強,且具有介孔結(jié)構(gòu),更利于生物醫(yī)藥等方面的應用。將c-FSNs作為pH傳感器研究,發(fā)現(xiàn)其響應迅速,熒光強度在pH 5.2-7.8內(nèi)幾乎呈線性增長,pKa約6.32,且具有良好的可逆性、重現(xiàn)性、準確性和生物相容性�；�于聚丙烯酸(PAA)具有pH響應性的特點,本文以RITC-APTES作熒光前驅(qū)體,采用W/O法合成鍵合異硫氰酸羅丹明B(RITC)的介孔熒光納米硅球(FMSNs),表面氨基化修飾后,經(jīng)過酰胺反應,連接PAA,制備具有pH響應性的熒光納米硅球(PAA-FMSNs),經(jīng)表征,制得的微球粒徑均一,約181 nm,分散性良好,孔徑16.6 nm,比表面積17.3 m2?g-1,生物相容性良好;接著,以鹽酸阿霉素(DOX)為模型藥物,研究PAA-FMSNs作為p H響應性納米藥物載體的能力,數(shù)據(jù)表明DOX∶PAA-FMSNs為1.5時,熒光納米硅球載體具有較高的包封率(94.5%)和載藥量(58.6%),且在pH 5.4-7.4的范圍內(nèi),隨pH的降低,藥物釋放率明顯升高,具有顯著的pH響應性。
[Abstract]:In recent years, environmental pollution has become more and more serious, food safety has become more and more serious, human health has been seriously threatened, new cases of cancer have been increasing year by year, it is urgent to develop effective detection methods and anticancer methods. With the development of nanotechnology, fluorescent nanomaterials play an increasingly important role in the field of biomedicine. In order to meet the needs of medical technology, fluorescent nanomaterials are developing towards good biocompatibility, stable and efficient fluorescent signals, strong specificity and easy functionalization. In view of the important regulation of pH on biological activity and the close relationship between the occurrence of life phenomena and the change of intracellular pH value, among the many functionalized fluorescent nanomaterials, Ph-responsive fluorescent nanocrystalline silica spheres stand out for their excellent properties. Since the pH response properties can be obtained not only from the fluorescent dyes themselves, but also through the modification of pH responsive functional groups, two kinds of fluorescent nanocrystals were prepared in this paper. Its application in pH sensor and drug release was studied. In this paper, fluorescent nanocrystalline silica spheres were prepared by using isothiocyanate dyes as fluorescent source and silica gel with good biocompatibility and easy surface modification. The classification, synthesis methods and potential application prospects of fluorescent nanoparticles and pH responsive materials are reviewed. Using silane coupling agent 緯 -aminopropyltriethoxysilane (APTES) to form Schiff base by addition of amino and iso-thiocyanate, the fluorescent nanospheres bonded with fluorescein isothiocyanate (FITC) were prepared by hydrolysis and condensation with TEOS. According to the position of FITC in microspheres, there will be two structure-cladding type (c-FSNs) and surface grafting type (s-FSNs). Compared with the surface grafting type, the coated fluorescent silicon sphere has low photobleaching degree and good photostability. The coated fluorescent nanocrystalline silica spheres prepared by the reverse microemulsion method (W / O) are smaller and easier to control than the Stouber method. The fluorescence signal is stronger and has mesoporous structure, which is more suitable for biomedical applications. Using c-FSNs as pH sensor, it was found that the response of c-FSNs was rapid, and the fluorescence intensity increased linearly about 6.32 in pH 5.2-7.8, and had good reversibility, reproducibility, accuracy and biocompatibility. Based on the pH response of polyacrylic acid (PAA), a mesoporous fluorescent nanospheres (FMSNs) bonded with Rhodamine isothiocyanate B (RITC) were synthesized by W / O method using RITC-APTES as fluorescence precursor. The fluorescent nanospheres (PAA-FMSNs) with pH response were prepared by linking PAA. The microspheres were characterized by uniform particle size, about 181 nm, good dispersibility, good pore size 16.6 nm, specific surface area 17.3 m2 路g -1, good biocompatibility, and doxorubicin hydrochloride (DOX) as the model drug. The ability of PAA-FMSNs as pH responsive nano-drug carrier was studied. The results showed that when DOX: PAA-FMSNs was 1.5, the encapsulation efficiency (94.5%) and drug loading (58.6%) of fluorescent silica nanoparticles were higher, and the pH value decreased with pH 5.4-7.4, and the results showed that PAA-FMSNs had high encapsulation efficiency (94.5%) and drug loading (58.6%) when DOX: PAA-FMSNs was 1.5. The drug release rate was significantly increased, and had significant pH response.
【學位授予單位】：河北大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：O613.72;TB383.1

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