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  本文選題：放射狀褶皺結(jié)構(gòu) + 介孔氧化硅��； 參考：《深圳大學(xué)》2015年碩士論文

【摘要】：納米銀具有很強(qiáng)的吸附性,表面能和化學(xué)活性,可吸附細(xì)菌使其失去活性而死亡。但是,隨著尺寸的減小,納米銀在實(shí)際應(yīng)用中分散性差、緩釋過快、且不易保存,將銀納米粒子(Ag NPs)均勻負(fù)載到結(jié)構(gòu)更為穩(wěn)定的無機(jī)納米載體上,預(yù)計能順利解決上述難題。介孔氧化硅材料生物相容性好、比表面積大,化學(xué)修飾性和穩(wěn)定性較好,在催化,藥物控釋,基因治療等領(lǐng)域應(yīng)用廣泛。本文利用原位化學(xué)還原將Ag NPs負(fù)載到具有豐富管道的放射狀褶皺結(jié)構(gòu)介孔二氧化硅材料內(nèi)外表面。這種新型結(jié)構(gòu)介孔二氧化硅的負(fù)載性、容納性及可修飾性優(yōu)于傳統(tǒng)介孔氧化硅。首先,向外開放的放射狀結(jié)構(gòu)能讓各種尺寸的客體通過并進(jìn)入到內(nèi)層,利于銀納米粒子的負(fù)載,增強(qiáng)納米銀的分散穩(wěn)定性能,并保證了單位體積內(nèi)納米Ag的密集分布。同時,Si O2球殼對鑲嵌在其內(nèi)表面上的納米Ag起到保護(hù)作用,降低其消耗速度。最后,多重尺度介孔的協(xié)同結(jié)合將在納米Ag逸出抗菌性能中充當(dāng)緩釋基體,延長所得納米抗菌劑的使用壽命。本文的主要實(shí)驗(yàn)路線是以分別修飾有巰基、氨基以及羧基活性基團(tuán)的放射狀褶皺結(jié)構(gòu)介孔氧化硅為載體,利用官能團(tuán)與Ag+的結(jié)合能力,有效調(diào)控介孔氧化硅內(nèi)外表面的銀離子濃度以及分布。接著,通過對吸附的銀離子進(jìn)行原位還原,即可制得載銀納米介孔二氧化硅材料。最后,我們對此材料的抗菌性能進(jìn)行了詳細(xì)的表征,具體工作分為以下幾個部分:(1)放射狀褶皺結(jié)構(gòu)介孔氧化硅載體的制備及表征。堿性環(huán)境下,以十六烷基三甲基溴化銨(CTAB)為模板劑,正硅酸乙酯(TEOS)和3-巰丙基三甲氧基硅烷(MPS)為硅源,乙醚為增溶劑,室溫條件下采用溶膠-凝膠法改變MPS添加量,合成一系列具有放射狀褶皺結(jié)構(gòu)的介孔氧化硅。其中,MPS/TEOS體積比=0.08時所得樣品形貌規(guī)整,粒徑均一,約為100 nm左右,比表面積可達(dá)696.59 m2/g;(2)對以上制得的巰基改性介孔氧化硅進(jìn)行磺化處理,利用靜電作用吸附Ag+,將其固定在介孔氧化硅整個表面,再將其原位還原。所得納米Ag在介孔氧化硅表面分布密集且均勻,粒徑只有3~5 nm,無團(tuán)聚現(xiàn)象,對大腸桿菌和金黃色葡萄球菌均表現(xiàn)出優(yōu)異的抗菌性。樣品對大腸桿菌的MIC為36.55 mg/L,MBC為48.55 mg/L,對金黃色葡萄球菌的最小抑菌濃度(MIC)為73.10 mg/L,MBC為97.10 mg/L,其中銀的負(fù)載量僅8.32%;(3)制備氨基、羧基改性放射狀褶皺介孔氧化硅,利用氨基和羧基的配位能力吸附Ag+,固定其在介孔氧化硅表面的分布,再原位將Ag+還原成Ag NPs,有效解決了Ag NPs易團(tuán)聚問題。測試結(jié)果表明:Ag NP@Si O2-NH2中納米Ag顆粒分布密集均勻,粒徑約10nm,而Ag NP@Si O2-COOH中納米Ag分布稀疏,粒徑較大,約20~30 nm。N-Ag對大腸桿菌和金黃色葡萄球菌的抗菌能力均遠(yuǎn)勝于C-Ag的抗菌能力。
[Abstract]:Silver nanoparticles have strong adsorbability, surface energy and chemical activity. However, with the decrease of size, the dispersion of silver nanoparticles in practical applications is poor, the slow release is too fast, and it is not easy to preserve. It is expected that the above problems can be solved by loading silver nanoparticles with Ag NPs evenly onto inorganic nano-carriers with more stable structure. Mesoporous silica materials have good biocompatibility, large specific surface area, good chemical modification and stability, and are widely used in catalysis, drug controlled release, gene therapy and so on. In this paper, Ag NPs were loaded into the inner and outer surfaces of porous silica materials with radial fold structure with abundant pipes by in situ chemical reduction. This new type of mesoporous silica is superior to traditional mesoporous silica in its load-carrying, accommodative and modifiable properties. Firstly, the radial structure which is open to the outside can make the objects of various sizes pass through and enter the inner layer, which is favorable to the loading of silver nanoparticles, enhance the dispersion and stability of silver nanoparticles, and ensure the dense distribution of nano-Ag in unit volume. At the same time, the spherical shell of SiO2 can protect the nano-Ag embedded on its inner surface and reduce its consumption speed. Finally, the synergistic combination of multi-scale mesoporous will act as the slow-release matrix in the antibacterial properties of nano-Ag escape, and prolong the service life of the prepared nano-antibacterial agent. In this paper, the main experimental route is to utilize the binding ability of functional groups to Ag by using mesoporous silicon oxide with radial fold structure modified with sulfhydryl, amino and carboxyl active groups, respectively. The concentration and distribution of silver ions on the inner and outer surfaces of mesoporous silica were effectively regulated. Then, the silver loaded nano mesoporous silica material can be prepared by in situ reduction of the adsorbed silver ions. Finally, the antibacterial properties of this material were characterized in detail. The specific work was divided into the following parts: 1) preparation and characterization of mesoporous silicon oxide carrier with radial fold structure. In alkaline environment, cetyltrimethylammonium bromide (CTAB) as template, tetraethyl orthosilicate (TEOS) and 3-mercaptopropyltrimethoxysilane (MPS) as silicon source, ether as solvent, and sol-gel method were used to change the amount of MPs at room temperature. A series of mesoporous silicon oxide with radial fold structure was synthesized. When the volume ratio of MPS / TEOS was 0.08, the sample was uniform in shape, about 100nm in size, with a specific surface area of 696.59 m2 / g ~ (-2). The sulfhydryl modified mesoporous silica was sulfonated, and Ag was adsorbed by electrostatic interaction. It is immobilized on the whole surface of mesoporous silica and then reduced in situ. The nanocrystalline Ag was distributed densely and uniformly on the surface of mesoporous silica with a particle size of only 3 ~ 5 nm without agglomeration. It showed excellent antibacterial activity against Escherichia coli and Staphylococcus aureus. The MIC of the sample to Escherichia coli was 36.55 mg / L MBC was 48.55 mg / L, and the minimum inhibitory concentration to Staphylococcus aureus was 73.10 mg / L MBC = 97.10 mg / L, in which the loading amount of silver was only 8.32 mg / L) to prepare amino, carboxyl modified radial fold mesoporous silicon oxide. Using the coordination ability of amino and carboxyl groups to adsorb Ag, to fix the distribution of Ag on mesoporous silica surface, and then to reduce Ag in situ to Ag NPs, which effectively solves the agglomeration problem of Ag NPs. The results showed that the distribution of nano-Ag particles was dense and uniform, and the particle size was about 10nmm. the distribution of nano-Ag in Ag NPSiO2-COOH was sparse and the size of nano-Ag was larger. The antibacterial ability of about 200.30nm.N-Ag against Escherichia coli and Staphylococcus aureus was much better than that of C-Ag.
【學(xué)位授予單位】：深圳大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TQ131.22;TB383.1

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