納米熒光探針的研究及應(yīng)用
發(fā)布時(shí)間：2018-11-09 20:45
【摘要】：納米熒光探針由于其尺寸與結(jié)構(gòu)的特殊性,表現(xiàn)出與宏觀物質(zhì)截然不同的理化性質(zhì),如小尺寸效應(yīng)、量子效應(yīng)、表面效應(yīng)與量子隧道效應(yīng)等,在醫(yī)療、科技、能源、軍事等領(lǐng)域具有廣闊的應(yīng)用前景。近年來(lái),將納米熒光探針應(yīng)用于化學(xué)傳感、生物醫(yī)學(xué)等領(lǐng)域一直是科學(xué)家研究的熱點(diǎn),其中最關(guān)鍵的是設(shè)計(jì)合成具有優(yōu)良性能的熒光納米材料,如粒徑均一、光學(xué)性質(zhì)穩(wěn)定、細(xì)胞毒性低、水溶性及生物相容性良好等。本論文采用簡(jiǎn)單一步法制得性能優(yōu)異的銀納米簇、碳點(diǎn)及其復(fù)合納米材料,并基于以上熒光納米材料構(gòu)建新的傳感平臺(tái),實(shí)現(xiàn)對(duì)S~(2-)、Fe~(3+)、Al~(3+)以及癌細(xì)胞的檢測(cè)。第一章:簡(jiǎn)述納米熒光探針的基本性能,對(duì)納米熒光探針(包括量子點(diǎn)、貴金屬納米簇、碳點(diǎn))的研究及應(yīng)用進(jìn)展進(jìn)行了綜述。第二章:常溫下,以溶菌酶(Lys)為穩(wěn)定劑,NaBH_4為還原劑,通過(guò)簡(jiǎn)單的一步法合成溶菌酶穩(wěn)定的銀納米簇(Lys-Ag NCs)�；赟~(2-)與Ag~+/Ag之間強(qiáng)烈的相互作用,S~(2-)可以顯著猝滅Lys-Ag NCs的熒光,進(jìn)而建立了一種高靈敏、高選擇性檢測(cè)S~(2-)的方法。該方法在5.0×10-6 M-1.0×10-4 M線性范圍內(nèi)對(duì)S~(2-)有良好的響應(yīng),對(duì)應(yīng)的檢出限為1.1×10-6M(S/N=3)。滿意的回收率結(jié)果(97.0-101.4%)表明該方法具有一定的可行性,可用于環(huán)境水樣中S~(2-)的檢測(cè)。此外,對(duì)S~(2-)與Lys-Ag NCs之間的作用機(jī)理也進(jìn)行了詳細(xì)地探討研究。第三章:以脯氨酸為碳源,乙二胺為氮源,通過(guò)簡(jiǎn)單的一步水熱法制備得到發(fā)藍(lán)色熒光的CDs。CDs表面的-NH2可以通過(guò)經(jīng)典的EDC/NHS反應(yīng)與葉酸(FA)表面的-COOH發(fā)生反應(yīng)生成CDs-FA復(fù)合物�；贔A與葉酸受體(FR)之間強(qiáng)烈的親和力以及FR介導(dǎo)的細(xì)胞內(nèi)吞作用,CDs-FA復(fù)合物可以特異性識(shí)別FR表達(dá)的癌細(xì)胞并對(duì)其完成熒光標(biāo)記,進(jìn)而將FR表達(dá)的癌細(xì)胞與FR不表達(dá)的正常細(xì)胞區(qū)分開(kāi)來(lái),這為癌癥的早期診斷與治療提供一定的依據(jù)。第四章:以環(huán)糊精為碳源,通過(guò)一步水熱法制得發(fā)藍(lán)色熒光的CDs。CDs表面豐富的羥基、環(huán)氧基等含氧基團(tuán)使得CDs不僅具有還原劑的特性,而且可以在納米簇的合成過(guò)程中充當(dāng)保護(hù)劑,基于此,將制得的CDs與Ag~+通過(guò)簡(jiǎn)單水熱法合成發(fā)綠色熒光的CDs-Ag NCs復(fù)合物。當(dāng)Fe~(3+)存在時(shí),該CDs-Ag NCs復(fù)合物的熒光發(fā)生猝滅,而當(dāng)Al~(3+)存在時(shí),該CDs-Ag NCs復(fù)合物的熒光得到增強(qiáng),由此,分別構(gòu)建了“斷開(kāi)式”Fe~(3+)傳感體系和“開(kāi)啟式”Al~(3+)傳感體系,兩個(gè)傳感體系對(duì)應(yīng)的線性范圍分別是5.0×10-6M-3.6×10-4M和2.0×10-5M-1.8×10-4M,檢出限分別為2.6×10-6M與4.8×10-7 M(S/N=3)。此外,兩者的回收率實(shí)驗(yàn)都取得了滿意的結(jié)果,表明該CDs-Ag NCs復(fù)合物在Fe~(3+)與Al~(3+)的分析檢測(cè)中具有很大的應(yīng)用潛力。第五章:對(duì)本論文中銀納米簇、碳點(diǎn)及其復(fù)合物作為熒光探針/標(biāo)記物,在離子檢測(cè)和靶向細(xì)胞成像方面的研究結(jié)果做了總結(jié),并對(duì)后續(xù)的工作進(jìn)行了展望。
[Abstract]:Because of the particularity of its size and structure, the nanoscale fluorescent probe has different physicochemical properties from macroscopical materials, such as small size effect, quantum effect, surface effect and quantum tunneling effect, etc., in medical treatment, science and technology, energy, etc. Military and other fields have broad application prospects. In recent years, the application of nano-fluorescent probes in chemical sensing, biomedicine and other fields has been the focus of scientists, the most important is the design and synthesis of fluorescent nanomaterials with excellent properties, such as uniform particle size, stable optical properties. Low cytotoxicity, good water solubility and biocompatibility. In this paper, silver nanoclusters, carbon dots and their composite nanomaterials with excellent performance were obtained by a simple one-step method. Based on the above fluorescent nanomaterials, a new sensing platform was constructed to realize the synthesis of S2-, Fe~ (3). Detection of Al~ (3) and cancer cells. In chapter 1, the basic properties of nano-fluorescent probes are reviewed. The research and application of nano-fluorescent probes (including quantum dots, noble metal nanoclusters and carbon dots) are reviewed. Chapter 2: under normal temperature, using lysozyme (Lys) as stabilizer and NaBH_4 as reducing agent, a simple one-step method was used to synthesize lysozyme stabilized silver nanoclusters (Lys-Ag NCs). Based on the strong interaction between S2- and Ag~ / Ag, S2- can significantly quench the fluorescence of Lys-Ag NCs and establish a highly sensitive and selective method for the detection of S2-. The method has a good response to S2- in the linear range of 5.0 脳 10-6 M-1.0 脳 10-4 M and the detection limit is 1.1 脳 10-6 M (S/N=3). The satisfactory recovery (97.0-101.4%) showed that the method was feasible and could be applied to the determination of S2- in environmental water samples. In addition, the interaction mechanism between S2- and Lys-Ag NCs is also studied in detail. Chapter III: proline as carbon source, ethylenediamine as nitrogen source, The-NH2 of the blue fluorescent CDs.CDs surface was prepared by a simple one step hydrothermal method. The CDs-FA complex can be formed by classical EDC/NHS reaction with-COOH on the (FA) surface of folate. Based on the strong affinity between FA and folate receptor (FR) and the intracellular endocytosis mediated by FR, the CDs-FA complex can specifically recognize and label FR expressed cancer cells. Furthermore, the FR expressed cancer cells were distinguished from the normal cells not expressed by FR, which provided a basis for the early diagnosis and treatment of cancer. Chapter 4: using cyclodextrin as carbon source, the blue fluorescent CDs.CDs surface with abundant hydroxyl, epoxy and other oxygen-containing groups can be prepared by one-step hydrothermal method, which makes CDs not only have the properties of reductant. And it can be used as a protective agent in the synthesis of nanoclusters. Based on this, CDs and Ag~ were synthesized by a simple hydrothermal method to synthesize green fluorescent CDs-Ag NCs complexes. In the presence of Fe~ (3), the fluorescence of the CDs-Ag NCs complex is quenched, and when Al~ (3) exists, the fluorescence of the CDs-Ag NCs complex is enhanced. The "open" Fe~ (3) sensing system and the "open" Al~ (3) sensing system are constructed respectively. The linear ranges of the two sensing systems are 5.0 脳 10-6M-3.6 脳 10-4M and 2.0 脳 10-5M-1.8 脳 10-4M, respectively. The detection limits were 2.6 脳 10 ~ (-6) M and 4.8 脳 10 ~ (-7) M (S/N=3), respectively. In addition, satisfactory results have been obtained in both the recovery experiments, indicating that the CDs-Ag NCs complex has great potential for application in the analysis and detection of Fe~ (3) and Al~ (3). Chapter 5: the research results of silver nanoclusters, carbon spots and their complexes as fluorescent probes / markers in this thesis are summarized in ion detection and targeted cell imaging, and the future work is prospected.
【學(xué)位授予單位】：山西大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O657.3
本文編號(hào)：2321514
[Abstract]:Because of the particularity of its size and structure, the nanoscale fluorescent probe has different physicochemical properties from macroscopical materials, such as small size effect, quantum effect, surface effect and quantum tunneling effect, etc., in medical treatment, science and technology, energy, etc. Military and other fields have broad application prospects. In recent years, the application of nano-fluorescent probes in chemical sensing, biomedicine and other fields has been the focus of scientists, the most important is the design and synthesis of fluorescent nanomaterials with excellent properties, such as uniform particle size, stable optical properties. Low cytotoxicity, good water solubility and biocompatibility. In this paper, silver nanoclusters, carbon dots and their composite nanomaterials with excellent performance were obtained by a simple one-step method. Based on the above fluorescent nanomaterials, a new sensing platform was constructed to realize the synthesis of S2-, Fe~ (3). Detection of Al~ (3) and cancer cells. In chapter 1, the basic properties of nano-fluorescent probes are reviewed. The research and application of nano-fluorescent probes (including quantum dots, noble metal nanoclusters and carbon dots) are reviewed. Chapter 2: under normal temperature, using lysozyme (Lys) as stabilizer and NaBH_4 as reducing agent, a simple one-step method was used to synthesize lysozyme stabilized silver nanoclusters (Lys-Ag NCs). Based on the strong interaction between S2- and Ag~ / Ag, S2- can significantly quench the fluorescence of Lys-Ag NCs and establish a highly sensitive and selective method for the detection of S2-. The method has a good response to S2- in the linear range of 5.0 脳 10-6 M-1.0 脳 10-4 M and the detection limit is 1.1 脳 10-6 M (S/N=3). The satisfactory recovery (97.0-101.4%) showed that the method was feasible and could be applied to the determination of S2- in environmental water samples. In addition, the interaction mechanism between S2- and Lys-Ag NCs is also studied in detail. Chapter III: proline as carbon source, ethylenediamine as nitrogen source, The-NH2 of the blue fluorescent CDs.CDs surface was prepared by a simple one step hydrothermal method. The CDs-FA complex can be formed by classical EDC/NHS reaction with-COOH on the (FA) surface of folate. Based on the strong affinity between FA and folate receptor (FR) and the intracellular endocytosis mediated by FR, the CDs-FA complex can specifically recognize and label FR expressed cancer cells. Furthermore, the FR expressed cancer cells were distinguished from the normal cells not expressed by FR, which provided a basis for the early diagnosis and treatment of cancer. Chapter 4: using cyclodextrin as carbon source, the blue fluorescent CDs.CDs surface with abundant hydroxyl, epoxy and other oxygen-containing groups can be prepared by one-step hydrothermal method, which makes CDs not only have the properties of reductant. And it can be used as a protective agent in the synthesis of nanoclusters. Based on this, CDs and Ag~ were synthesized by a simple hydrothermal method to synthesize green fluorescent CDs-Ag NCs complexes. In the presence of Fe~ (3), the fluorescence of the CDs-Ag NCs complex is quenched, and when Al~ (3) exists, the fluorescence of the CDs-Ag NCs complex is enhanced. The "open" Fe~ (3) sensing system and the "open" Al~ (3) sensing system are constructed respectively. The linear ranges of the two sensing systems are 5.0 脳 10-6M-3.6 脳 10-4M and 2.0 脳 10-5M-1.8 脳 10-4M, respectively. The detection limits were 2.6 脳 10 ~ (-6) M and 4.8 脳 10 ~ (-7) M (S/N=3), respectively. In addition, satisfactory results have been obtained in both the recovery experiments, indicating that the CDs-Ag NCs complex has great potential for application in the analysis and detection of Fe~ (3) and Al~ (3). Chapter 5: the research results of silver nanoclusters, carbon spots and their complexes as fluorescent probes / markers in this thesis are summarized in ion detection and targeted cell imaging, and the future work is prospected.
【學(xué)位授予單位】：山西大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O657.3
【參考文獻(xiàn)】
相關(guān)期刊論文 前2條
1 Taotao Li;Jingjing Yang;Zeeshan Ali;Zunliang Wang;Xianbo Mou;Nongyue He;Zhifei Wang;;Synthesis of aptamer-functionalized Ag nanoclusters for MCF-7 breast cancer cells imaging[J];Science China(Chemistry);2017年03期
2 方靜美;劉利芹;趙希娟;李原芳;;鋁離子與羥基功能化熒光碳點(diǎn)的相互作用[J];應(yīng)用化學(xué);2013年10期
，本文編號(hào)：2321514
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