本文選題：納米材料 + 核苷酸　； 參考：《中國科學(xué)院研究生院（上海應(yīng)用物理研究所）》2015年博士論文

【摘要】：納米生物材料領(lǐng)域是納米科學(xué)中的一個(gè)核心領(lǐng)域，其技術(shù)的發(fā)展引發(fā)著新型材料的制造以及生物醫(yī)學(xué)領(lǐng)域的蓬勃發(fā)展。納米生物技術(shù)通過將生物分子連接到納米材料上，可以將納米材料的優(yōu)良特性及生物分子的識(shí)別能力結(jié)合在一起，構(gòu)建出多種新型的功能性材料，在生物傳感、藥物傳遞及靶向治療、材料科學(xué)及DNA納米技術(shù)等方面都有重要的應(yīng)用。該領(lǐng)域的關(guān)鍵問題之一是如何更有效地將生物分子（如DNA、蛋白質(zhì)等）與納米材料進(jìn)行連接，并且在此過程中仍很好地保持生物分子的活性，形成高效的分子識(shí)別界面。研究生物分子在納米界面上的反應(yīng)活性對(duì)于更好發(fā)揮生物納米材料的性能有著重要的意義。本論文的研究工作主要包括DNA在納米界面上反應(yīng)活性的系統(tǒng)研究以及新型的DNA功能化納米結(jié)構(gòu)體系的構(gòu)建。主要內(nèi)容如下： （1）基于課題組之前發(fā)展的新型嵌段DNA-納米金偶聯(lián)體制備方法，構(gòu)建了一系列密度和構(gòu)型可控的DNA-納米金偶聯(lián)體,并以此為基礎(chǔ)對(duì)DNA在納米界面上分子識(shí)別的熱力學(xué)和動(dòng)力學(xué)等物理化學(xué)性質(zhì)及生物分子活性進(jìn)行深入的探討和分析，研究了DNA自組裝方法、DNA分子的構(gòu)型及組裝密度等如何影響DNA在納米界面上的穩(wěn)定性和分子識(shí)別過程的反應(yīng)活性，建立理論模型。和傳統(tǒng)的巰基化學(xué)修飾方法相比，雙嵌段寡聚核苷酸DNA-納米金體系獨(dú)立調(diào)控DNA在納米金表面上的密度而不影響其構(gòu)型，因此所制備的DNA-納米金偶聯(lián)體非常適合作為模型證實(shí)、修正和闡釋DNA在納米界面上分子識(shí)別的物理化學(xué)性質(zhì)，用于單因素調(diào)節(jié)分析，有望為生物納米體系的構(gòu)建提供理論基礎(chǔ)。 （2）在雙嵌段DNA-納米金體系中，將DNA酶（DNAzyme）作為功能嵌段，構(gòu)建了一系列組裝密度和形貌可控的DNAzyme-AuNPs復(fù)合物，對(duì)DNAzyme在納米金上的反應(yīng)活性進(jìn)行研究。DNAzyme的組裝密度可以通過改變poly A的長度來調(diào)節(jié)，我們比較了納米金界面上不同組裝密度的雙嵌段DNAzyme和通過巰基自組裝的DNAzyme對(duì)鉛離子的響應(yīng)能力以及酶的催化能力，并與均相溶液體系進(jìn)行了比較。這項(xiàng)研究對(duì)8-17DNAzyme在納米金表面的催化過程和作用機(jī)制進(jìn)行了更為系統(tǒng)的研究，可能為生物傳感提供一個(gè)活性更高、特異性更好的酶催化平臺(tái)。 （3）利用胞嘧啶堿基與納米銀之間的吸附能力，發(fā)展了一種新的組裝納米銀-寡聚核苷酸復(fù)合探針的方法。這種方法通過富含胞嘧啶的序列將DNA自組裝于納米銀上，自組裝得到的復(fù)合探針在含鹽及高溫環(huán)境下仍能保持穩(wěn)定，并且通過這種方法組裝的探針在表面上擁有比巰基方法組裝的探針更好的分子識(shí)別能力。此外，我們可以通過改變胞嘧啶堿基的個(gè)數(shù)調(diào)節(jié)寡聚核苷酸在納米銀上的組裝密度，提高納米銀-DNA復(fù)合探針的穩(wěn)定性。這種組裝方法無需對(duì)寡聚核苷酸進(jìn)行修飾，降低了自組裝的成本且易于操作。所組裝的復(fù)合探針具備優(yōu)良的光學(xué)特性，可能在光學(xué)及生物傳感領(lǐng)域具有很大的應(yīng)用潛力。 （4）提出了一種制備納米尺度花狀結(jié)構(gòu)的超微金電極的新方法。將微米級(jí)碳纖維進(jìn)行火焰刻蝕至納米級(jí)，在其表面進(jìn)行電化學(xué)沉積電泳漆，，加熱烘烤處理后，通過電化學(xué)沉積納米金得到納米花狀超微金電極。掃描電鏡結(jié)果表明該方法可以得到尺寸在100μm左右，表面花刺在納米級(jí)別的納米花狀超微金電極。通過將納米花狀超微金電極與核酸適體技術(shù)及電化學(xué)檢測技術(shù)相結(jié)合，開發(fā)了一種基于核酸適體構(gòu)象變化的超微電極傳感器。將其應(yīng)用于生物分子（如可卡因）的檢測中，響應(yīng)速度快，特異性好。該體系有望應(yīng)用于單細(xì)胞及其他微環(huán)境中生物活性分子的檢測中。
[Abstract]:The field of nanoscale materials is a core field in nanoscience. The development of its technology leads to the development of new materials and the flourishing development of biomedicine. By connecting biological molecules to nanomaterials, nanotechnology can combine the excellent characteristics of nanomaterials and the recognition ability of biomolecules. A variety of new functional materials have been constructed, which have important applications in biosensing, drug delivery and targeting therapy, material science and DNA nanotechnology. One of the key issues in this field is how to effectively connect biomolecules (such as DNA, protein, etc.) with nanomaterials, and remains well maintained in this process. The activity of biomolecules can form an efficient molecular recognition interface. It is of great significance to study the reactive activity of biomolecules on the nano interface for better performance of the properties of biological nanomaterials. The research work of this paper mainly includes the systematic study of the reactive activity of DNA on the nano interface and the new DNA functionalized nanostructure The main content of the system is as follows:
(1) based on the new block DNA- nano Au couple preparation method developed before the project group, a series of DNA- nanoscale conjugates with controllable density and configuration are constructed, and on this basis, the thermodynamic and kinetic properties of the molecular recognition of DNA at the nano interface and the biological and molecular activity are deeply discussed and analyzed. The DNA self-assembly method, the configuration and the assembly density of DNA molecules affect the stability of DNA at the nano interface and the reaction activity of the molecular recognition process, and establish a theoretical model. Compared with the traditional sulfhydryl chemical modification method, the diblock oligonucleotide DNA- nanoscale system independently regulates the density of DNA on the surface of gold nanoparticles. As a result, the prepared DNA- nanoscale coupling is very suitable as a model to confirm the physical and chemical properties of the molecular recognition of DNA at the nano interface. It is expected to provide a theoretical basis for the construction of the biological nano system.
(2) in the double block DNA- nanoscale gold system, DNA enzyme (DNAzyme) is used as a functional block. A series of DNAzyme-AuNPs complexes with controlled assembly density and morphology are constructed. The reaction activity of DNAzyme on gold nanoparticles can be studied by changing the length of poly A. We compare the nano gold interface. The response ability of DNAzyme with different assembly density and the ability to respond to lead ions by the self assembled DNAzyme by mercapto, and the catalytic ability of the enzyme, are compared with the homogeneous solution system. This study has carried out a more systematic study on the catalytic process and mechanism of 8-17DNAzyme on the surface of gold nanoparticles, which may provide a biological sensing method. An enzyme catalyzed platform with higher activity and better specificity.
(3) a new method of assembling the nano silver oligonucleotide probe was developed by using the adsorption capacity between the cytosine base and the silver nanoparticles. This method is self-assembled on the nano silver through the sequence rich in cytosine, and the self assembled composite probe can remain stable in the salt and high temperature environment, and through this method, DNA can be maintained by this method. In addition, we can adjust the density of oligodeoxynucleotides on nano silver by changing the number of cytosine bases to improve the stability of the nano silver -DNA composite probe. This assembly method does not need to repair oligonucleotides. It reduces the cost of self-assembly and is easy to operate. The assembled probe has excellent optical properties, and may have great potential in the field of optical and biological sensing.
(4) a new method of preparing nano scale flower like ultragold electrode was proposed. The micrometer carbon fiber was etched to nanoscale by flame etching to nanoscale, electroelectrophoretic coatings were deposited on its surface. After heating and baking, nano flower like ultragold electrode was obtained by electrochemical deposition of nano gold. The results of scanning electron microscopy showed that this method could be used. A nano flower like ultramicro gold electrode was obtained on the surface with a size of about 100 m. The nano flower like ultragold electrode was inserted at the nano scale. A super microelectrode sensor based on the conformational change of nucleic acid was developed by combining the nano flower like ultramicro gold electrode with the aptamer technique and electrochemical detection technology. It should be used for the detection of biomolecules (such as cocaine). This system is expected to be applied to the detection of bioactive molecules in single cells and other microenvironments.
【學(xué)位授予單位】：中國科學(xué)院研究生院（上海應(yīng)用物理研究所）
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2015
【分類號(hào)】：TB383.1;O629.74

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