發(fā)布時間：2018-07-07 17:37

  本文選題：碳點 + 層狀雙金屬氫氧化物��； 參考：《北京化工大學》2016年博士論文

【摘要】：碳點是一種粒徑小于10 nm的碳納米晶,由于具有良好的生物相容性和低毒性、良好的水溶性、很好的化學惰性、抗光漂白性以及可調的帶隙等優(yōu)點,作為碳納米家族的一顆新星,引起了人們的廣泛關注。尤其是碳點具備獨特的光學和電化學性質,在傳感、光電子、生物醫(yī)藥和電催化等領域具有潛在的應用。乙酰膽堿,作為一種研究最為普遍的神經(jīng)遞質,在中樞和外周神經(jīng)系統(tǒng)起著神經(jīng)傳導的作用。乙酰膽堿在多種生命過程中,如學習、記憶、情感和運動等,都起到了重要的作用。因此,神經(jīng)系統(tǒng)中乙酰膽堿的檢測十分重要。另外,乙酰膽堿不僅存在于神經(jīng)系統(tǒng)中,而且普遍存在于一切活細胞中,包括上皮細胞、內皮細胞、免疫細胞等,這些細胞中合成的乙酰膽堿屬于非神經(jīng)性乙酰膽堿系統(tǒng)。在非神經(jīng)性乙酰膽堿系統(tǒng)中,乙酰膽堿可以調節(jié)不依賴神經(jīng)的細胞功能,如增殖、分化、細胞骨架構建、運動、分泌、鞭毛活動和局部釋放調節(jié)等。然而,非神經(jīng)性乙酰膽堿系統(tǒng)中,乙酰膽堿的含量非常低,為pmol L-1級。因此,非神經(jīng)性乙酰膽堿系統(tǒng)中乙酰膽堿的檢測不僅非常重要,而且還是一項具有很大挑戰(zhàn)性的工作。在本論文研究中,我們開發(fā)了一種新的制備碳點的方法,并利用碳點/層狀雙金屬氫氧化物復合物和碳點/陽離子二肽納米囊泡復合物分別構筑乙酰膽堿電化學和電致化學發(fā)光生物傳感器。具體工作如下：1、高能球磨法制備碳點利用高能球磨活性炭和氫氧化鉀的混合物,再經(jīng)過超濾純化的方法制備了具有豐富表面態(tài)的碳點。所制備的碳點展現(xiàn)了雙波長熒光性質。進一步研究表明,第一個發(fā)射峰與表面含氧官能團數(shù)量有關,且不隨激發(fā)波長的移動而移動；第二個發(fā)射峰與碳點的粒徑有關,且隨著激發(fā)波長的增加單調紅移。同時,所制備的碳點也展現(xiàn)了雙波長電致化學發(fā)光性質。2、基于碳點修飾花狀鎳鋁層狀雙金屬氫氧化物構筑無酶乙酰膽堿傳感器利用水熱方法合成了由納米片交叉連接構成的高比表面積花狀鎳鋁層狀雙金屬氫氧化物,之后,將帶有負電荷的碳點修飾到鎳鋁層狀雙金屬氫氧化物表面而獲得鎳鋁層狀雙金屬氫氧化物/碳點復合物。與純的鎳鋁層狀雙金屬氫氧化物相對比,鎳鋁層狀雙金屬氫氧化物/碳點復合物展現(xiàn)了更好的導電性和電催化氧化乙酰膽堿的能力。此鎳鋁層狀雙金屬氫氧化物/碳點復合物修飾的玻碳電極對乙酰膽堿的檢測具有寬的線性范圍(5-6885μmoL-1),高的靈敏度(133.20±0.03mAM-1cm-2)和低的檢測限(1.7μmol L-1)。同時,此生物傳感器還表現(xiàn)出了良好的耐久性和長期穩(wěn)定性,以及非常好的選擇性。這些優(yōu)異的性能要歸功于鎳鋁層狀雙金屬氫氧化物和碳點之間的協(xié)同作用：由納米片交叉連接構成的高比表面積花狀鎳鋁層狀雙金屬氫氧化物有效地提高電極與電解液的接觸面積,從而加快了反應動力學；帶有負電荷的碳點修飾在帶有正電荷的層狀雙金屬氫氧化物的層板上,提高了鎳鋁層狀雙金屬氫氧化物/碳點復合物的導電性,生物相容性以及對乙酰膽堿的親和力。3、基于陽離子二肽納米囊泡/碳點復合物構筑乙酰膽堿電致化學發(fā)光傳感器利用陽離子二肽納米管向陽離子二肽納米囊泡的微結構轉變,將單分散的碳點嵌入到陽離子二肽納米囊泡壁內形成陽離子二肽納米囊泡/碳點復合物。此復合物具有良好的生物相容性,結構穩(wěn)定性以及由于二肽納米囊泡和碳點雙電致發(fā)光體之間的協(xié)同作用而產(chǎn)生的穩(wěn)定而強烈的電致化學發(fā)光信號。此陽離子二肽納米囊泡/碳點復合物修飾電極可以用于乙酰膽堿超靈敏檢測,檢測限可低至2.4 pmol L-1(信噪比為3),同時,此體系還具有很好的選擇性和長期穩(wěn)定性。此優(yōu)異的性能要歸功于陽離子二肽納米囊泡和碳點之間的協(xié)同作用：帶陰離子表面電荷的碳點嵌入到陽離子二肽納米囊泡內,形成穩(wěn)定的結構；二肽納米囊泡和碳點形成復合物,使電致化學發(fā)光的路徑增加；二肽納米囊泡和碳點都對乙酰膽堿具有很好的選擇性。這種具有協(xié)同作用的納米復合材料將在生物傳感器、生物成像、生物藥物、生物電子、生物催化和生物能源等領域具有廣闊的應用前景。
[Abstract]:Carbon point is a carbon nanocrystalline with a particle size less than 10 nm. Due to its good biocompatibility and low toxicity, good water solubility, good chemical inertness, anti photobleaching and adjustable band gap, it has attracted wide attention as a new star of carbon nanofamily. Especially, carbon points have unique optics and electrification. It has potential applications in the fields of sensing, photoelectrons, biopharmaceutical and electrocatalysis. Acetylcholine, as one of the most common neurotransmitters, plays the role of nerve conduction in the central and peripheral nervous systems. Acetylcholine plays an important role in a variety of life processes, such as learning, memory, emotion, and exercise. Therefore, the detection of acetylcholine in the nervous system is very important. In addition, acetylcholine exists not only in the nervous system but also in all living cells, including epithelial cells, endothelial cells, immune cells and so on. The acetylcholine in these cells is a non neurogenic acetylcholine system. In non neurogenic acetylcholine. In the system, acetylcholine can regulate the function of cells that do not depend on the nerve, such as proliferation, differentiation, cytoskeleton construction, movement, secretion, flagellum activity and local release regulation. However, the content of acetylcholine in non neurogenic acetylcholine system is very low, pmol L-1. Therefore, the assay of acetylcholine in non neurogenic acetylcholine system Measurement is not only very important, but also a very challenging task. In this paper, we developed a new method of preparing carbon points, and constructed acetylcholine electrochemiluminescence and electrochemiluminescence using carbon point / layered double metal hydroxide complex and carbon point / cationic two peptide Nanovesicles. The specific work is as follows: 1, a high energy ball milling method is used to prepare a mixture of activated carbon and potassium hydroxide with high energy ball milling, and then a rich surface state carbon point is prepared by ultrafiltration. The carbon points prepared have shown the dual wavelength fluorescence properties. Further research shows that the first emission peak and the surface oxygen functional energy have been shown. The number of clusters is related and does not move with the movement of the excitation wavelengths; the second emission peaks are related to the particle size of the carbon point and monotonically red shift with the increase of the excitation wavelengths. At the same time, the prepared carbon points also exhibit a double wavelength electrochemiluminescence property.2, based on the carbon point modification of the flower like nickel aluminum layered double metal hydroxide to construct an enzyme free acetylcholine. The sensor uses a hydrothermal method to synthesize a high specific surface area flower like nickel aluminum layered double metal hydroxide formed by the cross connection of nanoscale. After that, the negative charge carbon point is modified to the surface of the nickel aluminum layered double metal hydroxide, and the nickel aluminum layered double metal hydroxide / carbon point complex is obtained. The nickel aluminum layered double metal hydroxide / carbon point complex showed better conductivity and electrocatalytic oxidation of acetylcholine. The nickel aluminum layered double metal hydroxide / carbon point composite modified glassy carbon electrode has a wide linear peri (5-6885 moL-1) and high sensitivity (133.20 + 0) for the detection of acetylcholine. 3mAM-1cm-2) and low detection limit (1.7 Mu mol L-1). At the same time, the biosensor also shows good durability and long-term stability, and very good selectivity. These excellent properties are due to the synergism between the nickel aluminum layered double metal hydroxide and the carbon point: high specific surface area made up of nanoscale cross connections. Nickel aluminum layered double metal hydroxide improves the contact area of the electrode and the electrolyte, and thus accelerates the reaction kinetics, and the negative charge carbon point is modified on the laminates with positive charged layered double metal hydroxide, which improves the conductivity of the nickel aluminum layered double metal hydroxide / carbon point complex. The affinity.3 of acetylcholine, based on the cationic two peptide nano vesicle / carbon point complex to construct the electrochemiluminescence sensor of acetylcholine, uses the microstructural transformation of cationic two peptide nanotube to the cationic two peptide nanoscale, and the monodisperse carbon points are embedded into the cationic two peptide nanoscale wall to form a cationic two peptide nanoscale. This complex has good biocompatibility, structural stability and a stable and strong electrochemiluminescence signal produced by the synergistic effect of two peptide nanoscale and carbon point double electroluminescent bodies. This cationic two peptide nano vesicle / carbon point complex modified electrode can be used for acetylcholine hyper Sensitive detection, the detection limit can be as low as 2.4 pmol L-1 (signal-to-noise ratio 3). At the same time, the system also has good selectivity and long-term stability. The excellent performance is due to the synergism between the nano vesicles of the cationic two peptide and the carbon point: the carbon point with the surface charge of the anion is embedded into the cationic two peptide nanoscale to form a stable junction. The two peptide Nanovesicles and carbon dots form complex to increase the path of electrochemiluminescence; the two peptide nanoscale and carbon dots have good selectivity to acetylcholine. This synergistic nanocomposite will be used in biosensors, bioimaging, Bioelectronics, Bioelectronics, biocatalysis and bioenergy. The domain has a broad application prospect.
【學位授予單位】：北京化工大學
【學位級別】：博士
【學位授予年份】：2016
【分類號】：O613.71;TP212.3

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