本文選題：MoS_2 + 類過氧化物酶��； 參考：《濟(jì)南大學(xué)》2017年碩士論文

【摘要】：天然酶因其具有催化效率高、催化性能專一的優(yōu)點被廣泛應(yīng)用在醫(yī)藥合成、臨床檢測、環(huán)境監(jiān)測和農(nóng)業(yè)等各個領(lǐng)域。但由于其不耐酸堿、不耐高溫、穩(wěn)定性不好、提純繁瑣、價格昂貴等不足限制了它的廣泛應(yīng)用。因此,利用化學(xué)合成的方法合成一類具有催化性能的類酶來代替這種傳統(tǒng)的生物酶非常有必要。進(jìn)來,隨著納米材料的不斷開發(fā)和研究,因其具有良好的表面效應(yīng)、量子尺寸效應(yīng)被廣泛的應(yīng)用在了各個領(lǐng)域,但是其類過氧化物酶的特性往往被忽略。自從2007年閻錫蘊(yùn)課題組成功合成了四氧化三鐵磁性納米粒子的類過氧化物酶的特性以來,隨后金屬氧化物、金屬硫化鉬、MOF等納米材料的類過氧化物酶的特性都被相繼發(fā)現(xiàn)。并且與天然酶相比類酶具有很多優(yōu)點:催化性能高,穩(wěn)定性好,合成簡單,成本低�；谝陨蟽�(nèi)容,本文主要工作是系統(tǒng)開發(fā)和研究不同形貌的MoS_2類過氧化物酶,研究其催化機(jī)理,并將其應(yīng)用在電化學(xué)和電化學(xué)發(fā)光生物傳感領(lǐng)域,用于檢測腫瘤標(biāo)志物和寡核苷酸序列的含量。三年來主要開展了以下四方面的研究工作:(1)采用簡單的方法合成MoS_2-Au復(fù)合物,在過氧化氫存在的條件下,片狀MoS_2能夠催化氧化TMB變色,證明MoS_2具有類過氧化物酶的性質(zhì),它能夠催化過氧化氫分解產(chǎn)生穩(wěn)定的電流信號,并且MoS_2-Au復(fù)合物的酶催化活性比MoS_2好,原因是引入了導(dǎo)電性良好的Au NPs,因此,將其應(yīng)用在免疫傳感器上,用于檢測CEA的含量。MoS_2-Au復(fù)合物用于標(biāo)記一抗,二抗標(biāo)記在Ag NPs-GOx的復(fù)合物上。產(chǎn)生的電流強(qiáng)度與CEA含量的對數(shù)值成線性關(guān)系,采用電化學(xué)方法可以靈敏檢測CEA的含量。此方法操作簡單、重現(xiàn)性好、成本低,可用于血清樣品中腫瘤標(biāo)志物的檢測。(2)制備具有良好導(dǎo)電性的金-紙工作電極,合成粒徑小的MoS_2納米片,實驗證明,和大粒徑的MoS_2納米片相比,其對過氧化氫的催化性能更好,類過氧化物酶的特性更穩(wěn)定�；诖酥苽淞艘粋�便攜式的夾心型免疫傳感器,用于測定CA125的含量,該紙芯片免疫傳感器可用于臨床腫瘤標(biāo)志物的實時檢測,這種操作簡單的分析手段在臨床診斷有很好的應(yīng)用前景。(3)將合成的MoS_2納米片應(yīng)用在DNA傳感器上,在量子點-過氧化氫體系中起到猝滅Cd S/Zn S電化學(xué)發(fā)光的作用。利用該原理構(gòu)建電化學(xué)發(fā)光傳感器用于檢測寡核苷酸序列的含量,此方法操作簡單、靈敏度高、選擇性好,可用于血清中DNA含量的檢測。MoS_2類過氧化物酶可以廣泛的應(yīng)用在生物技術(shù)和基因領(lǐng)域,在臨床診斷中具有很好的應(yīng)用價值。(4)為了增大MoS_2的有效催化比表面積,采用水熱法一步合成3D-花狀MoS_2,由于有效催化表面積的增加,3D-花狀MoS_2的催化活性比片狀MoS_2好�；诖诵再|(zhì),構(gòu)建了一種基于魯米諾發(fā)光試劑的新型檢測腫瘤標(biāo)志物PSA的電化學(xué)發(fā)光免疫傳感器。電化學(xué)發(fā)光強(qiáng)度與PSA濃度的對數(shù)值成線性關(guān)系,線性范圍是0.001 ng·m L~(-1)~100ng·m L~(-1),檢測限低至0.28 pg·m L~(-1)。該MoS_2類酶顯著的催化活性使它代替了天然酶用于構(gòu)建基于酶的分析方法,這種方法可以用于鑒別其他的目標(biāo)分子。
[Abstract]:Natural enzymes have been widely used in various fields, such as pharmaceutical synthesis, clinical testing, environmental monitoring and agriculture, because of their high catalytic efficiency and catalytic performance. But because of their lack of acid-base, high temperature resistance, poor stability, tedious purification, high price and so on, it has limited its wide application. Therefore, chemical synthesis methods are used. It is necessary to be a class of enzyme like enzymes with catalytic properties instead of this traditional enzyme. With the continuous development and research of nanomaterials, the quantum size effect has been widely used in various fields because of its good surface effect. But the properties of its peroxidase like enzyme are often ignored. Since 2007, Yan Xiyun Since the project team successfully synthesized the properties of the peroxidase of iron oxide magnetic nanoparticles, the properties of peroxidase in metal oxide, molybdenum sulfide, MOF and other nanomaterials have been discovered successively. And compared with natural enzymes, the enzyme class has many advantages: high catalytic performance, good stability, simple synthesis and low cost. Based on the above, the main work of this paper is to develop and study the different morphologies of MoS_2 peroxidase, to study its catalytic mechanism, and to apply it in the field of electrochemical and electrochemiluminescence biosensors to detect the content of tumor markers and oligonucleotide sequences. In the past three years, the following four research work has been carried out. (1) a simple method is used to synthesize the MoS_2-Au complex. Under the presence of hydrogen peroxide, the flake MoS_2 can catalyze the oxidation of TMB. It is proved that MoS_2 has the properties of peroxidase, which can catalyze the decomposition of hydrogen peroxide to produce stable current signal, and the enzyme catalytic activity of MoS_2-Au complex is better than that of MoS_2. The reason is the introduction of the result. Au NPs, which has good electrical conductivity, is applied to the immune sensor to detect the content of CEA content.MoS_2-Au complex for labeling one anti, two anti labeling in Ag NPs-GOx complex. The current intensity is linear with the value of CEA content, and the electrochemical method can detect the content of CEA sensitively. This method is simple to operate. Single, reproducible and low cost can be used in the detection of tumor markers in serum samples. (2) the preparation of gold paper working electrodes with good conductivity and the synthesis of small size MoS_2 nanoscale have proved that compared with the large size MoS_2 nanoscale, the catalytic properties of the hydrogen peroxide are better and the properties of the peroxidase are more stable. Based on this A portable sandwich immunosensor was prepared to determine the content of CA125. The paper chip immune sensor can be used to detect the clinical tumor markers in real time. This simple method of analysis has a good application prospect in the clinical diagnosis. (3) the synthesized MoS_2 nanoscale is applied to the DNA sensor, and the quantum dot - peroxy is used. The chemical luminescence of Cd S/Zn S was quenched in the hydrogen system. The electrochemiluminescence sensor was used to detect the content of oligonucleotide sequence. This method is simple, sensitive and selective, and can be used for the detection of DNA content in serum.MoS_2 peroxisase, which can be widely used in biotechnology and gene. The field has good application value in clinical diagnosis. (4) in order to increase the effective catalytic surface area of MoS_2, 3D- flower like MoS_2 is synthesized by hydrothermal method. The catalytic activity of 3D- flower like MoS_2 is better than that of flake MoS_2 because of the increase of effective catalytic surface area. Based on this property, a new type of Lumino luminescent reagent is constructed. The electrochemiluminescence immunosensor of the tumor marker PSA was measured with a linear relationship between the electrochemiluminescence intensity and the concentration of PSA. The linear range was 0.001 ng. M L~ (-1) ~100ng. M L~ (-1), and the detection limit was low to 0.28 PG m. The method can be used to identify other target molecules.

【學(xué)位授予單位】：濟(jì)南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TQ136.12;O657.1

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