【摘要】：直接在微導(dǎo)管或者兩端檢測池中施加一定的電壓,處于該電場中的導(dǎo)體和溶液界面之間即會產(chǎn)生電勢差,當(dāng)電勢差達(dá)到一定值時就會引發(fā)電活性物質(zhì)在導(dǎo)體兩端發(fā)生氧化還原反應(yīng),這樣能在兩端發(fā)生電化學(xué)反應(yīng)的導(dǎo)體我們稱之為雙極電極。近年來,將雙極電極與電化學(xué)發(fā)光技術(shù)相結(jié)合,應(yīng)用于生命分析和環(huán)境監(jiān)測,已經(jīng)成為當(dāng)前的研究熱點(diǎn)之一。該方法具有諸多優(yōu)點(diǎn),如靈敏度高、成本低廉、裝置簡單等。目前,雙極電極-電化學(xué)發(fā)光技術(shù)(BPE-ECL)己經(jīng)成功運(yùn)用于分子篩選、可視化陣列化對細(xì)胞、DNA檢測等方面。研究微型的、便于攜帶的BPE-ECL分子識別平臺是今后研究重點(diǎn),本文以雙極電極-電化學(xué)發(fā)光技術(shù)為基礎(chǔ),通過合成、電沉積相關(guān)納米材料實(shí)現(xiàn)了 ECL信號的增強(qiáng),構(gòu)建了幾種不同的BPE-ECL檢測平臺,具體內(nèi)容如下:(1)基于以ITO作為雙極電極的BPE-ECL檢測平臺檢測H202實(shí)驗(yàn)以透光性好的ITO導(dǎo)電玻璃制備成雙極電極檢測平臺,但由于ITO在較高的驅(qū)動電壓下易損壞,影響ITO的導(dǎo)電性和相應(yīng)的ECL發(fā)光強(qiáng)度。實(shí)驗(yàn)在ITO表面電沉積Au膜,Au膜的作用在于防止ITO的損壞并增強(qiáng)ITO的導(dǎo)電性,在雙極電極的陽極電沉積PtNPs,催化檢測物H2O2,放大ECL信號。通過空氣等離子體處理ITO和PDMS檢測池,發(fā)生不可逆鍵合,構(gòu)建出BPE-ECL檢測平臺,創(chuàng)新地使用CdTe@ZnS油性量子點(diǎn)作為發(fā)光體,用于檢測H202,線性范圍為1.0×10-5-4.0×10-9M。最低檢測線為5.0×10-10M。(2)基于以鉛筆芯作為雙極電極的BPE-ECL紙基檢測平臺以簡單易得的鉛筆芯作為雙極電極,結(jié)合紙基,構(gòu)建出了一種新型的BPE-ECL檢測平臺,這種檢測平臺具有成本低廉、可一次性操作、攜帶方便等優(yōu)點(diǎn)。發(fā)光體系為傳統(tǒng)Ru(bpy)32+體系,實(shí)驗(yàn)分別研究了鉛筆芯的長度和直徑對ECL信號的影響,發(fā)現(xiàn)長度和直徑越大的鉛筆芯的ECL強(qiáng)度越大,其原因可由雙極電極的機(jī)理公式和電極面積解釋。為了擴(kuò)大制備的這種檢測平臺在生物分析上的應(yīng)用,類似的,我們在鉛筆芯的陰極端電沉積了 PtNPs,發(fā)現(xiàn)BPE-ECL檢測平臺對H2O2有著很好的響應(yīng),成功的對與細(xì)胞和酶代謝密切相關(guān)的H202進(jìn)行了檢測。(3)基于開關(guān)控制的BPE-ECL檢測平臺同時檢測CEA合成了 Pd-PtNPs,在不需要刻蝕的ITO檢測平臺上構(gòu)建出免疫三明治傳感器,制備成一個發(fā)光池和多個傳感檢測池的環(huán)形檢測平臺。開關(guān)的使用可以在外部控制反應(yīng)發(fā)生的反應(yīng)區(qū)域和反應(yīng)時間,每一個單獨(dú)的開關(guān)代表同一類或者不同的反應(yīng),可實(shí)現(xiàn)操作簡單的對不同濃度的CEA抗原濃度進(jìn)行檢測。通過透射電鏡對合成的Pd-PtNPs進(jìn)行了表征,實(shí)現(xiàn)ECL信號的增強(qiáng)。實(shí)驗(yàn)發(fā)現(xiàn)這種結(jié)合開關(guān)的BPE-ECL檢測平臺有著很好的穩(wěn)定性和重復(fù)性,成功地對不同濃度的CEA抗原進(jìn)行了同時檢測。
[Abstract]:If a certain voltage is applied directly to the microcatheter or the two detection cells, the potential difference will occur between the conductor in the electric field and the interface of the solution. When the potential difference reaches a certain value, the redox reaction of the electroactive material will occur at the two ends of the conductor, which is called the bipolar electrode. In recent years, the application of bipolar electrode and electrochemiluminescence technology in life analysis and environmental monitoring has become one of the research hotspots. This method has many advantages, such as high sensitivity, low cost, simple device and so on. At present, bipolar electrochemiluminescence (BPE-ECL) technology has been successfully used in molecular screening, visual array detection of cell DNA, and so on. The research of micro and portable BPE-ECL molecular recognition platform is the focus in the future. Based on bipolar electrochemiluminescence (ECL) technology, the enhancement of ECL signal is achieved by synthesis and electrodeposition of related nanomaterials. Several different BPE-ECL detection platforms are constructed. (1) based on the BPE-ECL detection platform with ITO as the bipolar electrode, the H202 test platform is fabricated by using the ITO conductive glass with good light transmittance to make the bipolar electrode detection platform. However, ITO is easily damaged at high driving voltage, which affects the conductivity of ITO and the corresponding luminescence intensity of ECL. The purpose of the experiment is to prevent the damage of ITO and enhance the conductivity of ITO by electrodeposition of Au film on the surface of ITO. The anodic electrodeposition of PtNPs, catalyst H _ 2O _ 2 at bipolar electrode can amplify the ECL signal. The ITO and PDMS detection cells were treated by air plasma, and the BPE-ECL detection platform was constructed. The CdTe@ZnS oil quantum dots were used as luminescent, and the linear range was 1.0 脳 10 ~ (-5) -4.0 脳 10 ~ (-9) M. The minimum detection line is 5.0 脳 10 ~ (-10) m. (2) based on the BPE-ECL paper-based detection platform with lead pen core as bipolar electrode and simple and easy to obtain lead pen core as bipolar electrode, a new type of BPE-ECL detection platform is constructed, which has low cost. One-time operation, easy to carry and so on. The effect of the length and diameter of the lead pen core on the ECL signal is studied experimentally in the traditional Ru (bpy) 32 system. It is found that the larger the length and diameter of the lead pen core is, the greater the ECL intensity of the lead pen core is, and the reason can be explained by the mechanism formula of the bipolar electrode and the electrode area. In order to expand the application of the platform to biological analysis, similarly, we found that the BPE-ECL detection platform is very responsive to H2O2 by electrodeposition of PtNPs, on the lead pen core. H202, which is closely related to cell and enzyme metabolism, was successfully detected. (3) the BPE-ECL detection platform based on switch control simultaneously detected CEA synthesis and constructed an immune sandwich sensor on the ITO detection platform without etching. A ring detection platform for a light emitting cell and a plurality of sensing detection cells is prepared. The use of switches can control the reaction area and reaction time externally. Each single switch represents the same or different reactions. It can be operated simply to detect the concentration of CEA antigen in different concentrations. The synthesized Pd-PtNPs was characterized by transmission electron microscope (TEM) to enhance the ECL signal. It is found that this BPE-ECL detection platform has good stability and repeatability. Different concentrations of CEA antigens have been successfully detected at the same time.
【學(xué)位授予單位】：東南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O657.1;TP212.3

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