【摘要】：社會(huì)經(jīng)濟(jì)的不斷進(jìn)步與發(fā)展使人類的生活水平日益提高的同時(shí),相應(yīng)的也凸顯出諸多社會(huì)性問(wèn)題,諸如人口老齡化的加劇、生態(tài)環(huán)境的破壞、食品安全問(wèn)題及現(xiàn)代人不健康的生活方式等,致使罹患癌癥的人數(shù)不斷增多。近年來(lái),我國(guó)腫瘤發(fā)病率不斷上升,其死亡率也已高出世界水平,已成為必須高度重視的社會(huì)性問(wèn)題。目前,臨床上很多癌癥的治療多依賴于抗腫瘤藥物,但它在人體內(nèi)的存在量直接影響人體健康狀況,因此構(gòu)建一種能快速、準(zhǔn)確檢測(cè)該藥物的方法對(duì)其相關(guān)疾病的診斷大有益處。本文以鹽酸阿霉素、長(zhǎng)春新堿和左氧氟沙星作為主要研究目標(biāo),利用分子印跡技術(shù)對(duì)研究目標(biāo)的選擇性識(shí)別,將分子印跡技術(shù)與電化學(xué)傳感器有效結(jié)合,通過(guò)自組裝、電化學(xué)聚合等方法在基體電極表面制備導(dǎo)電性良好且有生物相容性的納米復(fù)合膜,構(gòu)建一系列基于導(dǎo)電聚合膜的抗腫瘤藥物分子印跡傳感器,并將電化學(xué)技術(shù)作為主要測(cè)定手段對(duì)其各項(xiàng)性能進(jìn)行研究討論。納米復(fù)合膜比表面積大、導(dǎo)電能力強(qiáng)的性能可顯著提高所構(gòu)建傳感器的電流響應(yīng)、對(duì)目標(biāo)分子的有效識(shí)別能力以及檢測(cè)的靈敏度。優(yōu)化實(shí)驗(yàn)條件后,將所研制傳感器實(shí)用于生活,考察其實(shí)用價(jià)值,有望構(gòu)建一種能對(duì)該藥物進(jìn)行快速、靈敏、準(zhǔn)確識(shí)別和檢測(cè)的方法。主要研究?jī)?nèi)容如下:1.以3,4-乙烯二氧噻吩(EDOT)為功能單體,鹽酸阿霉素(DOX)為模板分子,在基體金電極表面通過(guò)電聚合等技術(shù)制備DOX印跡敏感膜(MIPs),構(gòu)建了一種可以對(duì)DOX進(jìn)行選擇性檢測(cè)的分子印跡傳感器。通過(guò)一系列電化學(xué)表征手段對(duì)所構(gòu)建傳感器的電化學(xué)性能進(jìn)行研究。優(yōu)化實(shí)驗(yàn)條件后,在含0.005 mol/LK3[Fe(CN)6]及0.1 mol/LKCl的PBS中測(cè)試其響應(yīng)性能。實(shí)驗(yàn)結(jié)果表明,該傳感器對(duì)DOX的檢測(cè)表現(xiàn)有良好重現(xiàn)性、穩(wěn)定性及選擇性,其檢出限(S/N=3)可達(dá)6.5×10-8 mol/L。將此傳感器應(yīng)用于實(shí)際生活中人體血樣內(nèi)DOX的測(cè)定也表現(xiàn)有較大的實(shí)用價(jià)值,結(jié)果較為滿意。2.將長(zhǎng)春新堿(VCR)、甲基丙烯酸(MAA)和馬來(lái)松香丙烯酸乙二醇酯(EGMRA)分別作為模板分子、功能單體和交聯(lián)劑,采用自由基熱聚合方式合成分子印跡聚合物,并將石墨烯-金納米粒子復(fù)合膜作為信號(hào)增敏材料電沉積至基體電極表面,由此研制一種可以選擇性測(cè)定VCR的新型傳感器并通過(guò)一系列電化學(xué)手段對(duì)其性能進(jìn)行優(yōu)化研究。實(shí)驗(yàn)結(jié)果表明,該研制傳感器對(duì)VCR的檢測(cè)范圍為5.0×10-8~5.0×10-6 mol/L,相關(guān)系數(shù)為0.9952,檢出限為2.6×10-8 mol/L,具有較好的選擇性。將此傳感器應(yīng)用于藥品中VCR的檢測(cè),其加標(biāo)回收率為90%~120%,有一定實(shí)用價(jià)值。3.以左氧氟沙星(LVFX)為目標(biāo)分子,吡咯(Py)為功能單體,采用電聚合技術(shù)在修飾有普魯士藍(lán)(PB)導(dǎo)電膜的基體電極表面研制一種可以選擇性檢測(cè)LVFX的分子印跡傳感器。采用電化學(xué)技術(shù)對(duì)其性能進(jìn)行表征,并考察所研制傳感器在pH、孵化時(shí)間、洗脫劑等不同實(shí)驗(yàn)條件下的電化學(xué)響應(yīng)變化。優(yōu)化實(shí)驗(yàn)條件后測(cè)試所研制傳感器的響應(yīng)性能,結(jié)果表明該傳感器對(duì)于LVFX的檢測(cè)表現(xiàn)有良好的選擇性和較寬的線性范圍,且檢出限達(dá)1.7×10-8 mol/L。將其用于左氧氟沙星膠囊中LVFX的分析與檢測(cè),其回收率為96%~105%,效果良好。
[Abstract]:With the continuous progress and development of social economy, the living standard of human beings is improving day by day. At the same time, many social problems are also highlighted, such as the aggravation of population aging, the destruction of ecological environment, the food safety problem and the unhealthy lifestyle of modern people. As a result, the number of cancer patients is increasing. The morbidity is rising, and the mortality rate is also higher than the world level. It has become a social problem that must be attached great importance to. At present, the treatment of many cancers in clinic mostly relies on antineoplastic drugs, but its presence in the body directly affects the health of the human body. Therefore, a rapid and accurate method for the detection of the drug phase is proposed. In this paper, doxorubicin hydrochloride, vincristine and levofloxacin were used as the main research targets. Molecular imprinting technology was used to selectively identify the research targets. Molecular imprinting technology was effectively combined with electrochemical sensors. Conductivity was prepared on the surface of substrate electrode by self-assembly and electrochemical polymerization. A series of molecularly imprinted sensors for antitumor drugs based on conductive polymeric membranes were constructed by using nanocomposite membranes with good properties and biocompatibility. After optimizing the experimental conditions, the developed sensor can be used in daily life to investigate its practical value. It is hopeful to construct a rapid, sensitive, accurate identification and detection method for the drug. The main research contents are as follows: 1. 3,4-ethylenedioxythiophene (EDOT) Doxorubicin hydrochloride (DOX) was used as a template molecule to prepare DOX imprinted sensitive membranes (MIPs) on the surface of the gold electrode. A molecular imprinted sensor for selective detection of DOX was constructed. The electrochemical performance of the sensor was optimized by a series of electrochemical characterization methods. The results show that the sensor has good reproducibility, stability and selectivity for the detection of DOX, and its detection limit (S/N=3) can reach 6.5 *10-8 mol/L. The application of the sensor to the determination of DOX in human blood samples in real life also shows that the sensor has good reproducibility, stability and selectivity. Vincristine (VCR), methacrylic acid (MAA) and maleic rosin ethylene glycol acrylate (EGMRA) were used as template molecules, functional monomers and crosslinkers respectively. Molecularly imprinted polymers were synthesized by free radical thermal polymerization, and graphene-gold nanoparticle composite films were used as signal sensitizers. A new sensor for selective determination of VCR was developed by electrodeposition on the surface of substrate electrode and its performance was optimized by a series of electrochemical methods. The experimental results show that the detection range of the sensor is 5.0 6550 This sensor has been applied to the determination of VCR in drugs with a recovery of 90%~120%. It has a certain practical value. 3. With levofloxacin (LVFX) as the target molecule and pyrrole (Py) as the functional monomer, a selective detection method was developed on the surface of the substrate electrode modified with Prussian blue (PB) conductive film by electropolymerization. Molecular imprinting sensor for measuring LVFX was developed. The performance of the sensor was characterized by electrochemical technique. The electrochemical response of the sensor under different experimental conditions, such as pH, incubation time, eluent and so on, was investigated. The method has good selectivity and wide linear range, and the detection limit is 1.7 *10-8 mol/L. The recovery of LVFX in Levofloxacin capsules is 96%~105%.
【學(xué)位授予單位】：山西師范大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TQ460.72;TP272;O657.1

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