【摘要】：抗生素作為獸藥和飼料添加劑已在畜牧業(yè)中廣泛使用,然而過度或濫用抗生素會導致抗生素殘留及耐藥菌產(chǎn)生,這既嚴重威脅人類健康,也會破壞生態(tài)平衡。因此,發(fā)展快速靈敏檢測抗生素的方法具有重要意義。電化學傳感器因具有設備簡單、操作方便、分析快速等優(yōu)點,已成為醫(yī)療檢測領域的研究熱點。鑒于此,本論文利用制備的類石墨烯功能納米復合材料,構筑了抗生素電化學傳感平臺,建立了新型抗生素檢測的電化學傳感分析方法,主要研究內(nèi)容如下:1、利用一步水熱法制備了三維氮雜石墨烯水凝膠/二硫化鉬納米復合材料(3D NGH/MoS_2),該材料具有比表面大、導電性良好、電子轉(zhuǎn)移效率高等優(yōu)異的性能,且可負載更多的生物識別分子。利用氯霉素(CAP)適配體與3D NGH/MoS_2之間的π-π吸附作用,構筑了識別CAP的光電化學(PEC)傳感界面。適配體吸附在3D NGH/MoS_2表面,阻礙了物質(zhì)傳遞,導致光電流強度顯著降低,當其與CAP特異性結(jié)合形成復合物后,脫離3D NGH/MoS_2表面,進而光電流強度得到恢復。基于這一原理,研制了一種CAP的PEC適配體傳感器。在優(yōu)化條件下,所恢復的光電流強度與CAP濃度在0.1~300 nmol L-1(R2=0.998)范圍內(nèi)呈良好的線性關系,其檢出限為0.03 nmol L-1,且所研制的傳感器具有良好的選擇性和重現(xiàn)性,可用于CAP的快速檢測。2、采用一步水熱法合成了石墨相氮化碳/石墨烯水凝膠納米復合材料(g-C_3N_4/GH)。對比研究發(fā)現(xiàn),g-C_3N_4/GH可與共反應劑K2S_2O8產(chǎn)生更強的電化學發(fā)光(ECL)信號(約為g-C_3N_4的4.2倍),表明GH的引入可有效增強K2S_2O8體系的ECL信號。以所制備的g-C_3N_4/GH為載體,利用其與四環(huán)素(TET)適配體間的π-π吸附作用,構筑了識別TET的傳感界面。適配體的吸附阻礙了物質(zhì)傳遞,導致ECL信號顯著降低,當其與TET結(jié)合形成后,脫離材料表面,ECL信號得到恢復。基于此原理,研制了一種TET的ECL適配體傳感器。在最優(yōu)條件下,所構建傳感器的工作范圍為0.5 nmol L-1~1μmol L-1,檢出限為0.17 nmol L-1,且具有良好的選擇性及重現(xiàn)性,為抗生素的檢測提供了新思路。3、通過煅燒法合成超薄石墨相氮化碳/氧化鎢(utg-C_3N_4/WO_3)納米復合材料。對比實驗發(fā)現(xiàn),utg-C_3N_4的引入提升了WO_3導電性及電荷轉(zhuǎn)移的效率,延長了光生載流子的壽命,并有效抑制了光生電子-空穴的分離。基于葡萄糖可被空穴氧化,進而增強光電流的原理,構建了一種靈敏的葡萄糖PEC傳感器。在優(yōu)化條件下,所構建的PEC傳感器具有線性范圍寬(10~7120μmol L-1)、檢出限低(3.33μmol L-1)、選擇性高及穩(wěn)定性好等優(yōu)點,為構建葡萄糖靈敏測定平臺提供了新方法。
[Abstract]:Antibiotics, as veterinary drugs and feed additives, have been widely used in animal husbandry. However, excessive or excessive use of antibiotics will lead to the production of antibiotic residues and drug-resistant bacteria, which will not only seriously threaten human health, but also destroy the ecological balance. Therefore, it is of great significance to develop a rapid and sensitive method for the detection of antibiotics. Electrochemical sensor has become a research hotspot in the field of medical detection because of its advantages of simple equipment, convenient operation and fast analysis. In view of this, a novel electrochemical sensing platform for antibiotics was constructed by using graphene like functional nanocomposites, and a novel electrochemical sensing analysis method for antibiotic detection was established. The main research contents are as follows: one step hydrothermal method was used to prepare three-dimensional aza-graphene hydrogel / molybdenum disulfide nanocomposite (3D NGH/MoS_2). The material has excellent properties such as large surface area, good conductivity, high electron transfer efficiency, etc. And more biometric molecules can be loaded. Based on the 蟺-蟺 adsorption between chloramphenicol (CAP) aptamer and 3D NGH/MoS_2, the photochemical (PEC) sensing interface for CAP recognition was constructed. The aptamer adsorbs on the surface of 3D NGH/MoS_2, hinders the material transfer, and results in a significant decrease in the photocurrent intensity. When the aptamer binds to CAP specifically to form a complex, it breaks away from the surface of 3D NGH/MoS_2, and the photocurrent intensity recovers. Based on this principle, a PEC adaptor sensor for CAP is developed. Under the optimized conditions, the recovered photocurrent intensity has a good linear relationship with the concentration of CAP in the range of 0.1 ~ 300 nmol ~ (-1) (R _ (2o) ~ (0.998), the detection limit is 0.03 nmol / L ~ (-1), and the developed sensor has good selectivity and reproducibility. The graphite phase carbon nitride / graphene hydrogel nanocomposite (g-C_3N_4/GH) was synthesized by one step hydrothermal method. It is found that the electrochemiluminescence (ECL) signal (about 4.2 times that of g-C_3N_4) can be produced by the co-reaction agent K2S_2O8. The results show that the addition of GH can effectively enhance the ECL signal of K2S_2O8 system. Using the prepared g-C_3N_4/GH as the carrier and the 蟺-蟺 adsorption between the tetracycline (TET) aptamer and the tetracycline (TET) aptamer, the sensing interface for TET recognition was constructed. The adsorption of aptamer hinders the material transfer, resulting in a significant decrease in the ECL signal. When the aptamer binds to the TET, the ECL signal is recovered from the surface of the material. Based on this principle, a ECL adaptor sensor for TET is developed. Under the optimal conditions, the working range of the sensor is 0. 5 nmol / L ~ (-1) and the detection limit is 0. 17 nmol / L ~ (-1). The sensor has good selectivity and reproducibility. It provides a new idea for the detection of antibiotics. The ultrathin graphite phase carbon nitride / tungsten oxide (utg-C_3N_4/WO_3) nanocomposites are synthesized by calcination method. The experimental results show that the introduction of tippg-C3Ns _ 4 improves the conductivity and charge transfer efficiency of WO_3, prolongs the lifetime of photogenerated carriers, and effectively inhibits the separation of photogenerated electrons and holes. Based on the principle that glucose can be oxidized by holes and thus enhanced photocurrent, a sensitive glucose PEC sensor is constructed. Under the optimized conditions, the PEC sensor has the advantages of wide linear range (10 ~ 7120 渭 mol ~ (-1), low detection limit (3.33 渭 mol ~ (-1), high selectivity and good stability.
【學位授予單位】：江蘇大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X830.2;O657.1

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相關期刊論文 前10條

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本文編號：2186144