类石墨烯基纳米复合材料电化学传感平台的构建及其应用研究
发布时间：2018-08-16 13:37
【摘要】：抗生素作为兽药和饲料添加剂已在畜牧业中广泛使用,然而过度或滥用抗生素会导致抗生素残留及耐药菌产生,这既严重威胁人类健康,也会破坏生态平衡。因此,发展快速灵敏检测抗生素的方法具有重要意义。电化学传感器因具有设备简单、操作方便、分析快速等优点,已成为医疗检测领域的研究热点。鉴于此,本论文利用制备的类石墨烯功能纳米复合材料,构筑了抗生素电化学传感平台,建立了新型抗生素检测的电化学传感分析方法,主要研究内容如下:1、利用一步水热法制备了三维氮杂石墨烯水凝胶/二硫化钼纳米复合材料(3D NGH/MoS_2),该材料具有比表面大、导电性良好、电子转移效率高等优异的性能,且可负载更多的生物识别分子。利用氯霉素(CAP)适配体与3D NGH/MoS_2之间的π-π吸附作用,构筑了识别CAP的光电化学(PEC)传感界面。适配体吸附在3D NGH/MoS_2表面,阻碍了物质传递,导致光电流强度显著降低,当其与CAP特异性结合形成复合物后,脱离3D NGH/MoS_2表面,进而光电流强度得到恢复。基于这一原理,研制了一种CAP的PEC适配体传感器。在优化条件下,所恢复的光电流强度与CAP浓度在0.1~300 nmol L-1(R2=0.998)范围内呈良好的线性关系,其检出限为0.03 nmol L-1,且所研制的传感器具有良好的选择性和重现性,可用于CAP的快速检测。2、采用一步水热法合成了石墨相氮化碳/石墨烯水凝胶纳米复合材料(g-C_3N_4/GH)。对比研究发现,g-C_3N_4/GH可与共反应剂K2S_2O8产生更强的电化学发光(ECL)信号(约为g-C_3N_4的4.2倍),表明GH的引入可有效增强K2S_2O8体系的ECL信号。以所制备的g-C_3N_4/GH为载体,利用其与四环素(TET)适配体间的π-π吸附作用,构筑了识别TET的传感界面。适配体的吸附阻碍了物质传递,导致ECL信号显著降低,当其与TET结合形成后,脱离材料表面,ECL信号得到恢复。基于此原理,研制了一种TET的ECL适配体传感器。在最优条件下,所构建传感器的工作范围为0.5 nmol L-1~1μmol L-1,检出限为0.17 nmol L-1,且具有良好的选择性及重现性,为抗生素的检测提供了新思路。3、通过煅烧法合成超薄石墨相氮化碳/氧化钨(utg-C_3N_4/WO_3)纳米复合材料。对比实验发现,utg-C_3N_4的引入提升了WO_3导电性及电荷转移的效率,延长了光生载流子的寿命,并有效抑制了光生电子-空穴的分离。基于葡萄糖可被空穴氧化,进而增强光电流的原理,构建了一种灵敏的葡萄糖PEC传感器。在优化条件下,所构建的PEC传感器具有线性范围宽(10~7120μmol L-1)、检出限低(3.33μmol L-1)、选择性高及稳定性好等优点,为构建葡萄糖灵敏测定平台提供了新方法。
[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.
【学位授予单位】：江苏大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X830.2;O657.1
[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.
【学位授予单位】：江苏大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X830.2;O657.1
【参考文献】
相关期刊论文 前10条
1 刘文静;;高效液相色谱法检测乳品饮料中四环素类抗生素[J];食品研究与开发;2016年21期
2 黄飞;蒲雪超;冉o，
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