金属-有机骨架材料及NiS纳米材料的制备及其在电化学传感器中的应用

发布时间：2018-03-04 00:24

本文选题：金属-有机骨架材料　切入点：硫化镍纳米颗粒　出处：《云南师范大学》2017年硕士论文　论文类型：学位论文

【摘要】：金属-有机骨架材料(MOFs)为多孔结构且孔径可调节,具有比表面积大、粒径可调节、易修饰等特点,已经受到越来越多科研工作者的青睐。本文合成了金属-有机骨架材料MIL-101,构建电化学传感器用于吗啡的快速检测。然而,MOFs材料因其本身导电性弱甚至绝缘的特点,在电化学方面的应用受到限制。本文在金属-有机骨架材料上负载了金属纳米颗粒,使其导电性增强的同时还具有好的生物相容性、较强催化性能等优点。本文合成了Au NPs/MIL-101、Pt NPs@UiO-66-NH2纳米复合材料,并将其用于构建免疫传感器检测微囊藻毒素(MC-LR)、C-反应蛋白(CRP)。除此之外,本文还合成了硫化镍(NiS)纳米颗粒作基底用于构建免疫传感器检测CRP。具体内容如下:(1)通过水热合成法合成一种Cr3+的金属-有机骨架材料MIL-101,制得电化学传感器(MIL-101/GCE)用于吗啡的快速灵敏检测。吗啡在MIL-101/GCE上的电化学行为用差分脉冲伏安法、循环伏安法来表征。在最佳条件下,测定吗啡的线性范围为1.5×10-6-2.0×10-4mol/L,检测下限为5×10-7mol/L,相关系数为0.9911。将该传感器用于血清中吗啡的检测,回收率为101.7%,结果令人满意。说明该传感器有良好应用前景。(2)在上述合成的金属-有机骨架材料(MIL-101)上负载了Au纳米颗粒(Au NPs),形成Au NPs/MIL-101复合材料,该材料对抗坏血酸的氧化具有良好的催化性。以还原氧化石墨烯(rGO)作为固定基质,以Au NPs/MIL-101复合材料作为标记材料,制备了一种竞争型的微囊藻毒素免疫传感器。该传感器检测微囊藻毒素的线性范围为0.05 ng/mL-75μg/mL,线性相关系数为0.9951,检测下限为0.02 ng/mL。(3)采用水热合成法合成了金属有机骨架材料UiO-66-NH2,负载了Pt纳米颗粒(Pt NPs)制得金属-有机骨架复合材料(Pt NPs@UiO-66-NH2),该材料对对硝基苯酚的还原具有较好的催化效果。以Pt NPs@UiO-66-NH2为固定基质将CRP抗体(anti-CRP)固定于玻碳电极上,当抗原与其发生特异性免疫反应时,会阻碍Pt NPs@Ui O-66-NH2对对硝基苯酚的催化作用,降低其响应电流,从而实现CRP的快速检测。在最优的实验条件下,该传感器在0.01-500 ng/mL有良好的线性关系,线性相关系数为0.9935,检测下限为0.02 ng/mL。该传感器制作简单,成本低廉,灵敏度高,稳定性高。(4)合成了负载金纳米(Au NPs)颗粒的硫化镍(NiS)纳米材料,通过壳聚糖(Chit)将其固定在玻碳电极表面作为电化学生物传感器的固定基质。将C-反应蛋白(CRP)抗体固定到修饰过的玻碳电极表面,利用二茂铁甲酸标记CRP抗体,构建夹心型CRP生物传感器。采用差分脉冲伏安法(DPV)检测标记物二茂铁甲酸在0.3 V左右的特征峰信号,该电流与培育的CRP抗原量成正比,从而实现对CRP的定量检测。本传感器检测CRP的线性范围为0.01-500 ng/mL,线性相关系数为0.9939,检测下限为3.3 pg/mL。该免疫传感器提供了一种更有效和更灵敏地检测CRP的方法。
[Abstract]:The metal-organic framework material (MOFs) is porous with adjustable pore size, large specific surface area, adjustable particle size, easy modification and so on. MIL-101, a metal-organic skeleton material, was synthesized and electrochemical sensors were constructed for the rapid detection of morphine. The application of electrochemistry is limited. In this paper, metal nanoparticles are loaded on metal-organic skeleton materials, which enhance their electrical conductivity and have good biocompatibility. In this paper, au NPs / MIL-101 Pt NPs@UiO-66-NH2 nanocomposites were synthesized and used to construct an immunosensor for the detection of microcystins MC-LRN C-reactive protein (CRP). In this paper, nickel sulphide (NiS) nanoparticles were also synthesized as substrates to construct an immunosensor for the detection of CRPs. The specific contents are as follows: (1) by hydrothermal synthesis, a metal-organic skeleton material MIL-101 of Cr3 was synthesized, and the electrochemical sensor MIL-101 / GCE-MIL-101 / GCEwas prepared for use in the detection of CRPs. Rapid and sensitive detection of morphine. The electrochemical behavior of morphine on MIL-101/GCE was determined by differential pulse voltammetry. Under the optimum conditions, the linear range of morphine was 1.5 脳 10-6-2.0 脳 10-4 mol / L, the detection limit was 5 脳 10-7 mol / L, and the correlation coefficient was 0.9911.The sensor was used to detect morphine in serum. The recovery rate is 101.7 and the results are satisfactory. The results show that the sensor has a good prospect of application. It shows that the sensor is loaded with au nanoparticles and au NPs to form au NPs/MIL-101 composites on the metal-organic skeleton material (MIL-101). This material has good catalytic properties for the oxidation of ascorbic acid. The reduced graphene oxide rgox is used as the fixed matrix, and the au NPs/MIL-101 composite is used as the marking material. A competitive microcystin immunosensor was prepared. The linear range of the biosensor for microcystins was 0. 05 ng/mL-75 渭 g / mL, the linear correlation coefficient was 0. 9951, and the detection limit was 0. 02 ng / mL. 3) the organometallic skeleton was synthesized by hydrothermal synthesis. The metal-organic matrix composite (Pt NPs) was prepared from UiO-66-NH _ 2 supported Pt nanoparticles. This material has a good catalytic effect on the reduction of p-nitrophenol. CRP anti-CRP was immobilized on the glassy carbon electrode with Pt NPs@UiO-66-NH2 as the stationary substrate. The specific immunoreaction of Pt NPs@Ui O-66-NH2 on p-nitrophenol will be blocked when the antigen reacts with it, and the response current of Pt NPs@Ui O-66-NH2 will be reduced, so that the rapid detection of CRP can be achieved. The sensor has a good linear relationship at 0.01-500 ng/mL. The linear correlation coefficient is 0.9935 and the detection limit is 0.02 ng / mL. The sensor has the advantages of simple fabrication, low cost, high sensitivity and high stability. Chitosan was immobilized on the surface of glassy carbon electrode as the immobilized substrate of electrochemical biosensor. The antibody against C-reactive protein was immobilized on the surface of modified glassy carbon electrode. Ferrocenyl formic acid was used to label CRP antibody. A sandwich CRP biosensor was constructed. The characteristic peak signal of ferroceneformic acid was detected by differential pulse voltammetry. The current was proportional to the amount of CRP antigen. The linear range of detection of CRP is 0.01-500 ng / mL, the linear correlation coefficient is 0.9939, and the detection limit is 3.3 PG / mL. This immunosensor provides a more effective and sensitive method for detecting CRP.
【学位授予单位】：云南师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O657.1;TP212.2

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