自支撑Ni-MOF衍生材料构建的无酶葡萄糖传感器
发布时间：2018-10-12 17:20
【摘要】：糖尿病因能引起身体多系统的损害而成为威胁全球人类健康的疾病之一。糖尿病患者在日常生活中,需要长期规律地监控血糖浓度从而降低持续高血糖引起的并发症发病几率,因此研发高效、可靠的葡萄糖传感器非常重要。目前,市售的血糖仪为酶基葡萄糖电化学传感器,该类传感器所使用试纸的活性物质为葡萄糖氧化酶,酶作为价格昂贵的生物活性分子且固定化过程复杂使得该类传感器的成本颇高,因此人们尝试用各种金属及碳材料等构建价格低廉、稳定性好的无酶葡萄糖电化学传感器,以期替代酶基葡萄糖电化学传感器。近些年,有部分研究工作致力于将金属有机骨架化合物(MOFs)用作硬模板或前驱体,以制备具有优异电催化氧化葡萄糖活性的MOFs衍生材料。但此类材料大多为粉体,需采用粘结剂将其涂覆于传统电极上制备成工作电极,导致制备复杂、电活性材料易脱落、稳定性也较差。鉴于此,本论文以泡沫镍为基材,利用水热合成法,在其上原位生长了Ni-MOF,并以此为模板制备出自支撑的Ni@C纳米片电极及CuNi@C电极,将其用于构建无酶葡萄糖传感器并对其性质进行研究。以下为本论文的主要研究结果:(1)通过水热合成、热解两个步骤制备了自支撑Ni@C纳米片电极,该电极具有三维多级孔道结构,在葡萄糖的无酶检测方面表现出优异的电催化活性。研究结果显示,该电极检测葡萄糖的灵敏度高达32.7944 mA·mM-1·cm-2,明显优于某些镍基材料电极,线性范围为0.15μmol·L-1~1.475 mmol·L-1,检出限低至50nmol·L-1,并且该电极对葡萄糖表现出良好的选择性,且具有较好的重现性、长期稳定性及抗氯离子毒化性能。此外,研究结果显示自支撑Ni@C纳米片电极可用于人体血清样品的实际检测,并且测定结果具有较高的准确度和精密度。(2)在自支撑Ni@C纳米片电极的基础上,通过恒电位电沉积的方法制备了自支撑CuNi@C电极,Cu纳米颗粒均匀生长于电极表面,由于Cu与Ni之间的协同催化作用,该电极具有优异的无酶葡萄糖传感性能。研究结果显示该电极检测葡萄糖的灵敏度高达17.1203 mA·mM-1·cm-2,线性范围为0.2μmol·L-1~2.7206mmol·L-1,检出限为66.67 nmol·L-1,电极对葡萄糖具有良好的选择性,且表现出较好的重现性、长期稳定性和抗氯离子毒化性能,在人体血清样品的检测中能够获得与医院检测报告相近的结果,表明该电极具有实际应用价值。
[Abstract]:Diabetes has become one of the diseases that threaten human health worldwide because it can cause damage to many systems. In order to reduce the incidence of complications caused by sustained hyperglycemia, it is very important to develop an efficient and reliable glucose sensor in the daily life of diabetic patients. At present, the blood glucose instrument on the market is an enzyme based glucose electrochemical sensor, and the active substance of the test paper used in this kind of sensor is glucose oxidase. Enzyme is an expensive bioactive molecule and the immobilization process is very complicated, so people try to use various metal and carbon materials to construct low price and good stability enzyme free glucose electrochemical sensor. In order to replace the enzyme-based glucose electrochemical sensor. In recent years, some researches have been devoted to the preparation of MOFs derivatives with excellent electrocatalytic oxidation of glucose by using organometallic skeleton compound (MOFs) as a hard template or precursor. However, most of these materials are powder, which need to be coated with binder on the traditional electrode to prepare working electrode, which leads to complex preparation, easy to fall off the electrically active material and poor stability. In view of this, Ni-MOF, was grown in situ by hydrothermal synthesis with nickel foam as the substrate and used as a template to prepare self-supported Ni@C nanochip electrode and CuNi@C electrode. It was used to construct enzyme-free glucose sensor and its properties were studied. The main results are as follows: (1) Self-supporting Ni@C nanochip electrode was prepared by hydrothermal synthesis and pyrolysis. The electrode has a three-dimensional multilevel pore structure and has excellent electrocatalytic activity in the non-enzymatic detection of glucose. The results show that the sensitivity of the electrode for glucose detection is as high as 32.7944 mA mM-1 cm-2, and the linear range is 0.15 渭 mol L ~ (-1) ~ 1.475 mmol ~ (-1). The detection limit is as low as 50nmol L ~ (-1), and the electrode has good selectivity for glucose. It also has good reproducibility, long-term stability and anti-chlorine poisoning property. In addition, the results show that the self-supporting Ni@C nanochip electrode can be used for the actual detection of human serum samples, and the determination results have high accuracy and precision. (2) based on the self-supporting Ni@C nanoscale electrode, Self-supporting CuNi@C electrode was prepared by potentiostatic electrodeposition. Cu nanoparticles grew uniformly on the surface of the electrode. Because of the synergistic catalysis between Cu and Ni, the electrode had excellent enzymatic glucose sensing performance. The results showed that the sensitivity of the electrode for glucose detection was as high as 17.1203 mA mM-1 cm-2, the linear range was 0.2 渭 mol L-1~2.7206mmol L -1, and the detection limit was 66.67 nmol L -1. The electrode had good selectivity for glucose, and showed good reproducibility, long-term stability and resistance to chloride poisoning. The results obtained in the detection of human serum samples are similar to those reported in hospitals, indicating that the electrode has practical application value.
【学位授予单位】：哈尔滨工业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：R587.1;O657.1
[Abstract]:Diabetes has become one of the diseases that threaten human health worldwide because it can cause damage to many systems. In order to reduce the incidence of complications caused by sustained hyperglycemia, it is very important to develop an efficient and reliable glucose sensor in the daily life of diabetic patients. At present, the blood glucose instrument on the market is an enzyme based glucose electrochemical sensor, and the active substance of the test paper used in this kind of sensor is glucose oxidase. Enzyme is an expensive bioactive molecule and the immobilization process is very complicated, so people try to use various metal and carbon materials to construct low price and good stability enzyme free glucose electrochemical sensor. In order to replace the enzyme-based glucose electrochemical sensor. In recent years, some researches have been devoted to the preparation of MOFs derivatives with excellent electrocatalytic oxidation of glucose by using organometallic skeleton compound (MOFs) as a hard template or precursor. However, most of these materials are powder, which need to be coated with binder on the traditional electrode to prepare working electrode, which leads to complex preparation, easy to fall off the electrically active material and poor stability. In view of this, Ni-MOF, was grown in situ by hydrothermal synthesis with nickel foam as the substrate and used as a template to prepare self-supported Ni@C nanochip electrode and CuNi@C electrode. It was used to construct enzyme-free glucose sensor and its properties were studied. The main results are as follows: (1) Self-supporting Ni@C nanochip electrode was prepared by hydrothermal synthesis and pyrolysis. The electrode has a three-dimensional multilevel pore structure and has excellent electrocatalytic activity in the non-enzymatic detection of glucose. The results show that the sensitivity of the electrode for glucose detection is as high as 32.7944 mA mM-1 cm-2, and the linear range is 0.15 渭 mol L ~ (-1) ~ 1.475 mmol ~ (-1). The detection limit is as low as 50nmol L ~ (-1), and the electrode has good selectivity for glucose. It also has good reproducibility, long-term stability and anti-chlorine poisoning property. In addition, the results show that the self-supporting Ni@C nanochip electrode can be used for the actual detection of human serum samples, and the determination results have high accuracy and precision. (2) based on the self-supporting Ni@C nanoscale electrode, Self-supporting CuNi@C electrode was prepared by potentiostatic electrodeposition. Cu nanoparticles grew uniformly on the surface of the electrode. Because of the synergistic catalysis between Cu and Ni, the electrode had excellent enzymatic glucose sensing performance. The results showed that the sensitivity of the electrode for glucose detection was as high as 17.1203 mA mM-1 cm-2, the linear range was 0.2 渭 mol L-1~2.7206mmol L -1, and the detection limit was 66.67 nmol L -1. The electrode had good selectivity for glucose, and showed good reproducibility, long-term stability and resistance to chloride poisoning. The results obtained in the detection of human serum samples are similar to those reported in hospitals, indicating that the electrode has practical application value.
【学位授予单位】：哈尔滨工业大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：R587.1;O657.1
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