基于硼酸识别的无酶电位型葡萄糖传感器的应用研究

发布时间：2018-05-22 21:06

本文选题：硼酸化合物 + 葡萄糖传感器　；参考：《大连理工大学》2015年硕士论文

【摘要】：近年来,全球范围内糖尿病患者数量的不断增加引起了人们对糖尿病的高度重视,各个领域的科研工作者们相继对葡萄糖传感器产生了浓厚的兴趣。目前,应用最广泛的血糖仪是一种电流型葡萄糖传感器。由于这种葡萄糖传感器易受葡萄糖氧化酶活性的影响,因此发展无酶型葡萄糖传感器是当前研究的热点。本文利用了硼酸化合物具有识别糖的特性并借助DFT理论计算,设计合成了一系列的双硼酸化合物。将稳定的硼酸化合物代替易失活的酶作为葡萄糖的识别分子,并结合其在四十二烷基掺杂的聚合物膜离子选择性电极上能产生阴离子电位响应的特点,建立了基于硼酸化合物识别的电位型葡萄糖传感器,并对其选择性、灵敏度等方面进行了应用研究。具体研究内容如下：1、发展了基于硼酸识别的液膜电极电位型葡萄糖传感器的新方法。依据硼酸能与1,2-或1,3-二羟基化合物结合生成硼酸酯的性质并利用DFT理论计算,设计合成了DBA、DBA1和DBA2三种双硼酸化合物。通过对三者和其与葡萄糖结合生成的硼酸酯的光物理性质及其电化学性质的探究和对识别分子的选择、识别分子的浓度以及缓冲溶液pH的优化,选择了10-5 M DBA作为识别分子在pH 8.0的磷酸缓冲溶液中作为检测葡萄糖的最优条件。利用DBA作为识别分子的聚合物液膜电极对葡萄糖检出限为0.2 mM,线性范围为1-100 mM,实现了对葡萄糖的高选择性检测且不受干扰物质的影响。将此电位型传感器应用于实际血样的检测,所得结果与商品化的血糖仪相比数据吻合。此研究方法的建立为临床医学中血糖的测定提供了新的思路。2、发展了基于硼酸识别的固体接触式电极电位型葡萄糖传感器。本研究建立了具有离子-电子传导特性的导电聚合物聚辛基噻吩(POT)和C60作为传导层的固体接触式电极和无传导层的固体接触式电极。以DBA作为识别分子,掺杂TDDA+Cl-的聚合物液膜作为电极的敏感膜,通过传导层的离子-电子传导作用,将溶液中葡萄糖浓度的变化间接转换成电信号,据此实现了对葡萄糖的检测。本研究突破了传统离子选择性电极需要内充液的缺点,通过对传导层材料的优化,建立了一种新型的固体接触式电极电位型葡萄糖传感器,为发展便携式、微型化的葡萄糖传感器提供了新方法。
[Abstract]:In recent years, the increasing number of diabetes patients worldwide has aroused great attention to diabetes, and researchers in various fields have been interested in glucose sensors. At present, the most widely used blood glucose sensor is an amperometric glucose sensor. Because the glucose sensor is easily affected by the activity of glucose oxidase, the development of non-enzymatic glucose sensor is a hot topic. In this paper, a series of diboric acid compounds were designed and synthesized by using the properties of boric acid compounds which recognize sugar and calculated by DFT theory. The stable boric acid compound was used as the recognition molecule of glucose instead of the inactivated enzyme, and the anion potential response could be produced on the ion selective electrode of 42 alkyl doped polymer membrane. A potentiometric glucose sensor based on boric acid recognition was established, and its selectivity and sensitivity were studied. The main contents are as follows: 1. A new method of liquid membrane electrode potentiometric glucose sensor based on boric acid recognition is developed. On the basis of the properties of boric acid binding with 1t2- or 1ta-3-dihydroxyl compounds and the calculation of DFT theory, three kinds of diboric acid compounds, DBA- DBA1 and DBA2, were designed and synthesized. By exploring the photophysical properties and electrochemical properties of these three borates and borate bound to glucose, the selection of recognition molecules, the concentration of recognition molecules and the pH of buffer solution were optimized. 10-5 M DBA was selected as the recognition molecule in pH 8.0 phosphoric acid buffer solution as the optimal condition for glucose detection. The detection limit of glucose is 0.2 mm and the linear range is 1-100 mm by using the polymer liquid membrane electrode with DBA as the recognition molecule. The detection of glucose is highly selective and unaffected by interfering substances. The potential sensor is applied to the detection of actual blood samples, and the results are in agreement with the commercial glycometer data. This method provides a new idea for the determination of blood glucose in clinical medicine and develops a solid contact electrode potentiometric glucose sensor based on boric acid recognition. In this study, solid contact electrodes with conducting polymer polyoctylthiophene (POT) and C60 as conducting layers and solid contact electrodes without conducting layer were established. Using DBA as the recognition molecule and TDDA Cl- doped polymer liquid film as the sensitive membrane of the electrode, the change of glucose concentration in the solution is indirectly converted into an electrical signal through the ion-electron conduction in the conduction layer. On the basis of this, the detection of glucose was realized. In this study, the shortcoming of the traditional ion selective electrode needed to be filled with liquid was overcome. By optimizing the conductive layer material, a new type of solid contact electrode potentiometric glucose sensor was established to develop portable glucose sensor. The miniaturized glucose sensor provides a new method.
【学位授予单位】：大连理工大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：R587.1;TP212

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