|Place of Conferral||北京|
|Keyword||氮、硫共掺杂介孔碳 循环伏安法 差示脉冲伏安法 邻苯二酚 对苯二酚 Pb(Ii)|
酚类化合物和有毒重金属物质都属于环境污染物，严重威胁人们健康和生命。因此，构建简便、灵敏和快速的传感器检测其含量是非常必要的。在酚类和重金属Pb(II)检测中，电化学传感器具有响应迅速、灵敏度高、选择性好、操作简单、稳定性强等优点，成为研究开发的热点。在电化学检测中，修饰电极的材料对电极的性能起到至关重要的作用。因此，电极材料的设计及合成是非常关键的。本文研究的主要内容是氮、硫共掺杂的介孔碳材料合成及其修饰玻碳电极(GCE)构建电化学传感器用于检测苯二酚及重金属Pb(II)。实验结果表明，构建的电化学传感器具良好的选择性、较高的稳定性、较低的检测限及较强的抗干扰能力。具体工作如下：1 氮、硫共掺杂的介孔碳修饰GCE同时检测HQ和CC对苯二胺和硫酸中和反应经碳化一步法制备氮、硫共掺杂的介孔碳(N,S-MPC)，经透射电镜(TEM)和氮气物理吸附仪分别表征其型貌和比表面积等结构性质。N,S-MPC修饰GCE制备电化学传感器，借助循环伏安法(CV)和差示脉冲伏安法(DPASV)对HQ、CC电化学性能进行探究。结果表明该修饰电极能够明显区分CC、HQ的氧化峰，有效提高其响应性和灵敏度。对浓度1~110 μM范围内的CC、HQ呈现良好的线性相关，检测限分别为0.209 μM和0.0506 μM。2 氮、硫共掺杂蛋黄壳结构介孔碳合成及其电化学检测Pb(II)氮、硫共掺杂蛋黄壳结构介孔碳(N,S-YSPCMSs)以巯基修饰的二氧化硅为模板，经聚合物高温煅烧方法合成，利用SEM、TEM、XPS、氮气物理吸附仪分别对材料进行表征。900 oC碳化的材料与Nafion-Bi(III)复合物修饰GCE制备了Pb(II)电化学传感器。借助DPASV对Pb(II)电化学性能进行研究，结果显示修饰的电极表现出优异的电化学性能，如：高的选择性和灵敏度。该修饰电极对浓度4~160 μg L-1的Pb(II)表现出很好的线性相关，最低检测限为0.49 μg L-1。同时，在检测鱼血清Pb(II)的测试中表现出良好的回收率，表明该电化学传感器在实际重金属检测中有着良好的应用前景。3 氮、硫共掺杂蜂窝状介孔碳合成及修饰GCE对Pb(II)的电化学检测性能研究实验制备了尺寸可调的氮、硫共掺杂蜂窝状介孔碳(N,S-PHCC)，并且探究了二氧化硅模板尺寸和碳化温度对检测Pb(II)电化学性能的影响。结果表明，以200 nm二氧化硅作为模板，在900 oC碳化合成的材料对检测Pb(II)响应电流值最大。制备的200-N,S-PHCC-900/Nafion/Bi/GCE电化学传感器对浓度0.75~120 μg L-1的Pb(II)表现出很好的线性相关，最低检测限为0.064 μg L-1。该电化学传感器在检测Pb(II)方面抗干扰能力、重复性、重现性及稳定性较好，在实际水样检测中具有良好的回收率。实验结果表明，200-N,S-PHCC-900/Nafion/Bi/GCE传感器可为实际水样的检测可提供一个平台。
Phenolic compounds and heavy metals are environmental pollutants, which is a serious threat to people's health and life. Therefore, it is necessary establish a simple method to detect the contents of these pollutants. Compared with the traditional analytic methods for phenyl dihydroxide and heavy metal detection, electrochemical sensor has the advantages of rapid response, high sensitivity, good selectivity, simple operation, good stability and so on. Thus, it has gradually become an alternative method for detection of the pollutants. In the electrochemical detection, the material of the modified electrode plays an important role in the performance of the electrode. Therefore, it is very vital for the design and synthesis of the materials. In this paper, we synthesise a novel nitrogen and sulfur co-doped mesoporou carbon and utilize them as electrode modifiers for detection the environmental pollutants of HQ, CC and Pb(II). The contents are as follows: 1 Simultaneous determination of catechol and hydroquinone based on nitrogen and sulfur co-doped mesoporous carbon modified electrodeThe nitrogen and sulfur co-doped mesoporous carbon (N,S-MPC) was synthesized by p-phenylenediamine neutralized with H2SO4 and then the solid mixture was directly calcined. The obtained material modified electrode was used to detect HQ and CC. The surface morphology and specific surface area of N,S-MPC were characterized by transmission electron microscopy (TEM) and nitrogen adsorption apparatus. Cyclic voltammetry (CV) and differential pulse voltammetry (DPASV) were employed to characterize the electrochemical properties of HQ and CC at the modified electrode. Experiment results showed that the oxidation peaks of CC and HQ were obvious distinguished. Also, the response and sensitivity have been greatly improved. The electrochemical sensor showed a wide liner range of 1~110 μM for both HQ and CC. The HQ and CC detection limits were about 0.056 μM and 0.209 μM, respectively. 2 Synthesis of nitrogen and sulfur co-doped yolk-shell porous carbon microspheres and their application for Pb(II) detection Nitrogen, sulfur co-doped co-doped yolk-shell porous carbon microspheres (N,S-YSPCMSs) were synthesized by combining silica templating strategy and high-temperature pyrolysis method. The as-prepared N, S-YSPCMSs were characterized by SEM, TEM, XPS and nitrogen adsorption apparatus. When applied as electrode components for Pb(II) detection, the N,S-YSPCMSs prepared at 900 oC showed enhanced electrochemical performance than their analogues obtained under other temperatures. The N,S-YSPCMSs based sensor showed a linear dependence over a notably wide Pb(II) concentration range of 4~160 μg L-1, with a detection limitation of 0.49 μg L-1. The electrochemical sensor was applied in detecting Pb(II) of fish serum samples with satisfying recoveries, indicating the developed N,S-YSPCMSs-900 is promising electrode components for electroanalysis.3 High electrochemical performance for Pb(II) detection based on N,S co-doped porous honeycomb carbon modified electrodes N,S co-doped porous honeycomb carbon (N,S-PHCC) with tunable size was successfully synthesized via a silica template and high-temperature pyrolysis method. We systematically investigate the effects of particle size and carbonization temperature on the electrochemical properties of Pb(II) detection. The results showed that the peak current response of Pb (II) was highest when the particle size was 200 nm and the carbonization temperature was 900 oC. The prepared 200-N,S- PHCC-900/Nafion/Bi/GCE electrochemical sensor showed a good linear range of 0.75~120 μg L-1 and a low detection limitation of 0.064 μg L-1. Moreover, the electrochemical sensor has a good anti-interference ability, excellent repeatability and reproducibility and good stability.
|徐瑞玉. 氮、硫共掺杂介孔碳对苯二酚和重金属离子电化学检测性能研究[D]. 北京. 中国科学院大学,2017.|
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