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不同形貌钼酸铁和钒酸铈的制备、表征及其模拟过氧化物酶活性研究

发布时间:2018-07-24 10:26
【摘要】:酶对很多化学反应的顺利进行起着决定性的作用,但由于大部分天然酶本质属于蛋白质或者RNA,对催化环境要求比较高,同时提取纯化也比较困难,所以很难大规模实际利用。人造模拟酶由于具有易制备、低成本、稳定性高、催化活性好等优点而成为有潜力的生物酶替代品,其中过氧化物模拟酶因在检测过氧化氢、葡萄糖等方面具有十分重要的意义而受到了广泛的关注。本研究通过水热合成法,采用不同反应条件,制备了Fe_2(MoO_4)_3-F(花状)、Fe_2(MoO_4)_3-P(片状)、Fe_2(MoO_4)_3-B(蝴蝶状)和Fe_2(MoO_4)_3-S(球状)四种形貌不同的钼酸铁纳米材料和CeVO_4-1.5(pH为1.5)、CeVO_4-2(pH为2)、CeVO_4-2.5(pH为2.5)和CeVO_4-3(pH为3)四种形貌不同的钒酸铈纳米材料,并使用TEM、FESEM?XRD?XPS、EDX、BET、Zeta电位测定等技术和手段对制备材料的形貌、组成、比表面积、Zeta电位等进行了表征,发现Fe_2(MoO_4)_3-F和CeVO_4-2具有相对最大的比表面积;酶活性实验表明Fe_2(MoO_4)_3-F和CeVO_4-2具有较好的过氧化物模拟酶性质并具有很好的重复利用性;通过对影响材料过氧化物酶活性的影响因素的研究,我们发现其酶活性与材料浓度、底物过氧化氢的浓度、反应的温度、pH等因素有关,其催化反应机制为乒乓机制;Fe_2(MoO_4)_3-F的最适反应条件为:Fe_2(MoO_4)_3-F 300μg/m L,H_2O_2 2.0 mM,反应温度25°C,反应pH4.0;CeVO_4-2的最适反应条件为:CeVO_4-2 300μg/mL,H_2O_2 2.0 mM,反应温度25°C,反应pH4.0;基于两种材料良好的过氧化物酶活性,我们建立了可视化检测过氧化氢的系统,对过氧化氢的检测限最低分别可达0.7和0.07μM,本研究不仅提供了一种快速、价廉、简便、灵敏的新型可视化H_2O_2检测方法,也为开发新型高效的模拟酶材料提供了基础。
[Abstract]:Enzymes play a decisive role in the smooth progress of many chemical reactions, but because most of the nature of natural enzymes belong to proteins or RNAs, the catalytic environment is very high, and it is difficult to extract and purify, so it is difficult to use on a large scale. Because of its advantages of easy preparation, low cost, high stability and good catalytic activity, artificial mimic enzymes have become potential substitutes for biological enzymes, in which peroxidase mimics are used to detect hydrogen peroxide. Glucose and other aspects are of great significance and have received extensive attention. In this study, different reaction conditions were adopted by hydrothermal synthesis. Four different morphologies of Fe_2 (MoO_4) 3-F (flowered) Feti2 (MoO_4) 3-P (flake) tip-Fe2 (MoO_4) 3-B (butterfly) and Fe_2 (MoO_4) 3-S (spherical) nanomaterials with different morphologies, such as CeVO_4-1.5 (pH 1.5) CeVO4-2 (pH 2), CeVO4-2.5 (pH 2.5) and CeVO_4-3 (pH 3), were prepared. The morphology, composition, specific surface area and Zeta potential of Fe_2 (MoO_4) 3-F and CeVO_4-2 were characterized by means of Tem Fesemer, XRDX, EDXX, and Zeta potential. The results showed that Fe_2 (MoO_4) 3-F and CeVO_4-2 had the largest specific surface area. The enzyme activity experiment showed that Fe_2 (MoO_4) 3-F and CeVO_4-2 had good properties of mimic peroxidase and had good reusability, and we found that the enzyme activity and material concentration were influenced by the factors affecting the activity of peroxidase. The concentration of substrate hydrogen peroxide, the temperature and pH of the reaction are related. The mechanism of catalytic reaction is the ping-pong mechanism. The optimum reaction conditions are: 1 Fe2 (MoO_4), 3 F 300 渭 g / m L ~ (-1), 3 ~ F 300 渭 g / m L ~ (-1) / L ~ (3) F ~ (300) 渭 g / m ~ (-1) / L ~ (-1) ~ 3 ~ (3) F ~ (-1), 20 ~ 2.0 mm / M, 25 掳C, pH _ 4.0 based on the optimum reaction conditions:% CeVO4-2 300 渭 g / mL H _ 2O _ 2O _ 2 2.0 mm, reaction temperature 25 掳C, reaction pH 4.0; based on the good peroxidase activity of the two materials, the optimum reaction conditions are as follows:% CeVO4-2 300 渭 g / mL H2O2 2.0 mm, reaction temperature 25 掳C We have established a visual detection system for hydrogen peroxide with the lowest detection limit of 0.7 渭 m and 0.07 渭 M for hydrogen peroxide, respectively. This study not only provides a new visual H_2O_2 detection method which is fast, inexpensive, simple and sensitive. It also provides a basis for the development of new and efficient mimic enzyme materials.
【学位授予单位】:国家海洋局第一海洋研究所
【学位级别】:硕士
【学位授予年份】:2017
【分类号】:TB383.1;O657.3

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