纳米粒子@MOFS复合材料模拟生物过氧化物酶的研究
发布时间：2018-07-27 18:43
【摘要】：本文主要针对纳米粒子与金属-有机骨架材料衍生复合材料的制备及其过氧化物酶的性能进行研究。天然的过氧化物酶在生物界中是无处不在的,所有的生物都依赖于酶进行着生命活动。它是具有生物催化功能的高分子物质,其研究与应用历史已有200多年。作为一种特殊的催化剂,生物酶有着高催化效率和专一性,这使其在药学、化工制造和环境分析等领域内有着普遍的切实应用。然而天然酶本身也具有一定的缺点和局限性,例如分离提纯困难、结构稳定性低、价格昂贵、易失活和储藏使用不便。因此,具有生物过氧化物酶活性的微纳米材料便成为人们所追求的目标。近几年来,金属-有机骨架材料(MOFs)是成长快速的新型高孔隙材料,超高的比表面积、孔道结构可调、丰富的骨架构造等一些优良的特征,使其一跃成为模拟生物酶体系中的理想材料。本文合成了三种 Fe(Ⅲ)-MOFs 材料 MIL-n(n=88A、88B、88B-NH2)和一种Cu(Ⅱ)-MOFs材料MOF-199,通过负载多种纳米粒子Fe_3O_4、Pt、Au等多种纳米粒子,成功制备出多种MOFs复合材料。对于Fe_3O_4@MOF-199材料,通过控制不同的煅烧条件,获得Fe_3O_4@Cu/C和Fe_3O_4@CuO/Cu_20两种衍生复合材料。本文以3,3',5,5'-四甲基联苯胺(TMB)为实验底物,研究了 Fe(Ⅲ)-MOFs、Cu(Ⅱ)-MOFs材料及其衍生复合材料的生物过氧化物酶活性,实验结果显示所制备的MOFs衍生复合材料具备优异的生物过氧化物酶活性。通过研究发现,Fe_3O_4@MOF-199的衍生复合材料Fe_3O_4@Cu/C和Fe_3O_4@CuO/Cu_20均具有较高的过氧化物酶活性,且前者高于后者,因此我们分析探讨了 pH、温度(T)以及H_2O_2浓度等因素对生物过氧化物酶活性的影响。研究结果显示出Fe_3O_4@Cu/C在pH=2.5、T=50℃、CH_2O_2=8 mM时酶具有最高的催化活性。模拟过氧化物酶动力学研究结果表明:Fe_3O_4@MOF-199的衍生复合材料催化反应符合典型的米氏方程动力学模型;Fe_3O_4@Cu/C对底物H_2O_2、TMB的米氏常数Km值均小于Fe_3O_4@CuO/Cu_2O的Km值,由此可知,Fe_3O_4@Cu/C对底物有着强的亲和力。将Fe_3O_4@MOF-199及其衍生复合材料用于有代表性的纺织染料物亚甲基蓝(MB)的催化降解,在80℃条件下0.05 mg/mL Fe_3O_4@Cu/C在5 min内完全降解亚甲基蓝,较其他MOFs材料有着更强的催化降解能力,在分析和检测环境有机污染物等领域有着巨大的应用远景。
[Abstract]:In this paper, the preparation and peroxidase properties of nano-particles and metal-organic matrix derived composites were studied. Natural peroxidase is ubiquitous in the biological world, and all living things depend on it for life. It has been studied and applied for more than 200 years. As a special catalyst, biological enzyme has high catalytic efficiency and specificity, which makes it widely used in pharmaceutical, chemical industry and environmental analysis. However, natural enzymes also have some disadvantages and limitations, such as difficulty in separation and purification, low structural stability, high price, inactivation and inconvenient storage. Therefore, micro- and nanomaterials with biological peroxidase activity have become the goal that people pursue. In recent years, metal-organic skeleton material (MOFs) is a new type of high porosity material with rapid growth, high specific surface area, adjustable pore structure, rich skeleton structure, and so on. It has become an ideal material in mimic biological enzyme system. In this paper, three kinds of Fe (鈪，
本文编号：2148800
[Abstract]:In this paper, the preparation and peroxidase properties of nano-particles and metal-organic matrix derived composites were studied. Natural peroxidase is ubiquitous in the biological world, and all living things depend on it for life. It has been studied and applied for more than 200 years. As a special catalyst, biological enzyme has high catalytic efficiency and specificity, which makes it widely used in pharmaceutical, chemical industry and environmental analysis. However, natural enzymes also have some disadvantages and limitations, such as difficulty in separation and purification, low structural stability, high price, inactivation and inconvenient storage. Therefore, micro- and nanomaterials with biological peroxidase activity have become the goal that people pursue. In recent years, metal-organic skeleton material (MOFs) is a new type of high porosity material with rapid growth, high specific surface area, adjustable pore structure, rich skeleton structure, and so on. It has become an ideal material in mimic biological enzyme system. In this paper, three kinds of Fe (鈪，
本文编号：2148800
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