稀土纳米模拟酶的制备及其在生物传感中的应用研究

The project intends to prepare series of rare-earth doped nanomaterials with different composition, morphology, particle size, surface modification, valence, charge, etc (including the hollow structure, core-shell structure, cubic structure, nano ball, nanorods, etc.), through solvothermal technology and controlling conditions of synthesis and modification. These nanometer materials will be used as nano-mimic enzymes. By the means of electrochemiluminescence analysis method, the relationship between the catalysis performance of rare-earth nano enzymes mimic and its structure and morphology will be studied systematically. To improve their stability, specificity and catalytic efficiency, we would regulate the catalytic activity of rare-earth nano-mimic enzymes and explain the phenomenon theoretically. Meanwhile, by selecting the efficient reaction agent, or using functional materials to modify electrochemiluminescence system, to improve the electrochemiluminescence performance. The final purpose is to develop electrochemiluminescence systems based on the rare-earth nano-mimic enzymes, applying to biological analysis and realizing rapid, accurate, cheap, high sensitive, high selective detection of the antigen, antibody, disease markers, harmful substances in food and environment, which would provide new materials, new technology and new method in the areas of disease diagnosis, detection of pests in food and environment.

本项目拟采用溶剂热法，控制合成和修饰条件，制备具有不同组成、形貌、粒径、表面修饰、价态、电荷等系列稀土掺杂纳米材料（包括空心结构，核壳结构，立方结构，纳米球，纳米棒等），用作纳米模拟酶。以电化学发光分析方法作为检测手段，系统地研究稀土纳米模拟酶催化性能与其结构、形态之间的关系，调控稀土纳米材料模拟酶催化活性，提高它们的稳定性、特异性和催化效率，并从理论上给予解释。同时，通过选择高效的共反应剂，或者采用功能材料修饰电化学发光体系，改进提高电化学发光性能。建立基于稀土纳米模拟酶的电化学发光分析体系，应用于生物传感，实现抗原、抗体、疾病标志物、食品和环境中有害物等物质的快速、准确、廉价、高灵敏、高选择性的检测，以期为疾病诊断、食品和环境中有害物的分析检测等领域提供新材料、新技术、新方法。

本项目采用水热法、溶剂热法以及共沉淀法，制备了系列系列稀土掺杂纳米材料，包括NaYF4:Yb,Er/Mn纳米棒，NaYF4:Yb,Tm/Mn纳米棒，Li+-NaYF4:Yb,Er纳米粒子， NaGdF4:Yb,Er@NaYF4核壳结构纳米粒子，NaYF4:Yb,Er,Gd纳米粒子，NaYF4:Yb,Tm,Gd纳米粒子，NaYF4:Yb,Er/NaGdF4核壳结构纳米粒子以及Fe3O4@Au纳米过氧化物模拟酶。对所制备的稀土掺杂纳米材料进行了表面功能化修饰，并进行了系统的表征。构建了基于稀土掺杂纳米材料和模拟酶的光致发光传感模型、化学发光传感模型、电化学发光传感模型，建立了癌症标记物-人体前列腺抗原、甲胎蛋白，鼠伤寒沙门氏菌，焦磷酸酶，酪氨酸酶，过氧化氢，尿酸，酪胺，谷胱甘肽，半胱氨酸，抗坏血酸，Hg2+，S2-，人瘦素等疾病标记物、食品和环境中有害物的高灵敏度、高选择性的检测方法，实现了抗原、抗体、疾病标志物、食品和环境中有害物等物质的快速、准确、廉价、高灵敏、高选择性的检测。本项目的研究成果为疾病诊断、食品和环境中有害物的分析检测等领域提供了新材料、新技术、新方法。