稀土纳米材料电化学发光性能及生物传感研究

This project was planed to study the electrochemiluminescence (ECL) property of rare earth nanomaterial and its applications in the field of biosensor. The morphology and size controlled rare earth nanomaterials would firstly be prepared via chemical liquid routes, and characterized by various techniques so as to analyze their elemental components, valence configurations and optical properties. Then, the electrochemical behavior of the prepared materials would be investigated in order to construct the model of the direct electron transfer (DET). For the purpose of fully studying the ECL property of rare earth nanomaterials, various experimental parameters, such as the different rare elements, scan potentials and co-reactants, would be employed to observe their effects on the ECL emission intensity. The ECL mechanism of rare earth and the optimistic conditions for the maximum emission intensity were schemed to be investigated. Via the utilization of ECL property, the novel and high-effected rare earth ECL biosensors were proposed to be fabricated. The ECL changes before and after the interaction between the probe and target analyte were proposed to be detected to achieve the target detection. This project plays an important role in the development of novel ECL material. In the meantime, it provides the solid scientific values to open the new high-effected utilization of rare earth, to expend rare earth's application scopes, so as to change the regional resource advantages into economic advantages.

本项目主要研究稀土纳米材料的电化学发光（ECL）性能及其在生物传感领域的应用。首先通过各种液相化学方法制备具有形貌和大小可控的稀土纳米材料；并对所制备的纳米材料进行表征，分析其元素组成，价态结构，光学性质等。测试稀土纳米材料的电化学行为，构建其直接电子传递模型。详细研究稀土纳米材料的电化学发光性能。分析不同稀土元素、不同扫描电位和不同共反应物对稀土ECL 发射光强度的影响；探讨稀土ECL 发光机理；寻求稀土ECL 最大发光强度所需的实验条件。利用稀土材料良好的生物相容性和ECL 性能，构建新型高效的稀土ECL 生物传感器。通过对传感器与目标分析物反应前后的ECL 发光强度的变化，实现对目标物的检测。本研究项目不仅对研制新型电化学发光材料具有重要意义，同时为开辟稀土资源有效利用的新途径、扩展其应用范围、把地区资源优势变为经济优势提供重要的科研价值。

稀土元素因其特殊的4f电子层结构而具备多种特有的物化性质，在光电磁等方面有着重要的应用价值，但将稀土纳米材料用于电化学传感器领域的领域却鲜有报道。基于此，本项目主要研究稀土纳米材料的制备、表征、电化学性能及其在生物传感器中的应用。首先通过水热法、溶胶-凝胶法、电沉积法等方法制备得到Er2O3、Dy2O3、HoPO4、PrFeO3和Dy2(MoO4)3等系列稀土纳米材料及其多元复合纳米材料；利用扫描电子显微镜、透射电子显微镜、X射线衍射仪、X射线能谱仪、红外光谱仪和紫外－可见分光光度计等设备所制备的纳米材料进行表征，分析材料的形貌、结构、组成等性质；利用循环伏安法、电化学阻抗法等技术研究纳米材料的电子传递性能和电化学导电性能；通过对相关稀土纳米材料与其他纳米材料之间的相互作用制备得到系列复合纳米材料，并将其用于化学修饰电极，实现了对亚硝酸盐等小分子的无酶检测；利用纳米材料良好的生物相容性将血红蛋白、葡萄糖氧化酶等酶固载到纳米材料用于构建生物传感器，实现对过氧化氢、葡萄糖等生物小分子的电化学检测。本项目研究内容表明相关稀土纳米材料具有良好的电子传递性能，能够很好的促进电子在电极表面和电解液之间的传递。实验结果还进一步证实相关稀土纳米材料具有良好的生物相容性，蛋白、酶等生物分子与稀土纳米材料结合后仍然可以保持其相应的生物活性。在本项目资助下，迄今共在Journal of The Electrochemical Society(影响因子：3.662)、 Microchimica Acta(影响因子：5.705)、Chemistry letters、《无机化学学报（英文版）》、《高等学校化学学报》和《分析化学》等期刊上发表SCI收录论文8篇，申请发明专利1项，培养研究生6名，对照项目计划书，较好的完成了预期的研究目标。