过渡金属氮化物纳米阵列电极的制备及电分析化学应用研究

The electroanalytical chemical method has great and valuable application in food detection, environmental analysis and disease diagnosis. Although great progress has been made, to reduce the signals of background and to improve the analytical reproducibility and stability are still important challenge to domestic and overseas researchers. This project will be started on the basis that comparing with the electrodes modified by disordered nanometer materials, the high orderly nanoarray electrodes have been more evident merits, like greater quantum effect, larger surface area, and the advantages of easier to control of size and shape, as well as the transition metal nitride has more evident merits, like good biocompatibility, high electric catalytic activity, high electrical conductivity, etc. Firstly, transition metal oxide nanoarray will be assembled directly onto the electrode via the hydrothermal method or electrodeposition method. Then, “conformal transformation” will be carried out from transition metal oxide nanoarray into transition metal nitride nanoarray. Using a variety of characterization methods, the relationship between the composition, morphology and size of the prepared nanoarray electrode and its electrochemical properties will be analyzed combined with computational chemistry related theory. After the mechanism of molecular recognition on the sensing interface of the prepared nanoarray electrode is explored, different strategies for signal amplification will be designed and kinds of electroanalytical chemical sensor will be fabricated for ultrasensitive detection of various analytes. Based on this project, an important scientific significance will be got from revealing the law of the influence of reproducibility and stability, and a new train of thought will be provided for designing high sensitive electroanalytical chemical sensors.

电分析化学方法在食品及环境分析和疾病诊断中有较大应用价值，但是降低背景信号、提高分析重现性及稳定性仍是国内外学者面临的重要挑战。本项目基于有序的纳米阵列电极具有比无序纳米材料修饰电极更加突出的量子效应、更大的表面积、尺寸及形貌更易调控等优点，以及过渡金属氮化物具有生物相容性好、电催化活性高、导电率高等优点，采用水热法和电沉积法在电极表面直接组装过渡金属氧化物纳米阵列，然后将其“保形”转化为氮化物，由此制得形貌、组成可控的过渡金属氮化物纳米阵列电极。利用各种表征手段分析其组成、形貌及尺寸，结合计算化学相关理论，分析其理化特性，通过探索传感界面分子识别机制，设计信号放大策略，从而发展重现性好、稳定性高的新型电分析化学传感器，实现对小分子化合物和大分子蛋白质的高灵敏检测。本项目的开展，为揭示电分析化学重现性和稳定性的影响规律有重要的科学意义，为设计制作高灵敏电分析化学传感器提供了一种新的思路。

电分析化学传感技术凭借其诸多优势，成为了进入二十一世纪以来优先发展的十大顶尖技术之一。电分析化学技术所开展的研究和应用均离不开电极的使用，但电极的修饰过程和科研人员操作的熟练程度对于传感界面的稳定性、重现性以及导电性所产生的影响，仍是国内外科研工作者不得不面对的重要挑战。本项目紧紧围绕开发新型传感检测平台这一主题，首先基于有序的纳米阵列电极具有比无序纳米材料修饰电极更加突出的量子效应、更大的表面积、尺寸及形貌更易调控等优点，以及过渡金属氮化物具有生物相容性好、电催化活性高、导电率高等优点，采用水热法或电沉积法在电极表面直接组装过渡金属氧化物纳米阵列，然后将其“保形”转化为氮化物，由此制得形貌、组成可控的过渡金属氮化物纳米阵列电极。利用各种表征手段分析其组成、形貌及尺寸，分析其理化特性。然后，设计科学有效的信号放大策略和传感分析策略，结合抗体-抗原的特异性免疫识别、DNA识别、分子印迹识别等对目标分析物的特异性识别方法，探索传感界面分子识别机制。最后，创新性地将过渡金属氮化物纳米阵列电极直接作为传感平台，将其和多种分子识别机制相结合，通过探索过渡金属氮化物纳米阵列电极的可控制备方法以及与不同分子识别机制的结合方法，针对环境污染物、食品污染物及肿瘤标志物等不同目标检测物，利用电化学、光电化学及电致化学发光等技术手段，设计不同信号放大策略，从而制备了一系列灵敏度高、重现性好、稳定性高的电分析化学传感器，对揭示电分析化学传感检测性能的影响规律有重要的科学意义，也为发展新型传感分析策略和传感平台提供了一种新的发展方向。