基于空间分辨的光电化学生物传感新方法及肿瘤标志物多元分析研究

Photoelectrochemical (PEC) biosensing technique has attracted great attentions because of its superior merits such as high sensitivity, simple instruments, and easier to miniaturization. However, the PEC biosensing methods based on the single signal response mode limit its capability in multiplex analysis. In addition, the sensitivity and selectivity of the PEC bioassay still need to be improved. The objective of this project is to construct the spatial-resolved PEC biosensing platform for the sensitive and multiplexed detection of tumor markers. The spatial-resolved electrode array was used for the construction of the platform. Notable metal-graphite-like carbon nitride (g-C3N4)-based heterojunctions with good stability and high photoelectric conversion efficiency were used as the matrix of the photoelectrode. The detection sensitivity of the method would be improved by using the amplification protocols such as redox cycling, energy transfer. The main contents of this project are as follows: (1) The synthesis of notable metal-g-C3N4-based ternary heterojunctions with high photoelectric conversion efficiency and good stability; The exploration of the mechanism and efficiency of the PEC enhancement; (2) The design and assembly of spatial-resolved electrode array and the construction of the PEC sensing platform; (3) The study of the sensitivity enhancement using the techniques such as redox cycling and energy transfer; (4) The application of the method for sensitive and multiplexed detection of multiple tumor markers and the early diagnosis of tumors. The proposed project would provide a novel strategy for the sensitive, multiplexed detection, and diagnosis of tumor.

光电化学（PEC）检测由于灵敏度高、装置简单、易于微型化等优点备受关注，近年来进展迅速。然而，目前的PEC检测主要是基于单信号响应模式，方法的多元分析能力受到限制。此外，PEC体系的灵敏度和选择性也还有待进一步提升。本项目拟将空间分辨技术引入PEC体系，利用贵金属-碳化氮基三元异质结纳米材料的诸多优点，结合氧化还原循环等信号放大技术和适配体、抗体的高特异性，构建空间分辨型PEC生物传感新平台及肿瘤标志物灵敏、多元检测新方法。主要内容有：（1）合成高光电转换效率、高稳定性贵金属-碳化氮基三元异质结纳米材料，探索光电信号增强作用机制；（2）设计、组装空间分辨型电极阵列并构建光电传感平台；（3）利用氧化还原循环等信号放大策略提高灵敏度；（4）将发展的新方法应用于肿瘤标志物的高灵敏、多元检测及早期诊断。本项目将为复杂生物样品的灵敏、多元检测及肿瘤诊断提供新技术和新方法，具有重要科学意义和应用价值。

光电化学（PEC）检测由于灵敏度高、装置简单、易于微型化等优点备受关注，近年来进 展迅速。然而，目前的PEC检测主要是基于单信号响应模式，方法的多元分析能力受到限制。此外，PEC体系的灵敏度和选择性也还有待进一步提升。基于此，项目合成了一系列具有高光电转换效率、高稳定性的二元、三元异质结纳米材料，并对其构效关系进行了系列表征，对异质结构电荷传输机制进行了探索；将空间分辨技术、电位分辨技术、自供能传感平台和劈裂式检测模式有效结合，利用异质结纳米材料和生物识别元素构建了光电传感界面；研究了CC氧化还原循环、光生空穴诱导的CC氧化还原循环等信号放大策略在PEC体系中的适用性，并对光电体系中氧化还原机制进行了探索，将能量转移、酶放大策略等信号放大策略与生物识别元件相结合，提高灵敏度，并开展了传感界面探针分子与靶分子结合研究；项目的成功实施为肿瘤标志物、心肌标志物等疾病标志物的高灵敏、多元、准确PEC检测提供了新方法和新技术。项目已经完成了计划内容，项目执行期内在Analytical Chemistry、Biosensors and Bioelectronics、Chemical Communications、Sensors and Actuators B、Analytica Chimica Acta、Analyst等国际SCI期刊上发表论文34篇（其中1区论文9篇，二区论文12篇），出版专著1部，授权国家发明专利1件。. 项目的开展为复杂生物样品的灵敏、多元检测及肿瘤、心肌疾病诊断提供了新技术和新方法，具有重要科学意义和应用价值。

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