上转换交叉响应传感芯片的制备与痕量多底物检测应用研究

The cross-reactive sensor array chip offers multiplex differential sensing response signal to process the multi-analytes discrimination. The critical requirement for successful multi-analyte recognition is to acquire abundant sensing information. However, the “multi to multi” sensor chip needs large numbers of serial probe compounds, which involve complicated chemical synthesis and valid compound screening..In this project，the triplet-triplet annihilation (TTA) upconversion materials are introduced into the optical cross-reactive sensor array. The ratio method and time-resolved detection channel are applied, which can effectively reduce the interference of the environmental factors and provide differentiated sensing signals more efficiently to improve the accuracy of detection. The TTA complex probes are loaded on single dispersed silica microsphere to prepare the printable "ink" materials. Inspired by the fog-collecting structure on Stenocara beetle’s back, a photonic crystal microchip with hydrophilic–hydrophobic micropattern was fabricated by inkjet printing. This cross-reactive sensor array chips based on upconversion materials can be used to realize high-sensitive ultratrace detection in environmental monitoring and biomedicine testing areas.

交叉响应传感阵列通过对不同被检测物的差异化信号进行处理，可以实现对多底物的识别。传统“多对多”方式的分析方法，为了要获得足够差异化信号，存在对探针需求种类量大、制备复杂、探针有效性筛选效率低等缺点，在实际应用过程中显现出巨大的局限性。.本项目首次把基于给受体能量传递的三线态-三线态湮灭（TTA）上转换体系引入到交叉响应传感阵列，增加时间分辨的信道，应用具有自校准特性的比率法，可更高效率构建传感阵列，提高对多底物的检测能力。.再将TTA上转换复合探针负载于单分散二氧化硅微球，制备成为可打印“墨水”。利用喷墨打印技术与自组装技术相结合的精细打印技术，通过对自然界沙漠甲虫背部结构集雾功能的模仿，构建以亲疏水图案化为基底，阵列单元具有光子晶体结构的上转换交叉响应传感芯片。利用亲疏水图案化的可控去浸润实现浓度富集，以及利用光子晶体对交叉传感信号的差异化增强，又进一步对芯片检测灵敏度实现了了双重提升。

通过使用数量更少、性能更优的探针分子获得更多更稳定的差异化传感信号，是提高多底物分析检测效率的重要突破口。三线态-三线态湮灭上转换发光材料，在多底物检测的光学交叉响应传感阵列设计中显示了很大的潜力。四年来，围绕项目“上转换交叉响应传感芯片的制备与痕量多底物检测应用研究”课题，开展了具有传感响应功能三重态分子探针的设计，TTA上转换探针体系的构建，以及底物检测等相关研究，取得主要相关创新性研究成果如下：.1.构建了基于TTA-UC的比率荧光探针，实现了对温度的可视化监测；.2.发展了以柠檬烯为代表的TTA-UC光化学除氧介质；.3.构建了系列基于TTA-UC的比率荧光探针，分别实现了对Fe3+，Mg2+，Hg2+以及pH等的检测；.4.多带隙光子晶体增强TTA上转换，为提高TTA上转换效率提供了新途径；.5.开发了可打印上转换余辉防伪材料；.6.开发了基于TTA-UC的固态白光发射材料。