多功能材料在光学阵列传感器中的应用研究
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摘要
在公共安全、环境监测、医学检测等领域普遍存在着对快速、灵敏、高通量、小型化检测仪器的需求。以阵列分析为基础的阵列传感器采用了人工模拟嗅觉系统的传感模式，可以实现平面上多点信息的同时获取，极大地提高了分析效率和检测通量，为小型化仪器的发展提供了新的契机。目前，发展用于阵列传感器的新传感材料和相应的传感机理仍是阵列传感器研究的主要方向。本论文研究了基于DNA-金纳米颗粒体系的比色阵列传感器和基于氧化石墨烯的三维光谱阵列传感器，合成了基于石墨烯和配位聚合物的新多功能材料，发展了基于有机电致发光材料和器件的新传感模式。主要成果包括：
1.系统研究了多种蛋白质在不同核酸适配体-金纳米颗粒体系上的比色响应行为，发现响应信号与蛋白质的物理化学性质及核酸适配体的结构有密切的关系。根据同一样品在不同识别单元上响应信号不同、不同样品在同一识别单元上响应信号也不同的现象，设计了基于新原理的阵列传感器，实现了对不同生物分子的快速、高灵敏和可视化检测。
2.研究了蛋白质对氧化石墨烯的内源性荧光、催化活性和自组装性质的影响，建立了氧化石墨烯的荧光、比色和浊度三维光谱阵列传感器，实现了对蛋白质的识别检测，扩展了用于单点多维信息获取方式的传感材料和传感模式。研究了氧化石墨烯在等离子体共振基质上的荧光增强行为。通过控制合成不同尺寸和厚度的银膜，实现了氧化石墨烯荧光10倍的增强。研究了多种金属离子对氧化石墨烯荧光增强行为的影响，实现了对不同种类金属离子的区分。
3.研究了可用于多维阵列传感器的新的多功能材料的设计和可控合成方法。选取石墨烯作为载体，将四氧化三铁纳米颗粒与其复合，获得了同时具有过氧化物酶催化活性、磁性和电化学性能的多功能材料。
4.研究了基于发光电化学池原理的有机电致发光材料和器件，并在气体传感中获得应用。在具有高比表面积的平面电极结构的器件上，光电双重信号会对氧气产生快速可逆的响应。基于这种传感器微阵列实现了对氧气含量的检测。
In the areas such as public safety, environmental monitoring and medical diagnosis,there is a widely requirement for fast reponse, sensitive and high-throughput sensorswith miniaturization. A sensor array is an artificial olfactory system based on the arrayanalysis method. On an array, information from different sensing units could becollected simultaneously, and this sensing mode is an effective way for theminiaturization of sensing device. At the moment the research of sensor array still focuson developing new sensing materials and methods. In our present work, we developedthe AuNP-based colorimetric sensor array and graphene oxide (GO)-basedtriple-channel sensing device. Also we synthesized new multi-funtional materials basedon graphene and coordination polymers, and developed new sensing methods withorganic light-emitting device. The main contents of the present dissertation are asfollows:
1. A new AuNP-based colorimetric sensor array for proteins detection anddiscrimination has been developed with three reported protein aptamers as nonspecificreceptors. The proteins at relatively low level could be well distinguished with nakedeye. The sensor array can also be used for the discrimination of cancerous fromnoncancerous cells.
2. The fluorescence, catalytic activity and assembly behavior of GO afterinteraction with proteins has been studied. As different proteins give distinct influencepatterns, proteins discrimination could be achieved on the triple-channel device in a‘lab-on-graphene’ approach. At the same time, a significant enhancement (~10fold) influorescence intensity is observed from GO on Ag substrate as compared to that onglass. The influence of Ag substrate metal size is investigated.
3. The design and synthesis of multi-functional materials for sensor array has beendeveloped. Fe3O4nanoparticles are anchored on reduced graphene oxide, and thenanocomposites exhibit peroxidase-like activity, electrochemical and magneticproperties. Superhydrophobic zinc coordination polymers particles (CPPs) withdifferent shapes are synthesized and ZnO calcined from these CPPs also exhibitsuperhydrophobic property and good photocatalytic activity.
4. The application of light-emitting electrochemical cells (LECs) for gassensing has been studied. The sensor is realized on an improved planar light-emittingdevice, and the current and light intensity show fast and reversible responses to oxygen.The LEC sensor microarray could be used for quantitative analysis of oxygenconcentration.
1.系统研究了多种蛋白质在不同核酸适配体-金纳米颗粒体系上的比色响应行为，发现响应信号与蛋白质的物理化学性质及核酸适配体的结构有密切的关系。根据同一样品在不同识别单元上响应信号不同、不同样品在同一识别单元上响应信号也不同的现象，设计了基于新原理的阵列传感器，实现了对不同生物分子的快速、高灵敏和可视化检测。
2.研究了蛋白质对氧化石墨烯的内源性荧光、催化活性和自组装性质的影响，建立了氧化石墨烯的荧光、比色和浊度三维光谱阵列传感器，实现了对蛋白质的识别检测，扩展了用于单点多维信息获取方式的传感材料和传感模式。研究了氧化石墨烯在等离子体共振基质上的荧光增强行为。通过控制合成不同尺寸和厚度的银膜，实现了氧化石墨烯荧光10倍的增强。研究了多种金属离子对氧化石墨烯荧光增强行为的影响，实现了对不同种类金属离子的区分。
3.研究了可用于多维阵列传感器的新的多功能材料的设计和可控合成方法。选取石墨烯作为载体，将四氧化三铁纳米颗粒与其复合，获得了同时具有过氧化物酶催化活性、磁性和电化学性能的多功能材料。
4.研究了基于发光电化学池原理的有机电致发光材料和器件，并在气体传感中获得应用。在具有高比表面积的平面电极结构的器件上，光电双重信号会对氧气产生快速可逆的响应。基于这种传感器微阵列实现了对氧气含量的检测。
In the areas such as public safety, environmental monitoring and medical diagnosis,there is a widely requirement for fast reponse, sensitive and high-throughput sensorswith miniaturization. A sensor array is an artificial olfactory system based on the arrayanalysis method. On an array, information from different sensing units could becollected simultaneously, and this sensing mode is an effective way for theminiaturization of sensing device. At the moment the research of sensor array still focuson developing new sensing materials and methods. In our present work, we developedthe AuNP-based colorimetric sensor array and graphene oxide (GO)-basedtriple-channel sensing device. Also we synthesized new multi-funtional materials basedon graphene and coordination polymers, and developed new sensing methods withorganic light-emitting device. The main contents of the present dissertation are asfollows:
1. A new AuNP-based colorimetric sensor array for proteins detection anddiscrimination has been developed with three reported protein aptamers as nonspecificreceptors. The proteins at relatively low level could be well distinguished with nakedeye. The sensor array can also be used for the discrimination of cancerous fromnoncancerous cells.
2. The fluorescence, catalytic activity and assembly behavior of GO afterinteraction with proteins has been studied. As different proteins give distinct influencepatterns, proteins discrimination could be achieved on the triple-channel device in a‘lab-on-graphene’ approach. At the same time, a significant enhancement (~10fold) influorescence intensity is observed from GO on Ag substrate as compared to that onglass. The influence of Ag substrate metal size is investigated.
3. The design and synthesis of multi-functional materials for sensor array has beendeveloped. Fe3O4nanoparticles are anchored on reduced graphene oxide, and thenanocomposites exhibit peroxidase-like activity, electrochemical and magneticproperties. Superhydrophobic zinc coordination polymers particles (CPPs) withdifferent shapes are synthesized and ZnO calcined from these CPPs also exhibitsuperhydrophobic property and good photocatalytic activity.
4. The application of light-emitting electrochemical cells (LECs) for gassensing has been studied. The sensor is realized on an improved planar light-emittingdevice, and the current and light intensity show fast and reversible responses to oxygen.The LEC sensor microarray could be used for quantitative analysis of oxygenconcentration.
引文
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