基于纳米材料表面化学发光的传感器阵列研究
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摘要
传感器阵列是传感器研究的活跃领域,它集成了单个传感器的功能,在食品安全、临床诊断、环境监测等领域有广泛的应用前景。光信号检测能够从强度、波长、发光寿命等方面提供丰富的识别信息,因此光学传感器阵列的研究最近得到了较快发展。本论文提出了基于纳米材料表面化学发光响应原理的传感器阵列,建立了快速筛选传感单元材料的新方法,发展了用于传感机理研究的分析表征手段,为传感器阵列的研究提供了新思路。研究内容包括:
1.提出了基于纳米材料表面化学发光响应原理的传感器阵列。系统研究了硫化氢、三甲胺、乙醇等不同种类的化合物在各种纳米材料表面的化学发光特性,发现不同的样品分子在同一种纳米材料表面的化学发光效率不同,同一种样品分子在不同纳米材料表面的化学发光效率也不同的现象。因此,样品分子在纳米材料表面发生催化反应所得到的发光信号可以提供分子的识别信息。根据这一现象,利用一组纳米催化材料设计了基于纳米材料表面化学发光的传感器阵列。
2.建立了快速筛选传感单元材料的新方法。设计了一组不同种类的负载贵金属的纳米氧化物催化材料,研究了纳米材料表面的化学发光性能与其催化活性之间的关系,发现纳米材料表面的化学发光性能与材料的催化活性之间存在着显著的相关性。这一方法不仅能够用于该传感器阵列所需要的传感材料的快速筛选,也能够用于催化材料的快速评价,对组合催化合成中高通量催化剂筛选有潜在的应用价值。
3.发展了用于传感机理研究的分析表征手段。研究了固体表面样品在介质阻挡放电低温等离子体中的解吸附/离子化现象,设计了新型常压质谱离子源,分别以阵列表面的氨基酸和爆炸物样品的分析为例,证明了该方法可用于阵列表面上痕量物质的实时、原位分析,为传感机理研究提供了必要的表征手段。这种离子源在其它化学反应过程的实时在线监测中具有潜在的用途。
Sensor array, which integrates the functions of multiple sensors, is one of the hot topics in the study of sensors. Sensor array has a wide variety of application areas including food and beverages, medical diagnostics, environmental monitoring, and a host of others. Abundant information can be provided by optical signals for the analyte identification, including luminescence intensity, wavelength, lifetime, etc. Thus, the rapid development for optical sensor arrays has been achieved recently. In the present dissertation, a sensor array of nanomaterial-based cataluminescence was developed. Based on this sensor array, a new way for rapid screening of sensor materials was reported. Furthermore, a new analysis technique was also designed for studying the sensing mechanism, which provides us a novel pathway for the research of sensor array. The main contents of the present dissertation are as follows:
1. A new sensor array based on nanomaterial-based cataluminescence was developed for analytes recognitions. By studying the cataluminescence behavior of sulfureted hydrogen, trimethylamine and ethanol on surfaces of nanomaterials, the specificity between cataluminescence signals and nanomaterials was established. The different cataluminescence responses were obtained both for the same analyte on different nanomaterials, and for the different analytes on the same nanomaterial. As a result, the optical information from the oxidation of analytes on the surfaces of nanomaterials can be used for analytes recognitions. Based on this phenomenon, an optical sensor array was developed with an array of different nanomaterials for analytes recognitions.
2. A new method for rapid screening of sensor materials was reported. A series of metal catalysts deposited on nanomaterials supports were prepared for studying the correlation between catalytic activities and cataluminescence responses for the CO oxidation. The well correlation between catalytic activities and cataluminescence intensities was established. Then, a cataluminescence-based imaging method was successfully used for the high-throughput screening of sensor materials.
3. A new analysis technique was designed for studying the sensing mechanism. An ambient ionization source for mass spectrometry was designed, which was based on desorption and ionization of analytes from the solid surfaces by the low temperature plasma of dielectric barrier discharge. The direct analysis of amino acids and explosives on the array surface was achieved, which demonstrated that the present method can be used for the real-time and in situ detection of trace analytes on the array surface. This provides us a novel pathway for studying the sensing mechanism.
1.提出了基于纳米材料表面化学发光响应原理的传感器阵列。系统研究了硫化氢、三甲胺、乙醇等不同种类的化合物在各种纳米材料表面的化学发光特性,发现不同的样品分子在同一种纳米材料表面的化学发光效率不同,同一种样品分子在不同纳米材料表面的化学发光效率也不同的现象。因此,样品分子在纳米材料表面发生催化反应所得到的发光信号可以提供分子的识别信息。根据这一现象,利用一组纳米催化材料设计了基于纳米材料表面化学发光的传感器阵列。
2.建立了快速筛选传感单元材料的新方法。设计了一组不同种类的负载贵金属的纳米氧化物催化材料,研究了纳米材料表面的化学发光性能与其催化活性之间的关系,发现纳米材料表面的化学发光性能与材料的催化活性之间存在着显著的相关性。这一方法不仅能够用于该传感器阵列所需要的传感材料的快速筛选,也能够用于催化材料的快速评价,对组合催化合成中高通量催化剂筛选有潜在的应用价值。
3.发展了用于传感机理研究的分析表征手段。研究了固体表面样品在介质阻挡放电低温等离子体中的解吸附/离子化现象,设计了新型常压质谱离子源,分别以阵列表面的氨基酸和爆炸物样品的分析为例,证明了该方法可用于阵列表面上痕量物质的实时、原位分析,为传感机理研究提供了必要的表征手段。这种离子源在其它化学反应过程的实时在线监测中具有潜在的用途。
Sensor array, which integrates the functions of multiple sensors, is one of the hot topics in the study of sensors. Sensor array has a wide variety of application areas including food and beverages, medical diagnostics, environmental monitoring, and a host of others. Abundant information can be provided by optical signals for the analyte identification, including luminescence intensity, wavelength, lifetime, etc. Thus, the rapid development for optical sensor arrays has been achieved recently. In the present dissertation, a sensor array of nanomaterial-based cataluminescence was developed. Based on this sensor array, a new way for rapid screening of sensor materials was reported. Furthermore, a new analysis technique was also designed for studying the sensing mechanism, which provides us a novel pathway for the research of sensor array. The main contents of the present dissertation are as follows:
1. A new sensor array based on nanomaterial-based cataluminescence was developed for analytes recognitions. By studying the cataluminescence behavior of sulfureted hydrogen, trimethylamine and ethanol on surfaces of nanomaterials, the specificity between cataluminescence signals and nanomaterials was established. The different cataluminescence responses were obtained both for the same analyte on different nanomaterials, and for the different analytes on the same nanomaterial. As a result, the optical information from the oxidation of analytes on the surfaces of nanomaterials can be used for analytes recognitions. Based on this phenomenon, an optical sensor array was developed with an array of different nanomaterials for analytes recognitions.
2. A new method for rapid screening of sensor materials was reported. A series of metal catalysts deposited on nanomaterials supports were prepared for studying the correlation between catalytic activities and cataluminescence responses for the CO oxidation. The well correlation between catalytic activities and cataluminescence intensities was established. Then, a cataluminescence-based imaging method was successfully used for the high-throughput screening of sensor materials.
3. A new analysis technique was designed for studying the sensing mechanism. An ambient ionization source for mass spectrometry was designed, which was based on desorption and ionization of analytes from the solid surfaces by the low temperature plasma of dielectric barrier discharge. The direct analysis of amino acids and explosives on the array surface was achieved, which demonstrated that the present method can be used for the real-time and in situ detection of trace analytes on the array surface. This provides us a novel pathway for studying the sensing mechanism.
引文
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