基于催化活性的双功能纳米材料光化学传感器研究
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摘要
光化学传感器由于响应速度快且具有高通量、可视化检测的特点，在公共安全、人类健康及环境监测等领域具有广泛的应用前景。利用纳米材料的催化活性来放大检测信号从而提高光化学传感器的灵敏度，是一个重要的研究方向。本论文设计了三种基于催化活性的双功能纳米材料光化学传感器，为提高光化学传感器的灵敏度提供了新思路。主要研究内容如下：
1.提出了利用具有荧光性质和催化活性的金纳米团簇设计荧光传感器的方法。利用具有生物功能的辣根过氧化物酶制备了金纳米团簇（HRP-AuNCs），无需后续的功能化修饰得到了同时具有荧光性质和酶催化活性的双功能纳米材料，用于构建光化学传感器。HRP-AuNCs表面的HRP可以催化H_2O_2的氧化还原反应，导致金纳米团簇的荧光淬灭，从而可以实现H_2O_2的检测。该方法对H_2O_2的检测限达30nM，与不具有酶催化活性的BSA-AuNCs相比灵敏度提高了10倍。
2.利用具有催化活性和识别性能的模拟酶纳米材料构建了高灵敏、高通量、可视化的蛋白质传感器阵列。制备了两种具有模拟酶活性的功能化Fe_3O_4NPs，其催化活性用于信号放大，其表面的功能化配体用于生物识别。生物分子与配体的相互作用可以调节其对显色底物的催化活性，从而提供响应信号的变化。由这两种双功能纳米材料组成的传感器阵列可有效区分11种蛋白质。响应灵敏度可低至50nM，对于部分蛋白质，最低可达1nM。与常规的显色阵列传感器相比，灵敏度提高了1000倍；与基于酶放大的阵列传感器的灵敏度相当，但纳米材料模拟酶比生物酶具有更好的稳定性且成本更低。
3.利用纳米材料的催化活性和吸附性能，设计了可实现室温富集-原位检测的高灵敏催化发光传感器。选取了同时具有吸附性和催化活性的纳米二氧化锆作为传感材料，其吸附性用于乙醇的预富集，其催化活性用于输出原位发光信号。与传统的催化发光传感器相比，其灵敏度提高了3000倍。该传感器具有寿命长、灵敏度高、能耗低、无需发光试剂的优点，成功用于酒后呼吸气中乙醇的检测。在此基础上，还发展了由不同纳米材料组成的室温富集-原位催化发光检测的传感器阵列，并将其用于信息素的识别。
Optical chemical sensors has a wide range of applications in areas such as publicsafety, human health and environmental monitoring due to their fast response,multiplexing capabilities and potential in naked eye detection. The catalytic activity ofnanomaterials can trigger a detectable signal amplification to increase the sensitivity ofoptical chemical sensors. In the present dissertation, dual functional nanomaterials withcatalytic activity have been employed for the design and development of opticalchemical sensors. This strategy paves the way to the devolopment of minaturizedoptical chemical sensors with high sensitivity. The main contents of the presentdissertation are as follows:
1. A new fluorescent sensor has been developed by using a dual functionalnanomaterial with catalytic activity and fluorescence properties. Horseradish peroxidasefunctionalized fluorescent gold nanoclusters (HRP-AuNCs) was successfully preparedvia a biomineralization process. We found HRP remains active and possesses itsintrinsic catalytic activity, thus HRP-AuNCs have dual functions including thefluorescence and catalytic ability. The fluorescence of HRP-AuNCs can be quenchedquantitatively by adding H_2O_2. The sensitivity for H_2O_2detection of this method (LOD=30nM) has been improved by10times compared with that using BSA-AuNCswithout catalytic activity. Accordingly, using biologically functional proteins for thepreparation of fluorescent gold nanoclusters, without subsequent modification, canobtain nanomaterials with dual functions of the fluorescence properties and biologicalactivity, which can be directly used to build up optical biosensors.
2. A new colorimetric sensor array for proteins detection has been designed byemploying dual functional iron oxide nanoparticles featuring intrinsic enzyme mimeticactivity and recognition capability. Two functionalized Fe_3O_4NPs were prepared andused as signal amplifiers in the array-based sensor for colorimetric protein sensing.Interactions between positively charged Fe_3O_4NPs and different analyte proteinsmodulate the peroxidase-like activity of Fe_3O_4NPs in different fashions, affordingcatalytically amplified colorimetric signal patterns, enabling the detection andidentification of11proteins at a50nM concentration, for some proteins as low as1nM. The sensitivity was increased by1000times when compared with the conventionalnanoparticles based protein array sensor, and equal to that of protein array sensor basedon enzyme amplification. Nanomaterials based enzyme mimic has better thermal andchemical stability than biological enzyme, and are cost-effective.
3. An optical chemical sensor for ethanol has been proposed by using anaomaterial with dual functions of catalytic activity and adsorption capability as sensingmaterials. Analytes were trapped on sensing nanomaterials and detected in situ byrecording the cataluminescence (CTL) signals with fast elevated temperature. Comparedthe previous CTL sensor, its sensitivity is3,000times improved. The sensor wassuccessfully applied to monitor the ethanol concentration in human expired gas afterdrinking, and the results agreed well with the reference values. This miniature ethanolsensor offers higher sensitivity, faster response and lower power consumption, whichmake it very promising in developing hand-hold sensing device for feld detection.Furthermore, a variety of nanomaterials with dual functions of catalytic activity andadsorption capality have been used to develop a sensor array for pheromone sensing.
1.提出了利用具有荧光性质和催化活性的金纳米团簇设计荧光传感器的方法。利用具有生物功能的辣根过氧化物酶制备了金纳米团簇（HRP-AuNCs），无需后续的功能化修饰得到了同时具有荧光性质和酶催化活性的双功能纳米材料，用于构建光化学传感器。HRP-AuNCs表面的HRP可以催化H_2O_2的氧化还原反应，导致金纳米团簇的荧光淬灭，从而可以实现H_2O_2的检测。该方法对H_2O_2的检测限达30nM，与不具有酶催化活性的BSA-AuNCs相比灵敏度提高了10倍。
2.利用具有催化活性和识别性能的模拟酶纳米材料构建了高灵敏、高通量、可视化的蛋白质传感器阵列。制备了两种具有模拟酶活性的功能化Fe_3O_4NPs，其催化活性用于信号放大，其表面的功能化配体用于生物识别。生物分子与配体的相互作用可以调节其对显色底物的催化活性，从而提供响应信号的变化。由这两种双功能纳米材料组成的传感器阵列可有效区分11种蛋白质。响应灵敏度可低至50nM，对于部分蛋白质，最低可达1nM。与常规的显色阵列传感器相比，灵敏度提高了1000倍；与基于酶放大的阵列传感器的灵敏度相当，但纳米材料模拟酶比生物酶具有更好的稳定性且成本更低。
3.利用纳米材料的催化活性和吸附性能，设计了可实现室温富集-原位检测的高灵敏催化发光传感器。选取了同时具有吸附性和催化活性的纳米二氧化锆作为传感材料，其吸附性用于乙醇的预富集，其催化活性用于输出原位发光信号。与传统的催化发光传感器相比，其灵敏度提高了3000倍。该传感器具有寿命长、灵敏度高、能耗低、无需发光试剂的优点，成功用于酒后呼吸气中乙醇的检测。在此基础上，还发展了由不同纳米材料组成的室温富集-原位催化发光检测的传感器阵列，并将其用于信息素的识别。
Optical chemical sensors has a wide range of applications in areas such as publicsafety, human health and environmental monitoring due to their fast response,multiplexing capabilities and potential in naked eye detection. The catalytic activity ofnanomaterials can trigger a detectable signal amplification to increase the sensitivity ofoptical chemical sensors. In the present dissertation, dual functional nanomaterials withcatalytic activity have been employed for the design and development of opticalchemical sensors. This strategy paves the way to the devolopment of minaturizedoptical chemical sensors with high sensitivity. The main contents of the presentdissertation are as follows:
1. A new fluorescent sensor has been developed by using a dual functionalnanomaterial with catalytic activity and fluorescence properties. Horseradish peroxidasefunctionalized fluorescent gold nanoclusters (HRP-AuNCs) was successfully preparedvia a biomineralization process. We found HRP remains active and possesses itsintrinsic catalytic activity, thus HRP-AuNCs have dual functions including thefluorescence and catalytic ability. The fluorescence of HRP-AuNCs can be quenchedquantitatively by adding H_2O_2. The sensitivity for H_2O_2detection of this method (LOD=30nM) has been improved by10times compared with that using BSA-AuNCswithout catalytic activity. Accordingly, using biologically functional proteins for thepreparation of fluorescent gold nanoclusters, without subsequent modification, canobtain nanomaterials with dual functions of the fluorescence properties and biologicalactivity, which can be directly used to build up optical biosensors.
2. A new colorimetric sensor array for proteins detection has been designed byemploying dual functional iron oxide nanoparticles featuring intrinsic enzyme mimeticactivity and recognition capability. Two functionalized Fe_3O_4NPs were prepared andused as signal amplifiers in the array-based sensor for colorimetric protein sensing.Interactions between positively charged Fe_3O_4NPs and different analyte proteinsmodulate the peroxidase-like activity of Fe_3O_4NPs in different fashions, affordingcatalytically amplified colorimetric signal patterns, enabling the detection andidentification of11proteins at a50nM concentration, for some proteins as low as1nM. The sensitivity was increased by1000times when compared with the conventionalnanoparticles based protein array sensor, and equal to that of protein array sensor basedon enzyme amplification. Nanomaterials based enzyme mimic has better thermal andchemical stability than biological enzyme, and are cost-effective.
3. An optical chemical sensor for ethanol has been proposed by using anaomaterial with dual functions of catalytic activity and adsorption capability as sensingmaterials. Analytes were trapped on sensing nanomaterials and detected in situ byrecording the cataluminescence (CTL) signals with fast elevated temperature. Comparedthe previous CTL sensor, its sensitivity is3,000times improved. The sensor wassuccessfully applied to monitor the ethanol concentration in human expired gas afterdrinking, and the results agreed well with the reference values. This miniature ethanolsensor offers higher sensitivity, faster response and lower power consumption, whichmake it very promising in developing hand-hold sensing device for feld detection.Furthermore, a variety of nanomaterials with dual functions of catalytic activity andadsorption capality have been used to develop a sensor array for pheromone sensing.
引文
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