Fluorescence Ratiometric Sensor for Trace Vapor Detection of Hydrogen Peroxide

Fluorescence Ratiometric Sensor for Trace Vapor Detection of Hydrogen Peroxide
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用于过氧化氢痕量蒸汽检测的荧光比率传感器

DOI:
10.1021/am501502v
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发表时间:
2014-06-11
影响因子:
9.5
通讯作者:
Zang, Ling
Zang, Ling
中科院分区:
材料科学2区
文献类型:
--
作者:
Xu, Miao;Han, Ji-Min;Zang, Ling

文献摘要

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过氧化氢(H2 O2)的痕量蒸气检测代表了对基于过氧化物的爆炸物进行无损检测的实用方法,所述基于过氧化物的爆炸物包括H2 O2和燃料的液体混合物以及高能过氧化物衍生物,例如三过氧化三丙酮(TATP)、二过氧化二丙酮(DADP)和三过氧化二胺(HMTD)。开发一个简单的化学传感器系统,响应H2 O2蒸汽具有高可靠性和足够的灵敏度(反应性)仍然是一个挑战。我们报告了一种荧光比率传感器分子,二乙基2,5-双(4-(4,4,5,5-四甲基-1,3,2-二氧杂硼杂环戊烷-2-基)苄基)氧基)羰基)氨基)对苯二甲酸酯(DAT-B),H2 O2,可以制成一个方便,可靠,灵敏的传感器系统,适用于痕量H2 O2的蒸汽检测。DAT-B在蓝色区域发荧光,在固态下在500 nm处有最大发射。在与H2 O2反应时,DAT-B被转化为电子“推挽”结构,2,5-二氨基对苯二甲酸二乙酯(DAT-N),其在以574 nm为中心的较长波长处具有发射峰。这种H2 O2介导的芳基硼酸酯的氧化可以通过加入有机碱如氢氧化四丁基铵(TBAH)来加速,导致在1 ppm的H2 O2蒸气下的响应时间小于0.5s。DAT-N的吸收带和DAT-B的发射带之间的强重叠使得能够实现有效的福斯特共振能量转移(FRET),从而允许进一步增强H2 O2蒸气的感测效率。滴铸DAT-B/TBAH膜的检测极限预计为7.7 ppb。通过将高灵敏度和选择性相结合,所报道的传感器系统可以通过将其制造成易于使用、具有成本效益的套件而在过氧化物基爆炸物和相关化学试剂的蒸气检测中找到广泛的应用。
Trace vapor detection of hydrogen peroxide (H2O2) represents a practical approach to nondestructive detection of peroxide-based explosives, including liquid mixtures of H2O2 and fuels and energetic peroxide derivatives, such as triacetone triperoxide (TATP), diacetone diperoxide (DADP), and hexamethylene triperoxide diamine (HMTD). Development of a simple chemical sensor system that responds to H2O2 vapor with high reliability and sufficient sensitivity (reactivity) remains a challenge. We report a fluorescence ratiometric sensor molecule, diethyl 2,5-bis((((4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl)oxy)carbonyl)amino)terephthalate (DAT-B), for H2O2 that can be fabricated into an expedient, reliable, and sensitive sensor system suitable for trace vapor detection of H2O2. DAT-B is fluorescent in the blue region, with an emission maximum at 500 nm in the solid state. Upon reaction with H2O2, DAT-B is converted to an electronic "push-pull" structure, diethyl 2,5-diaminoterephthalate (DAT-N), which has an emission peak at a longer wavelength centered at 574 nm. Such H2O2-mediated oxidation of aryl boronates can be accelerated through the addition of an organic base such as tetrabutylammonium hydroxide (TBAH), resulting in a response time of less than 0.5 s under 1 ppm of H2O2 vapor. The strong overlap between the absorption band of DAT-N and the emission band of DAT-B enables efficient Forster resonance energy transfer (FRET), thus allowing further enhancement of the sensing efficiency of H2O2 vapor. The detection limit of a drop-cast DAT-B/TBAH film was projected to be 7.7 ppb. By combining high sensitivity and selectivity, the reported sensor system may find broad application in vapor detection of peroxide-based explosives and relevant chemical reagents through its fabrication into easy-to-use, cost-effective kits.