Magnetic-room temperature phosphorescent multifunctional nanocomposites as chemosensor for detection and photo-driven enzyme mimetics for degradation of 2,4,6-trinitrotoluene

Magnetic-room temperature phosphorescent multifunctional nanocomposites as chemosensor for detection and photo-driven enzyme mimetics for degradation of 2,4,6-trinitrotoluene
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磁性室温磷光多功能纳米复合材料作为化学传感器用于检测和光驱动酶模拟物用于降解 2,4,6-三硝基甲苯

DOI:
10.1039/c2jm15139a
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发表时间:
2012-02
影响因子:
--
通讯作者:
Lian, Hong-Zhen
Lian, Hong-Zhen
中科院分区:
--
文献类型:
--
作者:
Zou, Wen-Sheng;Yang, Jing;Yang, Ting-Ting;Hu, Xin;Lian, Hong-Zhen

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近几十年来,与研究2,4,6-三硝基甲苯(TNT)相关的大量工作主要集中在开发超选择性和超灵敏的实时分析检测方法或开发高效、绿色的污染水处理技术。本论文将Fe3O4纳米颗粒的磁响应特性与量子点的化学传感特性相结合,制备了Fe3O4磁性纳米颗粒和掺锰硫化锌量子点纳米复合材料(MNPs/QDNCS),并将其用于水中超痕量TNT的室温磷光(RTP)传感和磁分离。值得注意的是,首次发现磁性RTP MNPs/QD NCS作为光驱动酶模拟物通过Haber-Weiss循环反应降解TNT。同时,通过猝灭4T1-6A1跃迁发射,MNPs/QD纳米管对TNT具有很高的选择性响应,检测下限可达12.5 nm。通过现场监测电子顺磁共振(EPR)信号,羟基自由基(OH·)的产生基本上归因于纳米Fe3O4表面金属离子的催化反应,而不是MNPs释放到溶液中的反应。所提出的方法不仅适用于超痕量TNT的检测和区分不同的硝基化合物,而且可以作为开发高效降解有机污染物污染水的最有前途的方法之一,以产生易于重复使用或排放到环境中的处理水,而不会产生任何有害影响。
In recent decades, considerable efforts related to the study of 2,4,6-trinitrotoluene (TNT) have been focused on either developing ultraselective and ultrasensitive methods for real-time analytical detection or exploiting highly efficient and green technologies for treatment of contaminated waters. In the present work, combining the magnetic response property of Fe3O4 nanoparticles with the chemosensory property of quantum dots (QDs), Fe3O4 magnetic nanoparticles and Mn-doped ZnS QD nanocomposites (MNPs/QD NCs) have been synthesized and used for room-temperature phosphorescence (RTP) sensing and magnetic separation of captured ultratrace TNT in water. Notably, magnetic-RTP MNPs/QD NCs were found as photo-driven enzyme mimetics for degradation of TNT through Haber–Weiss cycle reactions for the first time. Meanwhile, MNPs/QD NCs exhibited a highly selective response for TNT with detection limit down to 12.5 nM through the quenching of 4T1–6A1 transition emission. By in situ monitoring electron paramagnetic resonance (EPR) signals, production of hydroxyl radical (OH˙) is attributed fundamentally to the catalytic reactions occurring at metal ions on the surface of Fe3O4 nanoparticles rather than those released from the MNPs into a solution. The proposed methods, as well as being suitable for detecting ultratrace TNT and distinguishing different nitro-compounds, could be used as one of the most promising approaches for developing highly efficient degradation of organics contaminated waters to generate treated waters which could be easily reused or released into the environment without any harmful effects.
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