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丹磺酰基标记的纤维素作为双功能吸附剂,通过聚集诱导发光消除和检测水溶液中的汞。

Dansyl-labelled cellulose as dual-functional adsorbents for elimination and detection of mercury in aqueous solution via aggregation-induced emission.

作者信息

Li Ming, Zhang Siqi, Zhang Panpan, Qin Kexin, Chen Qian, Cao Qianyong, Zhang Yuling, Zhang Jinghong, Yuan Chungang, Xiao Huining

机构信息

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding, 071003, PR China; MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China.

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding, 071003, PR China; MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China.

出版信息

J Environ Manage. 2023 Jul 15;338:117773. doi: 10.1016/j.jenvman.2023.117773. Epub 2023 Mar 28.

Abstract

Dansyl chloride fluorophore exhibits typical aggregation induced fluorescence emission behavior in acetone/water solution. To realize the integration of detective and adsorptive functions, dansyl chloride is covalently immobilized on cellulose substrate to fabricate an efficient adsorbent for mercury ions in water. The as-prepared material exhibits excellent fluorescence sensing performance exclusively for Hg (II) with the presence of other metal ions. A sensitive and selective fluorescence quenching across the concentration range of 0.1-8.0 mg/L is observed with a detection limit of 8.33 × 10 M as a result of the inhibition of aggregation induced emission caused by the coordination between adsorbent and Hg (II). Besides, the adsorption properties for Hg (II) including the influence of initial concentration and contact time are investigated. Langmuir model and pseudo-second-order kinetics are demonstrated to fit well with the adsorption experiment for the uptake of Hg (II) by the functionalized adsorbent, also, intraparticle diffusion kinetic model is proved to aptly describe the Hg (II) removal in aqueous solution. In addition, the recognition mechanism is considered to originate from the Hg (II) triggered structural reversals of naphthalene ring units which are verified by the X-ray photoelectron spectroscopy and density functional theory calculation. Moreover, the synthesis method used in this work also provides a strategy for the sensing application of organic sensor molecules with AIE properties in which the aggregated behavior could be appropriately realized.

摘要

丹磺酰氯荧光团在丙酮/水溶液中表现出典型的聚集诱导荧光发射行为。为了实现检测和吸附功能的一体化,将丹磺酰氯共价固定在纤维素基质上,制备出一种高效的水中汞离子吸附剂。所制备的材料在存在其他金属离子的情况下,对Hg(II)表现出优异的荧光传感性能。由于吸附剂与Hg(II)之间的配位作用抑制了聚集诱导发射,在0.1 - 8.0 mg/L的浓度范围内观察到灵敏且选择性的荧光猝灭,检测限为8.33×10⁻⁸ M。此外,研究了Hg(II)的吸附性能,包括初始浓度和接触时间的影响。结果表明,Langmuir模型和伪二级动力学能很好地拟合功能化吸附剂对Hg(II)的吸附实验,同时,颗粒内扩散动力学模型也能恰当地描述水溶液中Hg(II)的去除情况。此外,识别机制被认为源于Hg(II)引发的萘环单元结构反转,这通过X射线光电子能谱和密度泛函理论计算得到了验证。而且,本工作中使用的合成方法也为具有聚集诱导发光性质的有机传感分子的传感应用提供了一种策略,其中聚集行为可以得到适当实现。

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