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在 Ag NPs@HKUST-1 复合材料中,银纳米颗粒显著促进了硫芥的水解降解。

Significant enhancement in hydrolytic degradation of sulfur mustard promoted by silver nanoparticles in the Ag NPs@HKUST-1 composites.

机构信息

State Key Laboratory of Chemical Resource Engineering, Institute of Science, Beijing University of Chemical Technology, Beijing 100029, China.

State Key Laboratory of Chemical Resource Engineering, Institute of Science, Beijing University of Chemical Technology, Beijing 100029, China.

出版信息

J Hazard Mater. 2018 Sep 15;358:113-121. doi: 10.1016/j.jhazmat.2018.06.043. Epub 2018 Jun 21.

Abstract

The Ag NPs@HKUST-1 composites have been successfully prepared with different loading amounts of silver nanoparticles in HKUST-1 featuring a three-dimensional system of channels constructed by benzene-1,3,5-tricarboxylate and dimeric cupric units by a simple one-pot hydrothermal method, and characterized by various microscopy and spectroscopy analysis techniques. The average particle size of Ag NPs increased with the increase of the loading amount of Ag NPs. The experimental results showed that the degradation of sulfur mustard (HD) under ambient conditions followed pseudo-first order reaction kinetics. Additionally, the optimized Ag NPs@HKUST-1 (wherein Ag is l6.67 wt%) exhibited the highest degradation efficacy with an equilibrium rate constant and half-life for HD of 0.0450 min and 15.34 min, respectively. These values were significantly higher than those for pure HKUST-1 with an equilibrium rate constant and half-life for HD of 0.0168 min and 41.29 min, under the same experimental conditions. Gas chromatography-mass spectrometry (GC-MS) analysis on the product of 2-chloroethylethyl sulfide (2-CEES) degraded by Ag NPs@HKUST-1 showed that 2-hydroxyethyl ethyl sulfide (2-HEES) is the sole product, indicating that the remarkable enhancement of the degradation of HD must be due to the Ag NPs, which can promote hydrolysis of the chemical war agent in the composite.

摘要

Ag NPs@HKUST-1 复合材料已成功制备,在具有由苯-1,3,5-三羧酸和二价铜单元构建的三维通道系统的 HKUST-1 中,采用简单的一锅水热法,以不同的银纳米粒子负载量为特征,并通过各种显微镜和光谱分析技术进行了表征。Ag NPs 的平均粒径随 Ag NPs 负载量的增加而增加。实验结果表明,在环境条件下硫芥(HD)的降解遵循拟一级反应动力学。此外,优化的 Ag NPs@HKUST-1(其中 Ag 为 16.67wt%)表现出最高的降解效率,其 HD 的平衡速率常数和半衰期分别为 0.0450min 和 15.34min。在相同的实验条件下,这些值明显高于纯 HKUST-1 的平衡速率常数和半衰期,分别为 0.0168min 和 41.29min。通过气相色谱-质谱(GC-MS)对 Ag NPs@HKUST-1 降解的 2-氯乙基乙基硫醚(2-CEES)产物进行分析表明,2-羟乙基乙基硫醚(2-HEES)是唯一产物,表明 HD 降解的显著增强必须归因于 Ag NPs,Ag NPs 可以促进化学战剂在复合材料中的水解。

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