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在太阳辐射下,氧化锌纳米粒子对典型新烟碱类杀虫剂:吡虫啉的光催化降解。

Photocatalytic degradation of a typical neonicotinoid insecticide: nitenpyrum by ZnO nanoparticles under solar irradiation.

机构信息

Department of Chemistry for Materials, Graduate School of Engineering, Mie University, Tsu, Mie, 514-8507, Japan.

Global Environment Center for Education & Research, Mie University, Tsu, Mie, 514-8507, Japan.

出版信息

Environ Sci Pollut Res Int. 2020 Jun;27(16):20446-20456. doi: 10.1007/s11356-020-08424-w. Epub 2020 Apr 3.

Abstract

The photodegradation and mineralization of the nitenpyrum [(E)-N-(6-chloro-3-pyridylmethyl)-N-ethyl-N'-methyl-2-nitrovinylidenediamine], which is one of the most popular neonicotinoid insecticides, were conducted in the presence of ZnO photocatalyst under solar irradiation. An initial nitenpyrum concentration of 10 ppm was completely degraded in the presence of ZnO after 30 min irradiation, while only 70% degradation was observed in the absence of ZnO. The effect of different parameters, for example, amount of ZnO, initial pH, light intensity, reaction temperature, and irradiation time, on the photocatalytic degradation of nitenpyrum was also evaluated. The drop of total organic carbon (TOC) as a consequence of mineralization of nitenpyrum was observed during the photocatalytic process. The kinetics of photocatalytic degradation followed a pseudo-first order law according to Langmuir-Hinshelwood model, and the rate constant is 0.140 min. CO, chloride, and nitrate ions were observed as the end-products after completing degradation of nitenpyrum. The four kinds of intermediate products were identified by GC-MS during the decomposition of nitenpyrum. In order to investigate the degradation pathway of nitenpyrum, the point charge and frontier electron density at each atom on the molecule were determined using molecular orbital (MO) stimulation. The degradation mechanism was proposed, based on the identified intermediates. The solar photocatalytic degradation method can become an effective technique for the treatment of nitenpyrum-polluted water.

摘要

在阳光下,使用 ZnO 光催化剂对一种最受欢迎的新烟碱类杀虫剂——吡虫清 [(E)-N-(6-氯-3-吡啶基甲基)-N-乙基-N'-甲基-2-硝基亚乙烯二胺] 进行光降解和矿化。在存在 ZnO 的情况下,初始吡虫清浓度为 10ppm,经 30 分钟照射后完全降解,而在不存在 ZnO 的情况下,降解率仅为 70%。还评估了不同参数(例如 ZnO 的用量、初始 pH 值、光强度、反应温度和照射时间)对吡虫清光催化降解的影响。在光催化过程中,观察到总有机碳 (TOC) 因吡虫清矿化而下降。光催化降解动力学遵循 Langmuir-Hinshelwood 模型的拟一级定律,速率常数为 0.140min。在完成吡虫清的降解后,观察到 CO、氯化物和硝酸盐离子作为最终产物。在吡虫清的分解过程中,通过 GC-MS 鉴定了 4 种中间产物。为了研究吡虫清的降解途径,使用分子轨道 (MO) 模拟确定了分子上每个原子的点电荷和前沿电子密度。基于鉴定的中间体,提出了降解机制。太阳能光催化降解方法可以成为处理吡虫清污染水的有效技术。

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