Activation of persulfate-based advanced oxidation processes by 1T-MoS2 for the degradation of imidacloprid: Performance and mechanism

过硫酸盐 降级(电信) 催化作用 化学 猝灭(荧光) 脱氢 水溶液 光化学 化学工程 荧光 有机化学 计算机科学 量子力学 电信 物理 工程类
作者
Xinzhi Wang,Zhenguo Chen,Yutian He,Xiaohui Yi,Chao Zhang,Qiao Zhou,Xuezhu Xiang,Yunan Gao,Mingzhi Huang
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:451: 138575-138575 被引量:56
标识
DOI:10.1016/j.cej.2022.138575
摘要

Imidacloprid (IMI) which has been widely detected in the natural water environment is potentially genotoxic to humans and should be effectively eliminated. Persulfate-based advanced oxidation processes are considered to be reliable means aiming at organic pollutants degradation, while an efficient catalyst is urgently needed for the activation of the reaction. As a two-dimensional material, 1T-MoS2 is expected to be applied for the activation of persulfates due to its abundant active sites and good electrical conductivity. Therefore, in this study, 1T-MoS2 was synthesized by a simple and safe two-step solvothermal reaction and proposed as an emerging activator of peroxymonosulfate (PMS) for the degradation of IMI. It was found that 1T-MoS2 has significantly better catalytic performance on PMS than 2H-MoS2 and Bulk-MoS2, reaching. 76.4 % at pH = 3. The degradation rate of IMI reduced under alkaline conditions due to the inhibition of catalytic processes. Among the different coexisting anions, HCO3- had the greatest degree of interference and inhibition to the degradation process, resulting in the lowest IMI degradation rate for only 42.45 %. Quenching experiments and EPR analysis showed that SO4-∙ and OH were the main reactive oxygen species in the 1T-MoS2/PMS process. In addition, the IMI degradation pathways analyzed by UPLC-Q-TOF-MS/MS included dehydrogenation, electrophilic addition, heterocyclic ring breakage and intramolecular rearrangement. This study promotes the application of 1T-MoS2 and is expected to provide a novel persulfate-based advanced oxidation process catalyzed by 1T-MoS2 for IMI elimination in the aqueous environment.
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