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Research on the reaction path of chlorobenzene oxidation by electrochemical-sodium persulfate system

Journal 2023 · IF 11.1 · 发表于 2023 年 8 月 3 日
作者: Shicheng Yuan,Hui Hu,Hao Huang,Zhongming Chen,Jiaxin Chen,Mi Zhang,Kunpeng Li,Ting Zhou,Ruibin Lv
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摘要

Chlorobenzene (CB) is an important organic chemical material that is volatile and difficult to degrade, and has received much attention because of its strong ozone generation potential. An electrochemical-sodium peroxydisulfate (PDS) system was constructed and the oxidation reaction path of chlorobenzene in this system was analyzed. The effects of current density, PDS concentration, initial pH, CB blow-off gas ratio and temperature on the oxidation and mineralization rate of chlorobenzene in the system were investigated respectively. At a current density of 168 A/m 2 , a PDS concentration of 0.5 mol/L, an initial pH of 10, a CB blow-off gas ratio of 20% and a reaction temperature of 60 °C, the CB conversion and mineralization rates were able to reach more than 90%. The results of electron paramagnetic resonance (EPR) experiments using 5,5-dimethyl-1-pyrroline N-oxide (DMPO) and 2,2,6,6-tetramethyl-4-piperidone hydrochloride (TEMP) as spin trapping agents indicate the presence of ⦁OH, · S O 4 − and 1 O 2 in the system. The signal of · O 2 − was also captured after the quenching of ⦁OH, which further indicates the presence of 1 O 2 . And the results of active substance quenching experiments showed that the active species that mainly contributed to the oxidation of chlorobenzene included ⦁OH, · S O 4 − and 1 O 2 , and their contributions to the oxidation of chlorobenzene were 25.0%, 31.7% and 22.2%, respectively. The Liquid Chromatograph Mass Spectrometer (LC-MS) characterization results showed that the formation of chlorophenol and hydroquinone and their ring-opening reactions were the most critical processes in the oxidative decomposition of chlorobenzene, and the reaction pathways for the oxidation of chlorobenzene by ⦁OH, · S O 4 − and 1 O 2 were proposed by these characterization results.

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