Ferrate(VI) oxidation of substituted nitrobenzene compounds: Kinetics, degradation, and oxidized products

Qi，Xiaochen1; Ding，Longzhen2; Jian，Chuanqi3; Liu，Rentao1; Liu，Na3; Qu，Dan4

2024-05-15

10.1016/j.cej.2024.150921

Chemical Engineering Journal   影响因子和分区

1385-8947

Nitrobenzene pollutants are discharged in large quantities into water bodies, posing a serious threat to the ecological environment. However, the effects of the nitrobenzene compounds with different structures on the Fe(VI) degradation process remain unclear. This research selects four different substituted nitrobenzene compounds (1,2-dinitrobenzene (1,2-DB), 4-nitrochlorobenzene (4-NCB), pentachloronitrobenzene (PCT), and 3,4-dinitrochlorobenzene (3,4-DTB)) and explores the oxidative degradation effect of ferrate(VI) based on experimental results and theoretical calculations. The reaction of Fe(VI) (800 μM) with each of the four nitrobenzene compounds (40 μM) reflected second-order reaction kinetics at pH 8: 4-NCB (127.08 Ms) > PCT (113.13 Ms) > 1,2-DB (100.1 Ms) > 3,4-DTB (96.459 Ms). Liquid chromatography time-of-flight mass spectrometry (LC-TOF-MS) analysis detected the main intermediates, which consisted of hydroxylation, ring-opening, coupling, and amine-based products. Free radicals in the reaction system were identified and analyzed, and hydroxyl radicals and carbon dioxide radicals were found. In addition, density functional theory (DFT) was used to explore the degradation mechanisms in the reaction between each of the four substances and hydroxyl radicals, with the active sites of the nitrobenzenes during the Fe(VI) degradation process determined through the calculation of molecular descriptors. Toxicity analysis with ECOSAR software indicated Fe(VI) reduced the toxicity of the nitrobenzenes. This study provides experimental and theoretical support for the reaction mechanism between nitrobenzenes and Fe(VI), as well as further understanding of the degradation mechanism of nitrobenzene compounds.

DFT method Ferrate(VI) Nitrobenzene pollutants Oxidation products

SCI ; EI

英语

其他

ENGINEERING

2-s2.0-85189675256

Scopus

1.College of Environment and Climate,Jinan University,Guangzhou,Guangdong,511443,China
2.School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
3.Department of Ecology,College of Life Science and Technology,Jinan University,Guangzhou,Guangdong,510632,China
4.Baohang Environment Co. Ltd.,Beijing,Beijing,100070,China

Qi，Xiaochen,Ding，Longzhen,Jian，Chuanqi,et al. Ferrate(VI) oxidation of substituted nitrobenzene compounds: Kinetics, degradation, and oxidized products[J]. Chemical Engineering Journal,2024,488.

Qi，Xiaochen,Ding，Longzhen,Jian，Chuanqi,Liu，Rentao,Liu，Na,&Qu，Dan.(2024).Ferrate(VI) oxidation of substituted nitrobenzene compounds: Kinetics, degradation, and oxidized products.Chemical Engineering Journal,488.

Qi，Xiaochen,et al."Ferrate(VI) oxidation of substituted nitrobenzene compounds: Kinetics, degradation, and oxidized products".Chemical Engineering Journal 488(2024).