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Fenton process for degradation of selected chlorinated aliphatic hydrocarbons exemplified by trichloroethylene

QIANG Zhimin, BEN Weiwei, HUANG Chin-Pao

《环境科学与工程前沿（英文）》 2008年第2卷第4期页码 397-409 doi: 10.1007/s11783-008-0074-0

摘要： The degradation of selected chlorinated aliphatic hydrocarbons (CAHs) exemplified by trichloroethylene (TCE), 1,1-dichloroethylene (DCE), and chloroform (CF) was investigated with Fenton oxidation process. The results indicate that the degradation rate was primarily affected by the chemical structures of organic contaminants. Hydroxyl radicals (OH) preferred to attack the organic contaminants with an electron-rich structure such as chlorinated alkenes (i.e., TCE and DCE). The dosing mode of Fenton’s reagent, particularly of Fe, significantly affected the degradation efficiency of studied organic compound. A new “time-squared” kinetic model, = exp(-), was developed to express the degradation kinetics of selected CAHs. This model was applicable to TCE and DCE, but inapplicable to CF due to their varied reaction rate constants towards OH. Chloride release was monitored to examine the degree of dechlorination during the oxidation of selected CAHs. TCE was more easily dechlorinated than DCE and CF. Dichloroacetic acid (DCAA) was identified as the major reaction intermediate in the oxidation of TCE, which could be completely removed as the reaction proceeded. No reaction intermediates or byproducts were identified in the oxidation of DCE and CF. Based on the identified intermediate, the reaction mechanism of TCE with Fenton’s reagent was proposed.

关键词： identified 1 1-dichloroethylene kinetic Dichloroacetic Chloride

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Hexachlorobutadiene emissions from typical chemical plants

Minxiang Wang, Lili Yang, Xiaoyun Liu, Zheng Wang, Guorui Liu, Minghui Zheng

《环境科学与工程前沿（英文）》 2021年第15卷第4期 doi: 10.1007/s11783-020-1352-8

摘要： Abstract • Unintentional HCBD production in typical chemical plants was investigated. • The highest HCBD concentrations were found in the bottom residue. • Tri/tetrachloroethylene production processes were important HCBD sources. Hexachlorobutadiene (HCBD) was classed as a persistent organic pollutant under the Stockholm Convention in 2015. HCBD is mainly an unintentionally produced by-product of chlorinated hydrocarbon (e.g., trichloroethylene and tetrachloroethylene) synthesis. Few studies of HCBD formation during chemical production processes have been performed, so HCBD emissions from these potentially important sources are not understood. In this study, HCBD concentrations in raw materials, intermediate products, products, and bottom residues from chemical plants producing chlorobenzene, trichloroethylene, and tetrachloroethylene were determined. The results indicated that HCBD is unintentionally produced at much higher concentrations in trichloroethylene and tetrachloroethylene plants than chlorobenzene plants. The sum of the HCBD concentrations in the samples from all of the trichloroethylene and tetrachloroethylene production stages in plant PC was 247000 mg/mL, about three orders of magnitude higher than the concentrations in the tetrachloroethylene production samples (plant PB) and about six orders of magnitude higher than the concentrations in the chlorobenzene production samples (plant PA). The HCBD concentrations were highest in bottom residues from all of the plants. The concentrations in the bottom residue samples contributed 24%–99% of the total HCBD formed in the chemical production plants. The bottom residue, being hazardous waste, could be disposed of by incineration. The HCBD concentrations were much higher in intermediate products than raw materials, indicating that HCBD formed during production of the intended chemicals. The results indicate the concentrations of HCBD unintentionally produced in typical chemical plants and will be useful in developing protocols for controlling HCBD emissions to meet the Stockholm Convention requirements.

关键词： Hexachlorobutadiene Chemical plant Chlorobenzene Trichloroethylene Tetrachloroethylene