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Thermal catalytic degradation of alpha-HBCD, beta-HBCD and gamma-HBCD over Fe3O4 micro/nanomaterial: Kinetic behavior, product analysis and mechanism hypothesis
Wu, Mingge; Zhao, Yanhui; Li, Qianqian; Su, Guijin; Liu, Wenbin; Wang, Qingliang; Li, Chuanqi
2019-06-10
Source PublicationSCIENCE OF THE TOTAL ENVIRONMENT
ISSN0048-9697
Volume668Pages:1200-1212
AbstractThe new persistent organic pollutant (POP), 1,2,5,6.9,10-hexabromocyclododecane (HBCD), has been widely detected in various environmental media and proved to be biotoxic. However, the research on catalytic degradation of HBCD is in its infancy. Herein, we examined the degradation of alpha-HBCD, beta-HBCD and gamma-HBCD. over Fe3O4 micro/nanomaterial at 200 degrees C. The pseudo-first-order kinetic rate constants were in the range of 0.04-0.15 min(-1), with half-life values of 5-19 min. gamma-HBCD is slightly less stable than beta-HBCD, but both of them readily convert into alpha-HBCD, as consistent with the Gibbs free energies of isomers themselves. The four products containing pentabromocyclododecene, two isomers of tetrabromocyclododecene and 1,5,9-cyclododecatriene were detected by conventional GC-MS. Interestingly, a high-throughput non-target product detection were performed by ESI-FT-ICR-MS, where up to 59 types of intermediate products were determined. It is tentatively proposed that different types of bromine-removed products (C12H17Br5, C12H18Br4, C12H19Br5, C12H24 and C12H19Br5O) and cyclododecane ring-opened products (C12H19Br7, C12H20Br6O and C12H20Br6) form via elimination reaction, nucleophilic substitution, hydrodebromination and addition reaction. Besides, most of the products that were detected contained oxygen. The average carbon oxidation state ((OSc) over bar) of the products indicate that the oxidation reaction is the dominant reaction type. Deep oxidation products, such as small molecular organic acids (formic, acetic, propionic, and butyric acids) and gas-phase oxidation products (CO2 and CO) were further detected by ion chromatography and GC-FID, respectively. This study might provide an alternative technique for the low-cost treatment of HBCD waste. (C) 2019 Elsevier B.V. All rights reserved.
Department环境纳米技术与健康效应重点实验室
KeywordHexabromocyclododecane Fe3O4 micro/nanomaterial Thermal catalytic degradation ESI-FT-ICR-MS Average carbon oxidation state ((OSc)over-bar)
Document Type期刊论文
Identifierhttp://ir.rcees.ac.cn/handle/311016/43215
Collection环境纳米技术与健康效应重点实验室
Affiliation1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Key Lab Environm Nanotechnol & Hlth Effects, POB 2871, Beijing 100085, Peoples R China
2.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Chem & Ecotoxicol, POB 2871, Beijing 100085, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
Recommended Citation
GB/T 7714
Wu, Mingge,Zhao, Yanhui,Li, Qianqian,et al. Thermal catalytic degradation of alpha-HBCD, beta-HBCD and gamma-HBCD over Fe3O4 micro/nanomaterial: Kinetic behavior, product analysis and mechanism hypothesis[J]. SCIENCE OF THE TOTAL ENVIRONMENT,2019,668:1200-1212.
APA Wu, Mingge.,Zhao, Yanhui.,Li, Qianqian.,Su, Guijin.,Liu, Wenbin.,...&Li, Chuanqi.(2019).Thermal catalytic degradation of alpha-HBCD, beta-HBCD and gamma-HBCD over Fe3O4 micro/nanomaterial: Kinetic behavior, product analysis and mechanism hypothesis.SCIENCE OF THE TOTAL ENVIRONMENT,668,1200-1212.
MLA Wu, Mingge,et al."Thermal catalytic degradation of alpha-HBCD, beta-HBCD and gamma-HBCD over Fe3O4 micro/nanomaterial: Kinetic behavior, product analysis and mechanism hypothesis".SCIENCE OF THE TOTAL ENVIRONMENT 668(2019):1200-1212.
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