ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Fan Xu,Jie Chen,Wei Wang,Lizhong Zhu
Polybrominated diphenyl ethers (PBDEs) in soils posed potential risks to crop growth and food safety due to their prevalence and persistence. PBDEs were capable of being absorbed and accumulated into crops, impacting their growth, whereas the interference on metabolic components and nutritional composition deserves further elucidation. This study integrated a combined non-targeted and targeted metabolomics method to explore the influences of 2,2',4,4'-tetrabromodiphenyl ether (BDE-47), 2,2',4,4',5-pentabromodiphenyl ether (BDE-99) and decabromodiphenyl ether (BDE-209) on the metabolic responses of rice ( Oryza sativa ). Metabolic pathways, which were associated with sugars, organic acids, and amino acids, were significantly disturbed under PBDE stresses. Particularly, 75% of the marked altered pathways belonged to amino acid metabolism, with alanine / aspartate / glutamate metabolism being commonly enhanced. The degradation of aspartic acid promoted the formation of downstream amino acids, among which the levels of lysine, methionine, isoleucine, and asparagine were increased by 1.31–3.15 folds compared to the control. Thus, the antioxidant capacity in rice plants was enhanced, particularly through the significant promotion of ascorbic acid-glutathione (AsA-GSH) cycle in rice leaves. The amino acids were promoted to resist reactive oxygen species (ROS) efficiently, thus were deficient for nutrient storage. When exposed to 4 μmol/kg PBDEs, the contents of amino acids and proteins in grains decreased by 9.1–32.1% and 8.6–34.8%, respectively. In particular, glutelin level was decreased by 5.6–41.2%, resulting in a decline in nutritional quality. This study demonstrated that PBDEs deteriorated the protein nutrition in rice grains by affecting amino acid metabolism, providing a new perspective for evaluating the ecological risks of PBDEs and securing agricultural products.
研究领域:
环境科学
·
农业
·
植物科学
·
食品安全
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Ming Lei,Zhiying Wang,Lihua Zhu,Wenshan Nie,Heqing Tang
Deep debromination of polybrominated diphenyl ethers (PBDEs) by visible light photocatalysis is still a challenge in the field of halogenated pollutants control. Here, an efficient photocatalyst (Pd/g-C 3 N 4 ) was prepared by a simple impregnation-chemical reduction method with bulk g-C 3 N 4 and PdCl 2 as precursors. Under preferred reaction conditions (visible light irradiation for 120 min), the use of the 0.5% Pd/g-C 3 N 4 composites (0.4 g L −1 ) yielded an almost complete debromination of BDE47 (10 μmol L −1 ) in methanol-water mixture, while the debromination of BDE47 did not occur on pure g-C 3 N 4 . A “Pd-promoted active H atom species attack and C-Br bond cleavage” route was proposed according to the identified degradation intermediates. A catalytic mechanism was further clarified: Pd nanoparticles exerted affinity interaction with bromine atoms, and the storing of electrons on Pd would increase the binding interaction. In the debromination process, methanol acts as both a hole scavenger and a hydrogen donor to provide active H atom species through the reaction of H + and photogenerated electrons on Pd nanoparticles. The initiation of BDE47 debromination on Pd nanoparticles required an induction period to enrich a critical amount of electrons for stretching the C-Br bond and its subsequent being attacked by active H atoms. The generated 2,2′-dibromodiphenyl ether (BDE4) would be further reduced to bromine-free products by hydro-debromination process or coupling reaction.
研究领域:
环境科学
·
化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tao Pan,Yu Wang,Xin Yang,Xiong-fei Huang,Rong-liang Qiu
Fe(II)-catalyzed peroxymonosulfate (PMS) activation process was able to degrade persistent organic pollutants, such as polybrominated diphenyl ethers (PBDEs), but the slow transformation rate from the generated Fe(III) to Fe(II) restricted the efficiency of this process. In this study, we found that the addition of small quantities of gallic acid (GA), a model compound of natural polyphenols, in the Fe(III)/PMS process (namely GA/Fe(III)/PMS process) could exert a long-term influence on Fe(II) recycle and accelerated the degradation of 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) over 72 h. Under conditions of 20.3 µM GA, 13.6 µM Fe(III) and 400 µM PMS, the degradation efficiency of BDE47 reached 85%, which was 9.4 times higher than that in the Fe(III)/PMS process. The degradation kinetics can be divided into an initial “fast stage” (k obs1 = 0.298 h −1 ) and a second “slow stage” (k obs2 = 0.021 h −1 ). Aromatic radicals such as hydroxycyclohexadienyl radical (poly-HCD ) produced by the attack of SO 4 − /HO on GA was proposed to be responsible for Fe(II) recycle in the first stage, while ring-opened products following SO 4 − /HO attack of GA-quinone mainly initiated Fe(III) reduction in the second stage. Owing to the multiple Fe(III) reduction pathways, PMS would be continuously activated by Fe(II) to form SO 4 − and HO , which were the dominant reactive species for BDE47 degradation. Finally, natural polyphenols extracted from green tea were proven effective in enhancing BDE47 degradation in Fe(III)/PMS process. This study not only provides a new way to propagate Fe(II)-activated persulfate chain reactions for the degradation of refractory organic contaminants, like PBDEs, but also sheds new insight into the reactivity of organic byproducts toward Fe in PMS-based oxidation system.
研究领域:
环境科学
·
化学
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高影响因子
ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Bingbing Sun,Eddy Y. Zeng
Considerable efforts on exposure assessment of microplastics (MPs) as an agent in transport of toxic contaminants have been performed in organisms. However, chemical diffusion of inherent hydrophobic organic contaminants from MPs under simulated gut conditions is poorly examined. The present study examined the transfer kinetics of polybrominated diphenyl ethers (PBDEs) from polystyrene (PS), acrylonitrile butadiene styrene (ABS), and polypropylene (PP) MPs under gut surfactants (sodium taurocholate) at two relevant body temperatures of marine organisms, and evaluated the importance of MP ingestion in bioaccumulation of PBDEs in lugworm by a biodynamic model. Diffusion coefficients of PBDEs range from 5.82 × 10 −23 to 7.96 × 10 −20 m 2 s −1 in PS, 5.49 × 10 −23 to 3.45 × 10 −20 m 2 s −1 in ABS, and 5.58 × 10 −21 to 5.79 × 10 −17 m 2 s −1 in PP, with apparent activation energies in the range of 33–148 kJ mol −1 . The biota–plastic accumulation factors of PBDEs leached from these plastics range from 1.44 × 10 −8 to 7.15 × 10 −5 . Although ingestion of MPs with the common size (>0.5 mm) showed the negligible contribution to bioaccumulation of PBDEs in lugworm, their contribution in PBDEs transfer can be increased with gradual breakdown of MPs.
研究领域:
环境科学
·
生态毒理学
·
海洋生物学
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PubMed
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Bin Li,Jianghong Shi,Xueling Xiang,Mengtao Zhang,Hui Ge,Shuhan Sun
Bromophenols has been proven to synthesize hydroxylated polybrominated diphenyl ethers (OH-PBDEs), which may pose additional environmental and health risks in the process of bioremediation. In this study, the removal of 2,4-dibromophenol (2,4-DBP) and 2,4,6-tribromophenol (2,4,6-TBP) and the biosynthetic of OH-PBDEs by Prorocentrum donghaiense were explored. The removal efficiencies of 2,4-DBP and 2,4,6-TBP ranged from 32.71% to 76.89% and 31.15%–78.12%, respectively. Low concentrations of 2,4-DBP stimulated algal growth , while high concentrations were inhibitory. Furthermore, exposure to 10.00 mg L −1 2,4-DBP resulted in the detection of 2′-hydroxy-2,3′,4,5′-tetrabromodiphenyl ether (2′–OH–BDE-68) within P . donghaiense . In contrast, increasing concentrations of 2,4,6-TBP considerably inhibited P . donghaiense growth, with 4′-hydroxy-2,3′,4,5′,6-pentabromodiphenyl ether (4′–OH–BDE-121) detected within P. donghaiense under 5.00 mg L −1 2,4,6-TBP. Metabolomic analysis further revealed that the synthesized OH-PBDEs exhibited higher toxicity than their precursors and identified the oxidative coupling as a key biosynthetic mechanism. These findings confirm the capacity of P. donghaiense to remove bromophenols and biosynthesize OH-PBDEs from bromophenols, offering valuable insights into formulating algal bioremediation to mitigate bromophenol contamination.
研究领域:
环境科学
·
海洋生物学
·
毒理学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 11.3
Junhui He,Nan Wang,Lihua Zhu,Long Zhao
Polybrominated diphenyl ethers (PBDEs) are highly hydrophobic and environmentally persistent, leading to their accumulation in soils and posing serious risks to ecosystems and human health. This study developed an efficient remediation strategy through the synergistic integration of chemical leaching and electron beam (EB) irradiation for treating PBDEs-contaminated soils. EB irradiation alone could directly degrade PBDEs in soil, while a combination with methanol extraction enhanced the process. Methanol effectively extracted BDE47 from soil with an efficiency exceeding 99 % and BDE47 in methanol was degraded rapidly under EB irradiation, achieving complete debromination at a dose of 12 kGy. The leaching agent exhibited excellent reusability over five consecutive cycles, with both extraction and debromination efficiencies remaining consistently high. Moreover, this method demonstrated broad applicability by effectively degrading multiple PBDE congeners. Mechanism studies through ESR and deuterated solvent experiments revealed that electron transfer is the rate-determining step in PBDE degradation, and the debromination rate was independent of the number and position of bromine substituents. This capability represents a significant advantage of EB irradiation over conventional reductive degradation techniques, enabling complete debromination of various PBDEs. This work presents a green and sustainable technology for the remediation of PBDE-contaminated sites, offering significant environmental benefits and promising practical prospects.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2017
·Vol. 24
·期 28
·22450-22457
·
IF 2.741
Deng Chao,Li Ying,Li Jinhui,Chen Yuan,Li Huafen
Though mechanical recycling of WEEE plastics is supposed to be a promising method, PBDEs release and the resulting contamination during its processing remain unclear yet. The distribution of PBDEs pollution in production lines was investigated from two flame-retardant plastic modification plants in Southern China. This was followed by laboratory simulation experiments to characterize the emission processes. PBDEs concentrations ranged from 37 to 31,305 ng/L in cooling water and from 40,043 to 216,653 ng/g dry wt in solid samples taken during the field investigation. In the laboratory simulation, concentrations ranged from 146 to 433 ng/L in cooling water and from 411,436 to 747,516 ng/Nm 3 in flue gas. All samples were dominated by BDE-209 among the congeners. Temperatures and impurities in plastic substrate can significantly affect PBDEs release. Special attention should be paid to the risks of water directly discharge from the cooling system, especially for the biological sludge and sediments, as well as flue gas emissions to the environment.
研究领域:
环境科学
·
污染控制
·
材料回收
·
毒理学
·
化学工程
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Bairong Fu,Dongqin Tan,Jing Jin,Lei Tong,Longxing Wang,Yihou Peng,Ningbo Geng,Lidong Wu,Huilian Ma,Yuwen Ni,Jiping Chen
The fragmentation behavior of isomeric hydroxylated polybrominated diphenyl ethers (OH-PBDEs) remains poorly elucidated, although LC-MS/MS is essential for their analysis. This study systematically characterizes their fragmentation behavior by LC-ESI-MS2, elucidating relationships between product ions, structural features, and instrument detection limits. Results demonstrated congener-specific variability in the signal intensity of [M–H]−, particularly among isomers. Fragmentation behavior is highly dependent on the hydroxyl location on the diphenyl ether scaffold, as well as the bromine substituent pattern. Three distinct mechanisms are identified: (1) Br abstraction via free radical-mediated rearrangement cleavage in meta-hydroxylated PBDEs, (2) preferential formation of the [Br]− ion via γ-elimination in ortho-hydroxylated PBDEs, and (3) characteristic formation of bromobenzoquinone anions via multistep fragmentation mechanisms in para-hydroxylated PBDEs. Furthermore, the ortho-effect, particularly pronounced in 2′–OH substituted congeners, significantly alters the fragmentation pathways. While the elucidated fragmentation pathways provided structural insights, the inherent weak signals challenged detection. A sensitivity-enhancing precolumn derivatization protocol with dansulfonyl chloride was introduced to solve the problem. The MS2 fragmentation of these derivatives was conveniently dominated by the cleavage of the C–S bond within the dansyl group, yielding abundant diagnostic ions that greatly aided in structural confirmation. As predicted, the derivatization strategy achieved a remarkable up to 15-fold improvement in the sensitivity. This investigation advances the understanding of OH-PBDE fragmentation, establishes an identification framework using specific patterns and diagnostic ions, and demonstrates a practical derivatization approach for enhanced sensitivity, elucidating structure-fragmentation relationships in brominated aromatics and providing methodological guidance for future analysis.
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PubMed
高影响因子
Processes
·
2025
·Vol. 13
·期 6
·1806
·
IF 2.8
Chenyu Zhang,Xiaodong Du,Songhan Zeng,Jinghong Wen,Jielei Luo,Sile Wu,Qian Zhang,Xueqin Tao,Guining Lu
Soil washing is an efficient method to remove polybrominated diphenyl ethers (PBDEs) from contaminated soils. The obtained solutions from soil-washing still contain PBDEs, requiring further treatment before disposal or reuse. Although photolysis is effective for PBDE degradation in solutions, the concurrent formation of toxic polybrominated dibenzofurans (PBDFs) may limit its practical application. In this study, 2,8-dibromodibenzofurans (2,8-BDF) formation rate and mechanisms during 2,4,4′-tribromodiphenyl ether (BDE-28) photolysis in various simulated soil-washing solutions was investigated. Results revealed significant effects of solubilizers on 2,8-BDF formation. The nonionic surfactants polysorbate (TW80), polyoxyethylene octylphenyl ether (TX series), and the cationic surfactant cetyltrimethylammonium bromide (CTAB) resulted in low 2,8-BDF formation rate (1–5%), while the β-cyclodextrin led to the highest 2,8-BDF formation rate (about 28%). The nonionic surfactants polyoxyethylene dodecyl ethers (Brij series), and the anionic surfactants sodium dodecylbenzene sulfonate (SDBS) and sodium dodecyl sulfate (SDS), also showed a high level of 2,8-BDF formation rate (7–17%). Solubilizer structure and its interaction with BDE-28 determined the 2,8-BDF formation. The role of the micelle microenvironment on 2,8-BDF formation was verified via an experiment and molecular dynamics simulation. The organic region of micelle exhibited high hydrogen donation ability, which inhibited 2,8-BDF formation. The results indicated distinct risks of PBDE photolysis in various soil-washing solutions, providing an important reference for solubilizer selection and the application of photolysis on the treatment of soil-washing solutions containing PBDEs.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Rui Wang,Ting Tang,Guining Lu,Zhiqiang Zheng,Kaibo Huang,Huafeng Li,Xueqin Tao,Hua Yin,Zhenqing Shi,Zhang Lin,Fengchang Wu,Zhi Dang
This study investigated the relative significance of electron transfer (e-transfer) and H-atom transfer (H-transfer) in a nanoscale zerovalent iron (n-ZVI) system and six n-ZVI-based bimetallic systems (Fe/Cu, Fe/Ni, Fe/Pd, Fe/Ag, Fe/Pt, and Fe/Au) through a case study of the debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47). The results revealed that the reactivities of these bimetallic particles to BDE-47 decreased in the following order: Fe/Pd > Fe/Ag > Fe/Cu > Fe/Ni > Fe/Au > Fe/Pt ≈ n-ZVI. Debromination of BDE-47 in metal-H 2 systems suggested that Ni, Pd, Pt, Cu and Au can utilize H 2 to debrominate BDE-47. In the H-transfer process, BDE-47 preferentially debrominated the para‑ bromine substituent to generate BDE-17, whereas in the e-transfer process, BDE-47 preferentially debrominate ortho‑ bromine substituent to generate BDE-28. The debromination pathways of BDE-47 in bimetallic and NaBH 4 -metal systems suggested that Fe/Ni, Fe/Pd and Fe/Pt debrominate polybrominated diphenyl ethers (PBDEs) through a H-transfer dominant mechanism, while Fe/Ag debrominate PBDEs through an e-transfer dominant mechanism. In the cases of Fe/Cu and Fe/Au, the e-transfer and H-transfer may be equally involved in the debromination of PBDEs. These results greatly improve our understanding of the relative significance of e-transfer and H-transfer in the dehalogenation of halogenated aromatic compounds (HACs) in various n-ZVI-based bimetallic systems.
研究领域:
环境科学
·
化学
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产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Leilei Xiang,Hongjie Sheng,Min Xu,Marc Redmile-Gordon,Yongrong Bian,Xinglun Yang,Xin Jiang,Fang Wang
Application of crop residues is a conventional practice that contributes to crop production through nutrient returns and other benefits to soil health: driving soil physicochemical and biological functions. However, little is known about the impacts of straw residue incorporation on the bioavailability of organic pollutants and associated changes in microbial community structure in contaminated soils. In this study, maize straw was added to a soil contaminated with a model polybrominated diphenyl ether (BDE-47). A pot experiment was conducted and planted with carrot ( Daucus carota L.). We found that straw addition greatly reduced the bioavailability of BDE-47, changed the bacterial community structure and affected a range of soil physiochemical properties. Moreover, the amount of BDE-47 that had accumulated in carrot roots and aboveground tissues was significantly reduced. This study may therefore describe an effective agronomic strategy to reduce the bioavailability of polybrominated diphenyl ethers (PBDEs) in a soil used to grow high value vegetable crops. This strategy draws on traditional wisdom and shows promise as a practical method to support horticultural production systems, remediate soils, and help to ensure food safety.
研究领域:
农学
·
环境科学
·
土壤微生物学
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DOI
PubMed
高影响因子
Processes
·
2022
·Vol. 10
·期 9
·1815
·
IF 3.352
Yao Ma,Haoliang Li,Chunsheng Xie,Xiaodong Du,Xueqin Tao,Guining Lu
Soil-washing is a potential technology for the disposal of soil contaminated by e-waste; however, the produced soil-washing effluent will contain polybrominated diphenyl ethers (PBDEs) and a large number of surfactants, which are harmful to the environment, so the treatment of PBDEs and the recycling of surfactants are the key to the application of soil-washing technology. In this study, coconut shell granular-activated carbon (GAC) was applied to remove PBDEs from Triton X-100 (TX-100) surfactant which simulates soil-washing effluent. The adsorption results show that, GAC can simultaneously achieve effective removal of 4,4′-dibromodiphenyl ether (BDE-15) and efficient recovery of TX-100. Under optimal conditions, the maximum adsorption capacity of BDE-15 could reach 623.19 μmol/g, and the recovery rate of TX-100 was always higher than 83%. The adsorption process of 4,4′-dibromodiphenyl ether (BDE-15) by GAC could best be described using the pseudo-second-order kinetic model and Freundlich isothermal adsorption model. The coexistence ions had almost no effect on the removal of BDE-15 and the recovery rate of TX-100, and the solution pH had little effect on the recovery rate of TX-100; BDE-15 had the best removal effect under the condition of weak acid to weak base, indicating that GAC has good environmental adaptability. After adsorption, GAC could be regenerated with methanol and the adsorption effect of BDE-15 could still reach more than 81%. Density functional theory (DFT) calculation and characterization results showed that, Van der Waals interaction and π–π interaction are dominant between BDE-15 and GAC, and hydrogen bond interactions also exist. The existence of oxygen-containing functional groups is conducive to the adsorption of BDE-15, and the carboxyl group (-COOH) has the strongest promoting effect. The study proved the feasibility of GAC to effectively remove PBDEs and recover surfactants from the soil-washing effluent, and revealed the interaction mechanism between PBDEs and GAC, which can provide reference for the application of soil-washing technology.Keywords:granular-activated carbon;polybrominated diphenyl ethers;Triton X-100;soil-washing effluent;adsorption;density functional theory calculation
研究领域:
环境科学
·
化学工程
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高影响因子
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