JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Jianqiao Xu,Junyan Wei,Ruixue Guo,Shengnan Zhang,Xiaolei Teng,Zunyao Wang,Ruijuan Qu
Decachlorobiphenyl (PCB-209) can be widely detected in suspended particles and sediments due to its large hydrophobicity, and some of its transformation products may potentially threaten organisms through the food chain. Here we investigate the photochemical transformation of PCB-209 on suspended particles from the Yellow River. It was found that the suspended particles had an obvious shielding effect to largely inhibit the photodegradation of PCB-209. Meanwhile, the presence of inorganic ions (e.g. Mg 2+ and NO 3 - ) and organic matters (e.g. humic acid, HA) in the Yellow River water inhibited the reaction. The main transformation products of PCB-209 were lower-chlorinated and hydroxylated polychlorinated biphenyls (OH-PCBs), and small amounts of pentachlorophenol (PCP) and polychlorinated dibenzofurans (PCDFs) were also observed. The mechanisms of PCP formation by double •OH attacking carbon bridge and PCDFs formation by elimination reaction of ionic state OH-PCBs were proposed using theoretical calculations, which provided some new insights into the inter-transformations between persistent organic pollutants. In combination with VEGA and EPI Suite software, some intermediates such as PCDFs were more toxic to organisms than PCB-209. This study deepens the understanding of the transformation behavior of PCB-209 on suspended particles under sunlight.
研究领域:
环境科学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Jianqiao Xu,Junyan Wei,Jiayu Zhang,Zhicheng Xing,Zunyao Wang,Ruijuan Qu
Dissolved organic matter (DOM) can affect the transformation of pollutants through photosensitization, but most current research focuses on hydrophilic pollutants, making it such that less attention is paid to hydrophobic pollutants. In this paper, the effect and action mechanism of coexisting DOM on the photodegradation of decachlorobiphenyl (PCB-209) on suspended particles collected from the Yellow River were systematically investigated in a heterogeneous system using DOM standards and model compounds. Through molecular probe experiments, mass spectrometry analysis and theoretical calculations, we found that the excited triplet state of DOM (3DOM*) could excite PCB-209 to undergo dechlorination reaction. Due to the different modes of electron transition, the presence of carbonyl groups decreased the energy of 3DOM*, whereas the electron-donating groups made the energy of 3DOM* higher. DOM containing phenolic hydroxyl groups led to a higher steady-state concentration of •OH, and DOM containing phenyl ketone structures had a stronger ability to produce •O2–. Compared with aqueous •OH, •O2– produced from hydrophobic microregions could react more readily with PCB-209. This study deepens the understanding of the role of different functional groups of DOM in the photosensitized transformation of hydrophobic compounds.
研究领域:
环境科学
·
理论化学
·
污染生态学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2025
·
IF 8
Xiang Shen,Zheshan Duan,Xike Tian,Hongtao Zheng,Dongsheng Wang,Xubo Gao
Inland freshwater is an essential resource for human survival and development; however, the occurrence of organochlorine pesticides (OCPs) in the largest freshwater lake in northern China remains largely unknown. Among the 24 OCPs detected in the lake sediments, hexachlorocyclohexanes (HCHs) and dichlorodiphenyltrichloroethanes (DDTs) were predominant compounds. The most abundant isomers were β-HCH and p,p'-DDT, reflecting their extensive use in agriculture and aquaculture. The Fuhe River, a critical channel for agricultural irrigation and domestic sewage, was identified as the primary pathway for transporting OCPs from upstream sources into Baiyang Lake. The residual OCPs in surface sediments were higher than those in deeper sediments, indicating the recent input of lindane, dicofol and dieldrin. Especially, the α-HCH/γ-HCH ratios (0–1.8) in the sediment cores, indicated a mixed historical input of both lindane and technical HCHs. The o,p'-DDT/p,p'-DDT > 0.5 in the bottom sediments were attributed to the earlier use of technical DDT. Notably, the DDTs in the upstream section of the Fuhe River, with high ERM values, posed a significant ecological risk, whereas the levels of DDD, DDE, and chlordane in the sediments were below the ERL values, indicating low potential ecological risks. The sediment assessment indicated potential ecological risks from HCHs and dieldrin in the residential areas. In contrast, the sediment-associated surface water posed no significant carcinogenic or non-carcinogenic risks to humans.
研究领域:
环境科学
·
生态毒理学
·
水文学
·
污染研究
·
沉积物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Jianqiao Xu,Xinyuan Wei,Junyan Wei,Mengqiang He,Xiaolei Teng,Zunyao Wang,Ruijuan Qu
While the reaction mechanism of direct photochemical dechlorination has been extensively studied, significant knowledge gaps remain regarding the specific roles of reactive species in governing dechlorination pathways during indirect photodegradation. By integrating mass spectrometry analysis, probe experiments and theoretical calculations, we propose for the first time an indirect dechlorination reaction mechanism for PCB-209 involving active species commonly found in DOM photosensitive systems, which differs significantly from that of direct photodegradation. Due to the lower bond energy of the C Cl bond at the position opposite the carbon bridge, PCB-209 primarily yielded PCB-208 in direct dechlorination systems. However, our study revealed that active species ( 3 DOM*, •O 2 − and 1 O 2 ) can specifically weaken the meta-positioned C Cl bond at the carbon bridge through electron transfer and cycloaddition mechanisms, thereby fundamentally altering the regioselectivity of dechlorination. Remarkably, our results confirm the indirect degradation of PCB-209 through DOM photosensitization to form dechlorination products dominated by PCB-207, a previously unrecognized transformation pathway in natural photochemical processes. This study refines the mechanism of indirect dechlorination mediated by reactive species and provides a predictive framework for the environmental fate of halogenated pollutants in real complex environmental systems.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Environmental Technology & Innovation
·
2024
·
IF 6.7
Kunfeng Zhang,Sheng Chang,Qi Zhang,Yunsong Bai,Enrui Wang,Yueting Fan,Xiang Tu,Qing Fu,Liangliang Wei,Yanling Yu
This study investigates the composition and distribution of 16 priority polycyclic aromatic hydrocarbons (PAHs) in 70 water samples collected from centralized drinking water sources (CDWSs) across 30 provinces (cities) in mainland China. Additionally, water quality and socio-economic data were collected to determine the influencing factors. The study discovered that the total concentrations of 16 priority PAHs (Σ 16 PAHs) varied from 0.17 to 176.71 ng/L (mean: 56.49 ± 38.58 ng/L). Lakes and reservoirs had significantly higher concentrations of PAHs than groundwater. The primary pollutants were low-molecular-weight (LMW) PAHs, such as phenanthrene, naphthalene, and fluorene. There was a strong correlation between LMW PAHs and Σ 16 PAHs ( p < 0.05). The mean Σ 16 PAHs in the seven geo-environmental zones were ranked as follows, under the comprehensive influence of emission density, natural, and social environmental factors: Northwest China (78.42 ± 66.96 ng/L) > Northeast China (73.70 ± 33.23 ng/L) > East China (64.35 ± 45.66 ng/L) > North China (50.95 ± 31.87 ng/L) > Southwest China (44.05 ± 32.56 ng/L) > Central China (41.68 ± 19.44 ng/L) > Southern China (40.99 ± 16.54 ng/L). The source modeling analysis revealed that the majority of PAHs came from chemical production and metal smelting (42.36%), as well as from the combustion of coal, wood, and biomass (34.17%), and other mixed sources. In addition, the study found a strong correlation between water quality and socio-economic factors with concentrations of PAHs, indicating that these factors may contribute to the re-enrichment, transport, and transformation of PAHs in overlying water to varying degrees. The mean incremental lifetime cancer risk (ILCR) was lower than the risk threshold. These findings provide scientific references for managing hazardous substances in the aquatic environment.
研究领域:
环境科学
·
公共卫生
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 10
·5506-5511
·
IF 3.361
Lin Yuan,Qiang Fu,Maojuan Zhou,Yunqian Ma,Lihua Zang,Yingjian Qin,Dandan Ji,Fengshan Zhang
Polychlorinated biphenyls (PCBs) are synthetic organic compounds that are extremely difficult to break down in water and can accumulate in human fat and organisms. However, methods that can be used to detect large amounts of PCBs remain unsatisfactory, as they are generally overly sensitive and involve complex operations. An aptamer-based catalytic hairpin assembly (aptamer-CHA) reaction for the selective detection of 3,3′,4,4′-tetrachlorobiphenyl (PCB 77) was developed. It combines the advantages of aptamers and signal amplification reactions. The aptamer selectivity recognizes the target, PCB 77, which triggers the sensitive CHA reaction to produce a fluorescence signal. CHA is a sensitive enzyme-free signal amplification method suitable for on-site detection. Therefore, the identification aptamer is the basis for the quantitative detection of PCB 77, with a detection range of 0.01 μg L−1 to 500 μg L−1 and a detection limit of 0.01 μg L−1. In this study, the aptamer was used to improve the selectivity of the reaction, and the CHA reaction improved the sensitivity of the detection system. Such high-sensitivity PCB detection capabilities with simplified procedures may be useful for real-time field detection and other monitoring tasks. This method can be used as a rapid fluorescence detection strategy for other targets in aquatic environments.
研究领域:
环境科学
·
分析化学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Linfeng Chen,Xike Tian,Yong Li,Chao Yang,Yunjie Huang,Yulun Nie
Simple and rapid sensing of polycyclic aromatic hydrocarbons (PAHs) remains a great technical challenge due to their chemical stability and structural similarity. Here, a simple, sensitive and cost-effective sensing strategy is proposed to detect multiple PAHs by utilizing the inner filter effect (IFE) and a reusable fluorescent sensor array consisting of four polyvinyl alcohol (PVA) composite carbon quantum dots (CDs) film sensors. The CDs/PVA films have a wide and tunable excitation range, which provide sufficient spectral overlap with PAHs and ensure the efficient occurrence of IFE. Under different excitations, the diverse UV absorption capacities of PAHs resulted in diverse spectral responses , enabling a unique chemical fingerprint for each PAH. Upon multivariate pattern recognition analysis, the array rendered high-throughput discrimination and sensitive quantification of 16 priority PAHs with 100% classification accuracy and detection limit as low as 57 nM. Moreover, the rapid and accurate screening of multiple environmental samples were also realized with the results consistent with high-performance liquid chromatography . This IFE-based reusable array is readily prepared, green and feasible, which exhibits great potential in environmental analysis and brings an advanced strategy to high-throughput sensing of more pollutants with similar structures and lack of recognition sites.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Zhaochao Deng,Songtao Hu,Leiming Tang,Lingbo Jiang,Junyu He,Keyu Shen,Yongjiu Xu,Rijin Jiang,Tiejun Li,Chunlei Chen,Bairu Chen,Hanghai Zhou,Dongdong Zhang,Jiawang Chen,Chunfang Zhang
The distribution characteristics and drivers of carbazole (CZ) and polyhalogenated carbazoles are still poorly understood. In this study, 96 samples were collected around the Zhoushan Archipelago, and their distribution characteristics were assessed. The results showed that CZ, 36-CCZ, and 36-BCZ were the top three abundant congeners in most collected samples. The bioaccumulation analysis revealed that marine plants prefer to accumulate CZ and bromocarbazoles rather than chlorocarbazoles. Both the mean concentrations of total carbazole and its derivants (ΣCZDs), as well as individual congeners, are the highest in sediments around the berthing areas of cargo ships and oil tankers . Meanwhile, ΣCZDs of these sediments are significantly influenced by the geo-weighted displacement of ships ( r = 0.61; p < 0.05), indicating the ballast water from these ships as potential contributor for marine CZDs. Moreover, the accumulation of CZ in plankton, planktonic origin of sedimentary organic matter, and relationship between CZ and C/N ratio ( p < 0.05) in sediments support the scenario that plankton absorbs and takes CZ into the sediments. These findings will promote the understanding of the sources, environmental behaviors, and fates of marine CZDs.
研究领域:
海洋生态学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）