MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Yake Luo,Shanshan Ma,Bo Sui,Luyang Zhang,Ajuan Yu,Jiaheng Zhang,Yanhao Zhang,Wuduo Zhao,Gangfeng Ouyang
Perfluorooctanoic acid (PFOA) has aroused global attention due to its persistence, biotoxicity and bioaccumulative properties. Monitoring PFOA levels in biological samples could give significant insights into its toxicity mechanism and health risk evaluation. Herein, to explore the distribution of PFOA in biological tissues, an indirect quantitation strategy for PFOA in biological samples was proposed based on fluorescence spectroscopy. F - ion was produced through highly efficient degradation of PFOA in polar aprotic solvent, and then F - ion was detected with highly selective F - ion fluorescent probe, which enabled the indirect quantitative detection of PFOA in biological samples. The sensitivity for PFOA was exhibited with limit of detection of 3.55 μM. The method’s accuracy and precision were validated by spiked biological sample experiment, with recovery rate ranging from 93.2 % to 105.5 % and relative standard deviation below 9.2 %. The content of PFOA was successfully detected in rats livers, kidneys and lungs tissues. Density function theory was employed to explore defluorination pathway, indicating that heating, alkaline and water conditions played a crucial role in the degradation of PFOA to produce F - ion. Thus, this novel strategy is suitable for quantitative analysis of PFOA in biological samples with high selectivity, sensitivity, recovery ratio, and simple sample preparation, which also provides a strategy for evaluating the levels of per- and polyfluoroalkyl substances in biological samples.
研究领域:
分析化学
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环境科学
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毒理学
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生物医学工程
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DOI
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
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2022
·Vol. 23
·期 3
·1428-1438
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IF 3.536
Li Yulong,He Liuyang,Chen Yulin,Xue Jianming,Zheng Li,Yang Shengmao,Wu Li,Chen Zhendong,Zhang Zulin,Yang Lie
Purpose Perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) in soils pose a severe threat to the soil ecosystem and human health. Soil aggregates play a critical role in the migration and transformation of pollutants. Materials and methods In this study, soil with different properties (Fluvisol and Planosol) spiked with PFOA/PFOS were incubated for 90 days, and then divided into five particle size fractions by wet sieving with low loss. The concentrations of PFOA and PFOS in soils and fractions were extracted using ultrasound-assisted extraction method with methanol as an extractant. The PFOA and PFOS were analyzed using high-performance liquid chromatography-tandem mass spectrometry (HPLC–MS/MS). Results and discussion The results showed that the ability of the soil aggregates to carry PFOA and PFOS initially decreased and then increased with decreasing particle sizes. Moreover, organic matter was the main factor influencing the PFOA and PFOS distribution in the soil aggregates, whereas soil types did not affect the accumulation capacity of PFOA and PFOS on soil particles. The macroaggregates (2000–250 µm) showed the highest accumulation capacity of PFOA and PFOS, suggesting high load of PFOA and PFOS. Additionally, the microaggregates (< 15 µm) played a dominant role in the PFOA and PFOS distribution due to the high proportion of this fraction in soil samples (51.73 ~ 62.47%). Conclusions Significantly bipolar immigrations of PFOA and PFOS into macroaggregates and microaggregates in soils were observed. This phenomenon can be explained by the fact that the particulate organic carbon (POM) can sorb the PFOA and PFOS in the macroaggregates, while the presence of SOC (highly humified) may increase the PFOA and PFOS contents in the microaggregates. Graphical Abstract
研究领域:
环境科学
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土壤学
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污染研究
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Zhiwen Tang,Timothy M. Vogel,Qing Wang,Changlong Wei,Mukhtiar Ali,Xin Song
In this study, the biodegradability of trifluoroacetate (TFA), perfluorooctanoic acid (PFOA), and perfluoro-2-methyl-3-oxahexanoic acid (HFPO-DA) by a native microbial community was evaluated over a 10-month incubation period. The observed microbial defluorination ratios and removal efficiency were 3.46 ( ± 2.73) % and 8.03 ( ± 3.03) %, 8.44 ( ± 1.88) % and 13.52 ( ± 4.96) %, 3.02 ( ± 0.62) % and 5.45 ( ± 2.99) % for TFA, PFOA and HFPO-DA, respectively. The biodegradation intermediate products, TFA and pentafluoropropionic acid (PFA), of PFOA and HFPO-DA were detected in their biodegradation treatment groups. Furthermore, the concentrations of the PFOA metabolites, perfluorohexanoic acid (PFHxA) and perfluoroheptanoic acid (PFHpA), in the aqueous solutions after incubation were quantified to be 0.21 and 4.14 µg/L. TFA, PFOA and HFPO-DA significantly reduced the microbial diversity and changed the structure of the community. The co-occurrence network analysis showed that low abundance species, such as Flexilinea flocculi , Bacteriovorax stolpii , and g_Sphingomonas , are positively correlated with the generation of fluoride ion, implying their potential collaborative functions contributing to the observed biodefluorination. The findings in this study can provide insights for the biodegradation of perfluoroalkyl carboxylic acids and their emerging alternatives by indigenous microorganisms in the environment.
研究领域:
环境微生物学
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生物修复
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化学生态学
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DOI
PubMed
高影响因子
RSC Advances
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2015
·Vol. 5
·期 103
·84856-84864
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IF 3.84
Qianchi Ma,Lei Liu,Wei Cui,Ruifeng Li,Tingting Song,Zhaojie Cui
Model aqueous solutions of perfluorooctanoic acid (PFOA, 100 mg L−1) were electro-oxidized in a homemade container. The electrocatalytic behavior and anodic performance of Ti/SnO2–Sb/Yb–PbO2, Ti/SnO2–Sb–PbO2 and Ti/SnO2–Sb–Yb anodes in sodium electrolytes were compared. The SnO2–Sb/Yb–PbO2 anode demonstrated better electrocatalytic performance compared with the SnO2–Sb–PbO2 and SnO2–Sb–Yb electrodes in terms of both degradation and defluorination. Then a systematic experimental study was designed as follows to analyze the influencing factors: initial concentration of PFOA (10 mg L−1 to 200 mg L−1), current density (1 mA cm−2 to 40 mA cm−2), initial pH value (3 to 11) and electrode distance (5 mm to 20 mm). After a 150 min electrolysis, the optimum reaction conditions were obtained and the degradation and defluorination ratios reached 95.11 ± 3.9% and 75.7 ± 2.8%, respectively. Under the optimum conditions, the degradation of PFOA followed pseudo-first-order kinetics (0.0193 min−1) and the degradation half-life was 35.9 min. The produced F− was measured using a fluoride ion selective electrode, whereas the intermediate PFCAs with short-chain lengths were measured using HPLC-MS. A detailed degradation pathway was proposed in this study by analyzing the intermediates and the recovery of fluoride.
研究领域:
环境科学
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化学工程
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分析化学
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产品关联
DOI
高影响因子
Journal of Water Process Engineering
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2023
·
IF 7
Wei Zhang,Qing Long,Guifeng Li,Zigong Ning,Lu Lu
Hydrated electron reduction in an ultraviolet (UV)-sulfite system and electrochemical oxidation on a boron doped diamond (BDD) anode both are efficient processes for the degradation of perfluorooctanoic acid (PFOA). However, hydrated electron reduction has inherent deficiency in the mineralization (i.e., converting organic carbon into CO 2 ) of PFOA. Furthermore, toxic byproducts such as partially hydrodefluorinated carboxylic acids (HDCAs) and perfluorosulfonic acids (PFSAs) might give secondary pollution if the wholly hydrodefluorination of PFOA is not achieved. BDD electrochemical oxidation can obtain a high mineralization efficiency, but it leads to a low defluorination (i.e., transforming C−F bonds into F − ions) efficiency due to the generation of toxic volatile fluorinated alkanes. Herein, we report a coupled process that is hydrated electron reduction as pre-treatment and BDD electrochemical oxidation as post-treatment to achieve a complete defluorination and mineralization of PFOA, the results demonstrate that 50 mg/L PFOA can be 100 % deluorinated and mineralized under 5 h UV-sulfite reduction followed by 10 h electrochemical oxidation. This coupled process strongly inhibits the production of the toxic volatile fluorinated pollutants and quickly converts the residual toxic sulfite in UV-sulfite system to the sulfate. Mechanism investigation demonstrates that BDD oxidation is able to transform HDCAs and PFSAs formed by hydrated electron reduction to the perfluorocarboxylic acids (PFCAs) with shorter carbon chain than PFOA, which can be further defluorinated and mineralized.
研究领域:
环境科学
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化学工程
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水处理
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污染物降解
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产品关联
DOI
高影响因子
TOXICOLOGY
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2025
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IF 4.6
Mei-Ling Le,Jia-Yu Xue,Li-Hai Wu,Xin-Yuan Zhao,Jing Ding,Yang-Yang Yuan,Yi-Qi Wan,Da-Lei Zhang
Hexafluoropropylene oxide (HFPO) homologues (HFPOs), specifically HFPO-dimeric acid (DA), HFPO-trimeric acid (TA) and HFPO-tetrameric acid (TeA), have emerged as industrial replacements for phased-out perfluorooctanoic acid (PFOA), garnering considerable attention due to their environmental ubiquity and bioaccumulation potential. Nevertheless, the reproductive toxicity of HFPOs remains incompletely characterized, particularly regarding their endocrine-disrupting effect and the underlying mechanisms involving Leydig cell dysfunction. In this study, we investigated the cytotoxic influences of HFPOs on TM3 Leydig cells, focusing on mitochondrial function and dynamics, oxidative stress, and apoptosis. Our findings demonstrated that exposure to HFPOs significantly compromised mitochondrial function and fusion-fission dynamics by disrupting the SIRT1/PGC1α signaling pathway. The mitochondrial dysfunction further triggered excessive ROS production and apoptosis, ultimately impairing TM3 Leydig cell viability and testosterone secretion. However, supplementation with the SIRT1 agonist SRT1720 relieved the inhibitory effect of HFPOs on SIRT1/PGC1α signaling pathway and reversed the expression of apoptosis-associated proteins (BAX/BCL2), oxidative stress-associated proteins (SOD1/SOD2), as well as proteins associated with mitochondrial fusion (MFN2/OPA1) and fission (DRP1/FIS1). These results elucidated the involvement of the SIRT1/PGC1α pathway in mediating the cytotoxicity of HFPOs. Notably, the activation of SIRT1 mitigated HFPO-induced toxicity in the TM3 cells, uncovering its potential in safeguarding testicular cells from the damage caused by HFPOs exposure.
研究领域:
毒理学
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环境健康
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内分泌学
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生殖生物学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2020
·
IF 7.864
Tuan-Tuan Wang,Guang-Guo Ying,Wen-Jun Shi,Jian-Liang Zhao,You-Sheng Liu,Jun Chen,Dong-Dong Ma,Qian Xiong
Perfluoroalkyl substances (PFASs) are persistent chemicals in the environment. So far, little is known about their uptake potential in wetland plants. Here, we investigated the uptake and translocation of perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) in eight common wetland plants, namely, Canna indica (Ci), Thalia dealbata (Td), Cyperus alternifolius (Ca), Phragmites australis (Pa), Arundo donax (Ad), Pontederia cordata (Pc), Cyperus papyrus (Cp), and Alisma orientale (Ao) by hydroponic experiments and visualized their tissue- and cell-level distribution with desorption electrospray ionization mass spectrometry (DESI-MS) and transmission electron microscopy equipped with energy-dispersive spectroscopy (TEM-EDS). The results showed that the PFASs accumulated in plants accounted for 1.67–16.7% of the total mass spiked into the hydroponic systems, and PFOS accumulated largely in roots (48.8–95.8%), while PFOA was stored mostly in the aboveground part (29.3–77.4%). DESI-MS and TEM-EDS analysis showed that PFASs in Ci, Td, Pa, and Ca were transported from the hydroponic solution to the root cortex via both apoplastic (e.g., across cell walls and/or intercellular spaces) and symplastic routes (e.g., across plasma membranes or via plasmodesmata) and further to the vascular bundle via symplastic route in Td and Pa and via both routes in Ci and Ca. These two chemicals were transported from roots to stems mainly through the cortex in Td and through both the cortex and vascular bundles in Ci and Ca.
研究领域:
环境科学
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植物生理学
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分析化学
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DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2021
·
IF 4.098
Fang Zhang,Jiaman Liang,Yang Liu,Qiuju Zhou,Yushuang Hong,Xianping Chen,Kejun Tan
Perfluorooctanoic acid (PFOA) and Perfluorooctane sulfonate (PFOS) are two typical perfluorinated compounds (PFCs) that poss potential ecological toxicity . In this work, a fluorescence and resonance light scattering (RLS) dual-readout strategy for the detection of PFCs at picomole level based on the water-soluble CdTe quantum dots (CdTe QDs) has been proposed. It is found that the CdTe QDs exhibit a quenching in the presence of PFCs and thus serve as useful probes for PFCs. The linear ranges are 0.032 – 10.0 nM with a limit of detection(LOD) of 32.02 pM for PFOA and 0.044 – 15.0 nM with a LOD of 43.96 pM for PFOS, respectively. Meanwhile, PFCs can form complexes with CdTe QDs in acid medium , resulting in remarkable RLS signals. The enhanced RLS intensities are in proportion to the concentrations of PFOA and PFOS, respectively. And the linear ranges are 0.048 – 5.0 nM with a LOD of 47.78 pM for PFOA, and 0.057 – 5.0 nM with a LOD of 56.72 pM for PFOS, respectively. This dual-mode detection increases the reliability of the measurement. The proposed method is simple, sensitive and cost-effective, with potential applications in environmental monitoring and assessment.
研究领域:
环境科学
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分析化学
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毒理学
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DOI
PubMed
高影响因子
WATER RESEARCH
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2022
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IF 13.4
Xianjun Tan,Zhenying Jiang,Wenhui Ding,Mingkun Zhang,Yuxiong Huang
The global occurrence of per- and polyfluoroalkyl substances (PFAS) in aquatic systems has raised concerns about their adverse effects on ecosystems and human health. Adsorption is a promising technique for the remediation of PFAS, yet effective adsorbents with rapid uptake kinetics and high adsorption capacity are still in high demand, and molecular-level understanding of the interfacial adsorption mechanisms is lacking. In this study, we developed a superior layered rare-earth hydroxide (LRH) adsorbent, ultrathin Y 2 (OH) 4.86 Cl 1.44 ·1·07H 2 O (namely YOHCl) nanosheets, to achieve the effective removal of perfluorooctanoic acid (PFOA). YOHCl nanosheets exhibited ultra-high adsorption capacity toward PFOA (up to 957.1 mg/g), which is 1.9 times and 9.3 times higher than the state-of-the-art layered double hydroxides (MgAl-LDH) and benchmark granular activated carbon (GAC) under the same conditions, respectively. Furthermore, YOHCl nanosheets pose stable performance on the removal of PFOA under various water matrices with robust reusability. We also developed YOHCl-based continuous-flow column, demonstrating its promise in simultaneously removing multiple PFAS with wide range of chain lengths at environmentally relevant concentrations. With the molecular-level investigations, we have revealed that multi-mechanism, including ion exchange, electrostatic attraction and bidentate/bridging coordination, contributed to the strong PFOA-YOHCl affinity, leading to the ultra-high adsorption capacity of PFOA. We have provided emerging LRHs-based adsorbents for the effective remediation of PFAS with molecular-level insights on the interfacial mechanisms.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Huike Dong,Guanghua Lu,Zhenhua Yan,Jianchao Liu,Yong Ji
Perfluorooctanoic acid (PFOA) has long been produced and widely used due to its excellent water and oil repellent properties. However, this trend has facilitated to the ubiquitous existence of PFOA in environmental matrix, and the potential ecotoxicity on aquatic organisms has not been fully elucidated. To study the tissue-specific bioconcentration and the nervous system- and energy-related biochemical effects of PFOA, as well as the phenotypic alterations by this chemical, male crucian carp ( Carassius auratus ) were exposed to gradient concentrations of PFOA (nominal 0.2, 10, 500 and 25,000 μg/L) in a flow-through apparatus for 7 days. PFOA was enriched in tissues following an order of blood > kidney ≥ liver > gill > brain > muscle. The bioconcentration factors ranged from 0.1 to 60.4. Acetylcholinesterase activity in the fish brain was inhibited, while liver carboxylesterase was induced in most cases and attenuated with time. The acyl-CoA oxidase activity was dose-dependently elevated and accompanied by a decline of ATP contents. PFOA treatments also inhibited the activity of the electron transport system (ETS). At the transcriptional level, ETS component complexes II and IV were concordantly depressed, and ATP synthesis was also downregulated. The mRNA level of peroxisome proliferator activated receptor α was increasingly upregulated, with related downstream genes upregulated in varying degrees. The phenotypes showed patterns of increased liver pathology and reduced swimming activity. In summary, PFOA leads to adverse effects in Carassius auratus related to multiple aspects, which may be associated with the nervous system, fundamental energy metabolism and other unpredictable factors. The results obtained in this study are expected to help clarify the PFOA toxic mechanisms on energy relevance.
研究领域:
环境科学
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毒理学
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鱼类生理学
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产品关联
DOI
PubMed
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 8
·2229-2239
·
IF 7.683
Xianjun Tan,Guanhan Chen,Dingyu Xing,Wenhui Ding,Hao Liu,Ting Li,Yuxiong Huang
More and more attention has been redirected to per- and polyfluorinated alkyl substances (PFASs), particularly perfluorooctanoic acid (PFOA), owing to their ecotoxicity and environmental risks. As one of the major emerging and persistent contaminants in the environment, the current treatment processes could not remove PFOA efficiently. The recent advances in heterogeneous photocatalysis have demonstrated high efficiencies in degrading persistent contaminants, which provides an alternative approach for PFOA removal. Notably, Ga2O3-based photocatalysts exhibited great potential for PFOA remediation due to their high oxidizing capability and energy sustainability. Thus, Ga2O3 hierarchical nanosheets modified by a series of transition metals were rationally developed, and applied as heterogeneous photocatalysts for fast and efficient PFOA degradation. Noteworthily, the indium modified Ga2O3 hierarchical nanosheets achieved prominent PFOA decomposition activity, which can completely degrade 20 mg L−1 PFOA within 1 hour. The In–Ga2O3 hierarchical composites have dramatically enhanced the degradation kinetics for PFOA, which was 7.8 times higher than that of pristine Ga2O3. With in-depth mechanism investigation, we have demonstrated that In modification can not only enhance light harvesting and suppress photogenerated carrier recombination, but also favor the improvement of the adsorption ability for PFOA through the coexistence of monodentate and bidentate/bridging coordination modes. The transition metals–modification strategy paves the way for fabricating high-performance nanoscale photocatalysts for the removal of PFASs in water.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Jiye Huang,Xi Wang,Zhaoqi Pan,Xukai Li,Yu Ling,Laisheng Li
Perfluorooctanoic acid (PFOA) could be efficiently degraded by the combined process of photocatalysis and ozonation, its degradation intermediates were fluoride ions and short-chain perfluorocarboxylic acids (PFCAs) including C 6 F 13 COOH, C 5 F 11 COOH, C 4 F 9 COOH, C 3 F 7 COOH and C 2 F 5 COOH. After 4 h reaction time, its degradation efficiency was 99.1% and defluorination ratio only reached to 44.3%. The degradation mechanism of PFOA by photocatalytic ozonation was proposed and found to be similar to Photo-Kolbe reaction: PFOA anion was degraded to produce PFOA radical by a direct electron transfer from its carboxyl group to photo-generated hole (h + ). Then PFOA radical was decarboxylated to produce perfluoroheptyl radical, and then be oxidized to form C 7 F 15 OH by hydroxyl radical ( OH) which was produced from ozone trapping photo-generated electron. Because of its thermal instability, C 7 F 15 OH would be converted to C 6 F 13 COF, which was further hydrolyzed to generate C 6 F 13 COO − . Therefore the combined process of photocatalysis and ozonation was efficient for PFOA degradation.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）