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PFOA
SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Two-in-one platform based on conjugated polymer for ultrasensitive ratiometric detection and efficient removal of perfluoroalkyl substances from environmental water

Xiaoyi Chen,Sameer Hussain,Yuhai Tang,Xi Chen,Sijie Zhang,Yue Wang,Pei Zhang,Ruixia Gao,Sicen Wang,Yi Hao

Continuous emergence of persistent organic pollutants perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS) in various water bodies around the world poses a serious threat to the global ecosystem. The exploration of advanced detection/removal techniques to monitor/treat such type of toxicants is urgently required. Herein, we unveiled a donor-acceptor type conjugated polymer PF-DBT-Im as a first-of-its-kind ratiometric fluorescent probe for visual, amplified, and specific monitoring of PFOA and PFOS with ultra-low detection limits of 6.12 nM (PFOA) and 14.3 nM (PFOS), respectively. PF-DBT-Im undergoes strong aggregation after binding with PFOA/PFOS as evident by transmission electron microscopy , zeta potential measurements, and dynamic light scattering studies. This promotes interchain Förster resonance energy transfer process to endorse an obvious emission color change from blue-to-magenta under ultraviolet lamp excitation. Consequently, a smartphone-integrated portable device is fabricated for realizing rapid and on-site detection of PFOA/PFOS. Besides, a new class of magnetic adsorbent Fe 3 O 4 @NH 2 &F 13 is also prepared and used in combination with PF-DBT-Im to remove PFOA/PFOS from the environmental water effectively and rapidly as confirmed by liquid chromatography-mass spectrometry analysis. Thus, utilizing the excellent signal amplification property of PF-DBT-Im and the remarkable magnetic separation capability of Fe 3 O 4 @NH 2 &F 13 , a multifunctional system is developed for step-wise recognition and separation of PFOA/PFOS from the environmental water proficiently and rapidly.

研究领域: 环境科学 · 分析化学 · 材料科学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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TOXICOLOGY · 2023 · IF 4.5

Direct inhibition of human and rat 11β-hydroxysteroid dehydrogenase 2 by per- and polyfluoroalkyl substances: Structure-activity relationship and in silico docking analysis

Congcong Zhao,Shaowei Wang,Yingna Zhai,Mengyun Wang,Yunbing Tang,Huitao Li,Young Jun Im,Ren-shan Ge

Per- and polyfluoroalkyl substances (PFAS) are persistent in the environment and may disrupt the endocrine system. Our previous study showed that perfluorooctanoic acid (PFOA, C8) and perfluorooctanesulfonic acid (PFOS, C8S) can inhibit 11β-hydroxysteroid dehydrogenase 2 (11β-HSD2) activity leading to an active glucocorticoid accumulation. In this study, we extended investigation for 17 PFAS, including carboxylic and sulfonic acids , with different carbon-chain lengths, to determine their inhibitory potency and structure-activity relationship in human placental and rat renal 11β-HSD2. C8-C14 PFAS at 100 μM significantly inhibited human 11β-HSD2 with a potency as C10 (half-maximal inhibitory concentration, IC 50 , 9.19 μM) >  C11 (15.09 μM) > C12 (18.43 μM) > C9 (20.93 μM) > C13 (124 μM) > C14 (147.3 μM) > other C4-C7 carboxylic acids , and C8S > C7S = C10S > other sulfonic acids. For rat 11β-HSD2, only C9 and C10 and C7S and C8S PFAS exhibited significant inhibitory effects. PFAS are primarily mixed/competitive inhibitors of human 11β-HSD2. Preincubation and simultaneous incubation with the reducing agent dithiothreitol significantly increased human 11β-HSD2 but not rat 11β-HSD2, and preincubation but not simultaneous incubation with dithiothreitol partially reversed C10-mediated inhibition on human 11β-HSD2. Docking analysis showed that all PFAS bound to the steroid-binding site and carbon-chain length determined the potency of inhibition, with the optimal molecular length (12.6 Å) for potent inhibitors PFDA and PFOS, which is comparable to the molecular length (12.7 Å) of the substrate cortisol . The length between 8.9 and 17.2 Å is the probable threshold molecular length to inhibit human 11β-HSD2. In conclusion, the carbon-chain length determines the inhibitory effect of PFAS on human and rat 11β-HSD2, and the inhibitory potency of long-chain PFAS on human and rat 11β-HSD2 showed V-shaped pattern. Long-chain PFAS may partially act on the cysteine residues of human 11β-HSD2.

研究领域: 环境科学 · 毒理学 · 内分泌学 · 分子生物学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Energy-efficient mineralization of perfluorooctanoic acid: Biomass energy driven solar photo-electro-fenton catalysis and mechanism study

Yang Wang,Shuaishuai Li,Yanming Shao,Liming Jing,Rongkai Ren,Liweng Ma,Xu Wang,Zhijian Li,Jianzhi Wang,Chen Hou

The smart eco-friendly biomass energy driven electrical degradation system was established by coupling of glucose fuel cells (GFC) and solar photo-electro-Fenton (SPEF) processes, which was proposed for the green, economical and efficient degradation of perfluorooctanic acid (PFOA). The CoFe alloy nanoparticles with oxygen defects (O*) based on metal–organic frameworks (MOFs) were decorated on polyacrylonitrile (PAN)-driven carbon nanofiber (CNF) membrane to obtain the bifunctional photocathode (CoFe-OVs@CNF) with both extraordinary photo-catalytic and electro-catalytic abilities. PFOA was highly mineralized on CoFe-OVs@CNF through the synergy of photocatalytic oxidation and electro-Fenton processes. Moreover, the energy consumption for degradation was generated from direct electro-oxidation of glucose as the clean power on anode (GFC). The possible mechanism and degradation pathway for PFOA mineralization was investigated in detail according to intermediate analysis, active species verification and the valence state change of Co and Fe on cathode. Besides, the toxicity evolution during PFOA degradation was also evaluated to deeper insight into risk assessment of intermedia products and relative toxicity, intending to prove the potential for practical elimination of PFOA and other toxicity recalcitrant pollutants in wastewater by GFC-SPEF system.

研究领域: 环境工程 · 化学工程 · 材料科学 · 环境科学
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WATER RESEARCH · 2024 · IF 11.4

Dielectric Barrier Discharge (DBD) enhanced Fenton process for landfill leachate nanofiltration: Organic matter removal and membrane fouling alleviation

Danjing Lu,Xin Mao,Ruoxi Wu,Bin Liu

This study investigated a sustainable approach through dielectric barrier discharge (DBD) enhanced Fenton technology coupling nanofiltration (NF) process for landfill leachate treatment. The DBD/Fe(II)/H 2 O 2 system exhibited significant synergistic effects, removing 55.07 % of TOC and 53.79 % of UV 254 within 60 min, respectively. Additionally, the DBD/Fe(II)/H 2 O 2 system demonstrated exceptional performance in removing fluorescent substances and large molecular organic compounds, thereby reducing the formation of cake layer on the nanofiltration membrane. Moreover, membrane flux increased by 2.34 times, with reversible and irreversible resistances decreasing by 75.79 % and 81.55 %, respectively. Quenching experiments revealed ·OH as the primary active species for perfluorooctanoic acid (PFOA) degradation in the DBD/Fe(II)/H 2 O 2 process. The degradation pathway of PFOA was also elucidated via capillary electrophoresis-quadrupole time-of-flight mass spectrometry analysis. Correlation analysis indicated that TOC and EEM were the primary fouling factors. Lastly, through an assessment of energy consumption, economic costs, and carbon dioxide emissions, the advantages and practical application potential of the DBD/Fe(II)/H 2 O 2 system were demonstrated. In summary, the DBD/Fe(II)/H 2 O 2 system emerges as a feasible strategy for NF pretreatment, holding immense potential for treating landfill leachate.

研究领域: 环境工程 · 水处理 · 膜技术 · 高级氧化过程
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ENVIRONMENTAL POLLUTION · 2024 · IF 7.6

Immunotoxicity of legacy and alternative per- and polyfluoroalkyl substances on zebrafish larvae

Dengdiao Yao,Jian Shao,Dantong Jia,Weiling Sun

Hexafluoropropylene oxide dimer acid (HFPO-DA) and perfluoroethylcyclohexane sulfonate (PFECHS) are increasingly used as alternatives for perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS). However, their immunotoxicity and underlying molecular mechanisms remain poorly understood. Here, to assess immunotoxic effects, zebrafish embryos were exposed to environmentally relevant concentrations of PFOA, PFOS, HFPO-DA, and PFECHS for four days. Results revealed that all four per- and polyfluoroalkyl substances (PFAS) resulted in decreased heart rate and spontaneous movement, and induced oxidative stress in zebrafish larvae. Notably, HFPO-DA exhibited more severe oxidative stress than PFOA. Immune dysfunction was observed, characterized by elevated cytokine, complement factor, nitric oxide, and neutrophil content, along with a significant decrease in lysozyme content. Transcriptomic analysis revealed the activation of Toll-like receptor (TLR)/NOD-like receptor (NLR)/RIG-I-like receptor (RLR) and associated downstream genes, indicating their pivotal role in PFAS-induced immunomodulation. Molecular docking simulations demonstrated stable interactions between PFAS and key receptors (TLR2, NOD2 and RIG-I). Overall, HFPO-DA and PFECHS exhibited immunotoxic effects in zebrafish larvae similar to legacy PFAS, providing important information for understanding the toxic mode of action of these emerging alternatives.

CAS / MDL: 13252-13-6
研究领域: 环境毒理学 · 免疫学 · 分子生物学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Air superhydrophilic-superoleophobic SiO2-based coatings for recoverable oil/water separation mesh with high flux and mechanical stability

Wei Xiong,Ling Li,Fen Qiao,Junwu Chen,Zhi Chen,Xuedong Zhou,Kaiwen Hu,Xiujian Zhao,Yi Xie

Due to the inherent differences in surface tension between water and oil, it is a challenge to fabricate air superhydrophilic-superoleophobic materials despite their promising potential in the field of oil/water separation. Herein, a facile approach is developed to fabricate air superhydrophilic-superoleophobic SiO 2 coating by combination of controllable modifying SiO 2 nanoparticle surface by both hydrophilic groups (i.e., –OH groups) and oleophobic groups (i.e., fluorinated groups) with constructing porous and hierarchical structures. Hydroxyl-modified SiO 2 nanoparticles (NPs) are synthesized using a base-catalysed procedure in the presence of ammonia or NaOH. Chitosan quaternary ammonium salt (HACC) is introduced to bind SiO 2 by forming a unique hydrogen bond between HACC and –OH, followed by adding pentadecafluorooctanoic acid (PFOA) to complex with HACC to form fluorinated groups. The SiO 2 coatings are fabricated on various substrates (e.g., glass, foam and Cu mesh) by spraying procedure and characterized using SEM, FTIR, XPS, etc. The contact angles of oils (e.g., pump oil, castor oil , corn oil, hexadecane and bean oil) and water on the coatings are over 150° and close to 0°, respectively. By optimization, the representative SiO 2 -coated Cu mesh displayed high - efficiency of 99.2% in separating water from mixture of water/pump oil, and high penetration flux of 1.41 × 10 4 L·m −2 ·h −1 . Besides, the coating maintains its superhydrophilic-superoleophobic properties even after 110 cycles of sandpaper abrasion or after being immersed in water for 3 h. After 20 cycles of oil/water separation, the coating retains separation efficiency up to 97.93%. This study provides a new and universal protocol to fabricate unique superwetting surfaces with effective oil/water separation performance, long-term durability and outstanding reusability.

研究领域: 材料科学 · 表面化学 · 环境工程
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