JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Zhenguo Qi,Xin Huang,Min Wang,Chunfeng Lv,Baoyou Shi
Activated carbon (AC) filtration is an effective technique to remove emerging contaminants in drinking water treatment plants. Adsorption onto AC and biodegradation by biofilm are two main mechanisms for the removal of emerging contaminants such as antibiotics. However, the effects of highly bioaccumulative and toxic poly- and perfluoroalkyl substances (PFAS) on antibiotic removal by AC filtration have not been well-understood. In this work, two AC columns were built and operated for 434 days to study the effects of ng-level PFAS on the removal of sulfamethoxazole (SMX). The results showed that 100 ng/L PFAS significantly decreased the removal rate of 1 μg/L SMX from 78.8% to 71.7%. Trace PFAS decreased the abundances of ammonia monooxygenase and nitrite-oxidizing bacteria, thus repressing nitrification co-metabolism process. Meanwhile, trace PFAS inhibited tricarboxylic acid (TCA) cycle by preventing pyruvate from generating acetyl-CoA, reducing energy supply for co-metabolism process. On the other hand, inhibiting TCA cycle led to a redirection of carbon from growth into polysaccharide intercellular adhesin biosynthesis. Trace PFAS also increased glutamate synthase and glutamine synthetase abundances, which promoted biofilm formation and then hindered SMX adsorption by AC. This study provides new insights into the adverse role of PFAS in antibiotic removal by AC filtration.
研究领域:
环境科学
·
微生物学
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DOI
PubMed
高影响因子
Environmental Technology & Innovation
·
2024
·
IF 6.7
Shengming Cheng,Cailin Li,Sisi Liu,Hongyan Zou,Guang-Guo Ying,Chang-Er Chen
To enhance the detection of the escalating presence of per- and poly-fluoroalkyl substances (PFAS) in aquatic environments, the development of innovative sampling techniques becomes imperative. This study focuses on testing a novel passive sampler for in situ sampling of PFAS, employing a ceramic filter tube (CFT) coupled with a hydrogel containing adsorbent-imbedded weak anion exchange resin (WAX) in rod format. The WAX gel rod demonstrated swift binding of the targeted PFAS and potential reusability at least five times. The integrated passive sampler, CFT-WAX, exhibited a linear accumulation pattern for five PFAS in the lab, resulting in a lower diffusive coefficient through the CFT wall than other samplers due to the thicker wall. Notably, variations in pH, ionic strength, and dissolved organic matter did not significantly influence the performance of CFT-WAX. Field deployment in a wastewater treatment plant (WWTP) demonstrated its reasonable performance compared to traditional grab sampling. Though further optimisation in the future is warranted, the findings of this study underscore the efficacy of the developed CFT-WAX passive sampler as a promising tool for in-situ sampling PFAS in aquatic environments.
研究领域:
环境科学
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分析化学
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DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Mark L. Brusseau,Sarah Van Glubt
Fluid-fluid interfacial adsorption has been demonstrated to be an important retention process for per and polyfluoroalkyl substances (PFAS) in porous media with air or non-aqueous phase liquids (NAPLs) present. The objective of this study was to characterize the influence of PFAS molecular structure on air-water interfacial adsorption in electrolyte solutions. Measured and literature-reported surface-tension data sets were aggregated to generate the largest compilation of interfacial adsorption coefficients measured in aqueous solutions comprising environmentally representative ionic strengths. The surface activities and interfacial adsorption coefficients (K i ) exhibited chain length trends, with greater surface activities and larger K i values corresponding to longer chain length. The impact of multiple-component PFAS solutions on the surface activity of a select PFAS was a function of the respective surface activities and concentrations. Quantitative structure-property relationship analysis (QSPR) employing a single molecular descriptor (molar volume) was used successfully to characterize the impact of PFAS molecular structure on air-water interfacial adsorption. A previously reported QSPR model based on PFAS data generated for deionized-water solutions was updated to include more than 60 different PFAS, comprising all head-group types and a wide variety of tail structures. The QSPR model developed for PFAS in electrolyte solution compared favorably to the model developed for deionized water. Additionally, the magnitude of ionic strength for non-zero ionic strength systems was determined to have relatively minimal impact on interfacial adsorption coefficients. The new QSPR model is therefore anticipated to be representative for a wide variety of PFAS and for a wide range of ionic compositions .
研究领域:
环境科学
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化学
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DOI
高影响因子
WATER RESEARCH
·
2022
·
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
Water
·
2025
·Vol. 17
·期 2
·149
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IF 3
Chenyu Chen,Ying Wang,Fei Chen,Xinyue Wang,Qiao Zhang,Jialong Sun,Si Li,Qiang Chen,Fangze Shang,Hui Zhang
Per- and polyfluoroalkyl substances (PFAS) have become a well-known class of anthropogenic pollutants in coastal regions. It is known that PFAS primarily enter the sea from nearshore sources, dry deposition, and wet deposition. However, the contribution of offshore sources to PFAS pollution in the sea remains poorly understood. Our study aims to investigate the occurrence of 74 PFAS across 15 groups in a coastal region of eastern China and to characterize their spatial distribution by focusing on the critical roles of both nearshore and offshore sources. Results revealed that 26 PFAS were detected in the coastal region (i.e., Ou River and Wenzhou Bay), with detection frequencies ranging from 4.3% to 100.0%. Notably, over 10 PFAS were detected for the first time in the region, such as perfluorooctane sulfonamide (FOSA), hexafluoropropylene oxide dimer acid (HFPO-DA), and 6:2 fluorotelomer sulfonic acid (6:2 FTSA), among others. The concentrations of detected PFAS ranged from 0.0018 to 76.31 ng/L, with perfluorooctanoic acid (PFOA) as the dominant congener. Spatial analysis indicated that the nearshore area was more severely polluted compared to the offshore area, with specific hotspots identified near industrialized areas. However, the distribution of certain PFAS, such as perfluorobutane sulfonic acid (PFBS) and perfluoro-3,6-dioxaheptanoic acid (PFDHA), exhibited a contrasting pattern, with higher concentrations observed in the offshore area and near island perimeters. These findings suggest that PFAS pollution in Wenzhou Bay originates from both nearshore and offshore sources, highlighting a complex interplay between nearshore and island-related activities.
研究领域:
环境科学
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海洋学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Yuwen Qi,Huimin Cao,Weijie Pan,Cuiping Wang,Yanna Liang
The negative effects of polyfluoroalkyl substances (PFAS) on the environment and health have recently attracted much attention. This article reviews the influence of soil- and water-derived dissolved organic matter (DOM) on the environmental fate of PFAS. In addition to being co-adsorped with PFAS to increase the adsorption capacity, DOM competes with PFAS for adsorption sites on the surface of the material, thereby reducing the removal rate of PFAS or increasing water solubility, which facilitates desorption of PFAS in the soil. It can quench some active species and inhibit the degradation of PFAS. In contrast, before DOM in water self-degrades, DOM has a greater promoting effect on the degradation of PFAS because DOM can complex with iron, iodine, among others, and act as an electron shuttle to enhance electron transfer . In soil aggregates, DOM can prevent microorganisms from being poisoned by direct exposure to PFAS. In addition, DOM increases the desorption of PFAS in plant root soil, affecting its bioavailability . In general, DOM plays a bidirectional role in adsorption, degradation, and plant uptake of PFAS, which depends on the types and functional groups of DOM. It is necessary to enhance the positive role of DOM in reducing the environmental risks posed by PFAS. In future, attention should be paid to the DOM-induced reduction of PFAS and development of a green and efficient continuous defluorination technology .
研究领域:
环境科学
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生态学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Xiaoyu Zhu,Chen Cheng,Xingao Qin,Ying Wang
Per- and polyfluoroalkyl substances (PFAS) have raised significant concerns; however, their accurate detection in aqueous environments remains a major challenge. In this study, a host-guest molecularly imprinted polymer-based electrochemical sensor with enhanced antifouling properties were developed using β-cyclodextrin embedded with methylene blue (βCD-MB MIP). This sensor demonstrated sensitive and selective quantification of perfluorooctanoic acid (PFOA) in real water samples. The βCD-MB MIP was fabricated by electro-polymerizing βCD and MB in the presence of the target molecule, PFOA, where βCD served as the functional monomer and MB as the signaling probe. The incorporation of βCD endowed the MIP with a stable hydration layer, promoting hydrophilicity and inhibiting fouling, while ensuring effective electron transfer from MB, resulting in significant current responses and outstanding antifouling performance. This sensor exhibits excellent sensing capabilities towards PFOA with a detection limit of 1.57 pg mL −1 , covering a wide concentration range from 4.14 ng mL −1 to 41.4 mg mL −1 . It also displayed high selectivity for PFOA with an imprint factor of 6.5, which is five to seven times higher than that of other perfluorinated analogs. This study introduces an innovative platform for the rapid quantification of PFAS using redox-active MIPs and sets the groundwork for developing integrated sensors for continuous PFAS monitoring in water.
研究领域:
环境科学
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电化学传感器
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材料科学
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DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Jinjing Huang,Kaixing Fu,Zhuoya Fang,Jinming Luo
The effective protocol for treating per- and polyfluoroalkyl substances (PFAS) in water at environmentally relevant concentrations (∼ ng L −1 ) has received unprecedented attention due to the stringent drinking water standards. In order to ensure safe water treatment, sorption using quaternary ammonium functionalized strong-base anion exchange resins (SB-AERs) is considered a viable option for treating PFAS when compared to commercialized activated carbon, as SB-AERs can be in situ regenerated with long-term operation capabilities. However, the harsh conditions required for traditional direct synthesis of SB-AERs (such as prolonged reaction times, complex processes, and environmental pollution caused by the organic reagents used) limit their applications. In this study, we present a novel indirect synthesis method that can effectively pre-functionalizes cellulose for quaternization. This modified cellulose is subsequently loaded onto chloromethylated polystyrene to produce a quaternized cellulose-functionalized polymer resin (QC-CMPS). The process is straightforward to implement, reduces the use of toxic chemicals, and effectively mitigates water safety risks associated with hazardous reagent leaks. As results, the prepared QC-CMPS demonstrates exceptional selective capability for PFAS removal in real environmental water matrices, achieving over 99 % removal efficiency at an initial concentration of 1000 ng L −1 . Additionally, QC-CMPS demonstrates low sensitivity to pH and background ions, effectively removing PFAS from both tap water and lake water with efficiency rates exceeding 95 %. The exhausted QC-CMPS can be readily rejuvenated by rinsing with 1 % NaCl and MeOH (V/V=3/7) mixture, as demonstrated by five successful consecutive cycles. The fixed-bed column test confirmed that ∼ 11,000 bed volumes (∼ 292.70 L) of the feed streams (∼250 ng L −1 ) can be effectively treated with the enrichment factor of 26.42, 25.16, 27.77 and 21.17 for PFOA, PFOS, PFBS, and GenX, respectively, highlighting significant potential for practical applications.
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
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Wei Chen,Mingxiang Liu,Mingmei Ding,Lei Zhang,Shibao Dai
Membrane separation technology has been favorably applied to acquire non-polluting permeate in conditions of contaminative aqueous environment . However, some emerging contaminants with critical impacts on human health and environmental safety such as poly- and perfluoroalkyl (PFAS) compounds composed of various molecular chains are frequently found in water treatment process steps. Especially, short-chain PFASs remain poorly understood in nanofiltration membrane. A thin-film composite membrane with a hyaluronic acid interlayer (TFCi) had been finely tailored to simultaneously gain ameliorative permeate and rejection. Experiments were performed on a small-scale installation to investigate the correlation between operating parameters and short-chain PFASs removal performances. Results showed effectual trace short-chain PFASs rejection during various pressure, temperature, pH, concentration and fouling conditions. Alginate fouling micelles increased PFAS retention and generated a rapid flux decline; nevertheless, the pollutant could be largely removed by washing. Furthermore, molecular dynamics simulations were utilized to reveal the mechanism of the trace short-chain PFASs rejection competence. The hyaluronic acid interlayer was able to suppress the diffusion rate toward the reaction boundary, facilitating the formation of fast water transport pores with good rejection performance for PFAS in polyamides . These results provide important insights into the mechanism of trace hydrophobic contaminants removal system and the interlayer design approach for efficient short-chain PFAS removal using nanofiltration membranes.
研究领域:
环境科学
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材料科学
·
化学工程
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
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IF 11.3
Hao Yu,Peng Zhang,Dongbao Song,Hao Chen,Peng Huang,Srđan D. Rončević,Hongwen Sun
The global concern of per- and polyfluoroalkyl substance (PFAS) contamination has gradually shifted from long- to ultrashort- and short-chain PFAS, but the widely used pyrogenic carbons (PCs) are almost ineffective at removing such hydrophilic pollutants. Herein, a polypyrrole (PPy) nanostructured coating strategy was proposed to modify PCs (PPy@P-BC) for rapid and efficient removal of ultrashort- and short-chain PFAS from water. Static batch tests revealed that the sorption rate constant and sorption capacity of PFAS (C2–C6) on PPy@P-BC are at least 38 times and 5 times greater than those on undecorated PCs and benchmark materials of granular activated carbon, respectively, and their sorption equilibrium time is within 300 s. The outstanding sorption performance of PPy@P-BC is maintained in dynamic column tests (>3120 bed volumes) and different types of real water contaminated by 36 PFAS, including 11 previously identified emerging PFAS (removal >95.3%). PPy@P-BC also exhibited excellent regeneration and reusability. The following dual-drive mechanisms for PFAS removal were identified based on experimental results and density functional theory (DFT) calculations: (i) electrostatic attraction between amino functional groups (especially −NH•+−) on the nanostructured PPy coating and anionic PFAS and (ii) pore filling facilitated by the well-preserved porous structure via construction of the nanostructured coating. Overall, these results provide a promising solution to address the ultrashort- and short-chain PFAS crisis.
研究领域:
环境科学
·
水处理技术
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纳米技术
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吸附过程
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化学工程
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材料科学
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污染控制
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环境化学
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DOI
PubMed
高影响因子
Toxics
·
2024
·Vol. 12
·期 1
·43
·
IF 3.9
Mingguo Peng,Yang Xu,Yao Wu,Xuewen Cai,Weihua Zhang,Lu Zheng,Erdeng Du,Jiajun Fu
Per- and Polyfluoroalkyl Substances (PFAS) bioaccumulate in the human body, presenting potential health risks and cellular toxicity. Their transport mechanisms and interactions with tissues and the circulatory system require further investigation. This study investigates the interaction mechanisms of six PFAS with Human Serum Albumin (HSA) using multi-spectroscopy, DFT and a molecular dynamics approach. Multi-spectral analysis shows that perfluorononanoic acid (PFNA) has the best binding capabilities with HSA. The order of binding constants (298 K) is as follows: “Perfluorononanoic Acid (PFNA, 7.81 × 106L·mol−1) > Perfluoro-2,5-dimethyl-3,6-dioxanonanoic Acid (HFPO-TA, 3.70 × 106L·mol−1) > Perfluorooctanoic Acid (PFOA, 2.27 × 105L·mol−1) > Perfluoro-3,6,9-trioxadecanoic Acid (PFO3DA, 1.59 × 105L·mol−1) > Perfluoroheptanoic Acid (PFHpA, 4.53 × 103L·mol−1) > Dodecafluorosuberic Acid (DFSA, 1.52 × 103L·mol−1)”. Thermodynamic analysis suggests that PFNA and PFO3DA’s interactions with HSA are exothermic, driven primarily by hydrogen bonds or van der Waals interactions. PFHpA, DFSA, PFOA, and HFPO-TA’s interactions with HSA, on the other hand, are endothermic processes primarily driven by hydrophobic interactions. Competitive probe results show that the main HSA–PFAS binding site is in the HSA structure’s subdomain IIA. These findings are also consistent with the findings of molecular docking. Molecular dynamics simulation (MD) analysis further shows that the lowest binding energy (−38.83 kcal/mol) is fund in the HSA–PFNA complex, indicating that PFNA binds more readily with HSA. Energy decomposition analysis also indicates that van der Waals and electrostatic interactions are the main forces for the HSA–PFAS complexes. Correlation analysis reveals that DFT quantum chemical descriptors related to electrostatic distribution and characteristics like ESP and ALIE are more representative in characterizing HSA–PFAS binding. This study sheds light on the interactions between HSA and PFAS. It guides health risk assessments and control strategies against PFAS, serving as a critical starting point for further public health research.Keywords:human serum albumin (HSA);per- and polyfluoroalkyl substances (PFAS);multi-spectroscopy;DFT calculations;molecular docking;molecular dynamics simulation
研究领域:
生物化学
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环境科学
·
毒理学
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DOI
PubMed
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Jun Ma,Yuanyuan Wang,Hang Xu,Mingmei Ding,Li Gao
Per- and polyfluoroalkyl substances (PFAS) are a class of ‘forever chemicals’ that have become a global concern owing to their innate chemical stability on humans and water resources. The separation of PFAS from water resources via membrane technologies are facing huge challenge. High permeance and rejection membrane are required for PFAS. To achieve this goal, herein, we propose an MXene-reinforced interfacial polymerization of negatively charged polyamide (PA) membranes for high rejection of short-chain PFAS. The morphologies and chemical properties were systematically investigated for the fabricated membrane. Attributed to the hydrophilic of MXene , the permeance of MXene-PA membranes increased without sacrificing rejection. Density functional theory (DFT) calculations and various experiments elucidated in detail the underlying mechanism of the interactions between the membrane and PFAS. The enhanced electrostatic interaction and hydrogen bonding leaded to increased PFAS rejection and permeance. Therefore, the MXene-regulated PA membrane effectively solved the trade-off between the selectivity and permeability. This work shows that MXene-regulated interfacial polymerization techniques can be used to tailor the effectiveness of PA nanofiltration membranes to overcome the trade-off phenomenon and pave the way for solving the crisis of short-chain PFAS.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）