ACS Nano
·
2025
·
IF 16
Xiaofeng Lu,Dong Zhong,Qi An,Liting Kang,Na Fan,Junjie Cao,Renjie Li,Qianqian Cao,Yudong Zhou,Xiaoyu Du,Shuanghong Yan,Juan Li,Xiaolei Qu,Yuqin Wang
Perfluoroalkyl and polyfluoroalkyl substances (PFASs) make up a large class of emerging chemical pollutants that have caused extensive contamination of global water sources. As the toxicity of PFAS becomes increasingly recognized, there is a growing demand for low-cost and rapid sensors capable of screening water samples for multiple PFAS species. However, most electrochemical and optical sensors can detect only one or two PFASs, despite the high structural diversity of these compounds in aquatic environments. Here, we report a single-molecule nanopore sensor that enables simultaneous detection of nine PFASs in a single measurement. By incorporating a β-cyclodextrin (β-CD) adapter into a mutant α-hemolysin (α-HL) nanopore, translocating PFAS molecules produce distinct current blockades that allow clear discrimination based on carbon chain lengths, hydrogen substitutions, and terminal functional groups. With assistance from a machine learning classifier, an overall identification accuracy of 95.83% is achieved. This strategy allows direct, label-free, and rapid discrimination of multiple PFASs in surface water samples at environmentally relevant concentrations as low as the microgram per liter level, without chemical labeling, separation, or enrichment. The successful demonstration of nanopore sensing in complex real-world matrices highlights its strong potential for practical, field-deployable environmental analysis.
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APPLIED CLAY SCIENCE
·
2025
·
IF 5.8
Ze-Wei Ke,Yu-Xin Liu,Sheng-Jie Wei,Peng Shen,Kun Yang,Yun-Min Chen,Yu-Chao Li
Per - and polyfluoroalkyl substances (PFAS) pose significant environmental and human health concerns due to their extreme persistence and bioaccumulation potential, and widespread contamination. Conventional clay-based barriers, such as geosynthetic clay liners, exhibit limited PFAS containment capabilities owing to their inherently low adsorption capacity. To overcome this challenge, this paper synthesized hexadecyltrimethylammonium-modified bentonite (HDTMA-NaB) as a high-performance adsorbent for engineered containment applications. Comprehensive batch adsorption experiments demonstrated that HDTMA-NaB achieves substantially greater PFAS adsorption capacity compared to pristine bentonite, with adsorption kinetics following a pseudo-second-order model and isotherms were well-described by both Langmuir and Freundlich models. Molecular dynamics simulations unveiled a distinctive “head-attracted, tail-parallel” adsorption configuration, where PFAS molecules align with HDTMA surfactants within montmorillonite interlayers. Chain-length-dependent adsorption patterns were observed, with short-chain PFAS preferentially adsorbing at clay particle edges while long-chain PFAS penetrated deeper into interlayer spaces. Potential of mean force analysis quantitatively verified stronger adsorption affinity for long-chain PFAS, consistent with adsorption experiment observations, through deeper and more numerous energy minima. Thermodynamic analysis indicated that PFAS adsorption was driven by both enthalpic and entropic contributions, with entropy playing the dominant role. The entropic contribution primarily arose from hydrophobic interactions between PFAS fluorinated carbon chains and HDTMA alkyl chains, providing a mechanistic explanation for the observed chain-length-dependent adsorption behavior in adsorption experiments. Meanwhile, the enthalpic contribution arose from electrostatic attraction between PFAS anionic headgroups and HDTMA cationic trimethylammonium groups. These molecular-scale insights provide a fundamental basis for designing high-performance clay-based containment systems for PFAS mitigation.
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ENVIRONMENT INTERNATIONAL
·
2026
·
IF 9.7
Helei Cai,Shihao Luo,Zhengrong Zhou,Feixia Chen,Jiawei Ying,Qiufang Wu,Yize Wu,Shihua Chen,Xinxin Yao,Feiqin Xie,Wenhui Xu,Ke Xu,Renyi Peng
Perfluorooctanoic acid (PFOA) and perfluorobutyric acid (PFBA), as representative long-chain and short-chain per- and polyfluoroalkyl substances (PFAS), are widely distributed in the environment. These compounds can interact with nanoplastics (NPs) to form complex mixed pollutants, posing potential threats to aquatic organisms and human health. The nervous system, characterized by high sensitivity and energy dependence, is particularly vulnerable to such pollutants. However, the mechanisms underlying neurological toxicity induced by co-exposure to PFOA, PFBA, and NPs remain largely unclear. In this study, zebrafish larvae and human neuroblastoma SH-SY5Y cells were employed as model systems to systematically evaluate the effects of PFOA and PFBA, alone or in combination with NPs, on neural development, behavior, cell viability, mitochondrial function, and autophagy. The results demonstrated that NPs exhibited a significantly higher adsorption capacity for PFOA than for PFBA, and that co-exposure exacerbated neurodevelopmental impairments, behavioral abnormalities, and reductions in cell viability. At the molecular level, co-exposure markedly inhibited the PINK1/Parkin-mediated mitophagy pathway, resulting in mitochondrial damage accumulation, disruption of energy metabolism, and blockade of autophagic flux. Through PINK1 overexpression and pharmacological activation experiments, the pivotal role of the PINK1/Parkin-mediated mitophagy pathway in mitigating neurotoxicity was functionally validated. Collectively, this study elucidates the molecular mechanism by which co-exposure to PFOA, PFBA, and NPs induces neurotoxicity via suppression of mitophagy. These findings identify a potential molecular target for the prevention and treatment of PFAS- and NPs-induced neurological injury and provide valuable theoretical and experimental evidence for evaluating the neurotoxic risks of mixed environmental pollutants.
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Journal of Food Measurement and Characterization
·
2026
·
IF 3.3
Yang Jiating,Wang Xinle,Chen Dongye,Wang Ning,Liu Xiaokun,Xu Zhe
Currently, the abuse of antibiotics is becoming increasingly severe, which leads to drug residues in food. Aminoglycoside antibiotics, as a traditional antibiotic, are widely used because of their wide antibacterial spectrum and low cost. Honey, highly valued for its nutritional benefits, is a common animal-derived food product. The current beekeeping practices are primarily characterized by scattered farming by rural households. Beekeepers often indiscriminately overuse aminoglycoside antibiotics to promote the growth of bees and treat larval diseases, resulting in drug residues in honey. However, the complex composition and numerous interfering substances in honey make the efficient extraction and analysis of aminoglycoside antibiotics a persistent challenge. Therefore, this study utilizes magnetic solid-phase extraction technology, employing the prepared magnetic graphene oxide composite material as an adsorbent, in conjunction with high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS), to establish an efficient method for the simultaneous analysis of aminoglycoside antibiotics—kanamycin sulfate (KAM) and tobramycin (TOM)—in honey. We conducted characterization of the materials and investigated both their static and dynamic adsorption properties. Under optimal experimental conditions, this method showed good linear range from 5 to 500 µg·kg − 1 (R 2 ≥ 0.998), the limits of detection were 0.61 µg·kg − 1 (KAM) and 0.75 µg·kg − 1 (TOM), good recoveries of spiked honey samples (94.0%-108.0%), and satisfied repeatability for intra-day and inter-day (KAM, RSD ≤ 8.62%; TOM, RSD ≤ 12.48%). These results indicate that the method has high sensitivity, good stability and can be successfully applied to the enrichment and analysis of KAM and TOM in actual honey samples.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 12.2
Ze-Wei Ke,Yu-Xin Liu,Ying-Le Wan,Yu-Chao Li
The widespread presence of per- and polyfluoroalkyl substances (PFAS) at industrial and military sites threatens subsurface environments and human health. Conventional barrier materials, such as those used in cutoff walls and compacted clay liners, retain PFAS poorly due to their low adsorption affinity. To address this, we engineered a robust functionalized clay (DMOAP-Kao) by covalently grafting dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium onto kaolinite. This grafting strategy ensures superior stability compared to modification by cation exchange. The resulting DMOAP-Kao exhibited a high PFAS adsorption capacity and sustained strong adsorption performance under various aqueous chemistry conditions. Permeation tests further confirmed that incorporating DMOAP-Kao as an amendment into soil-bentonite barrier materials enhances PFAS retardation performance. Molecular dynamics simulations identified three distinct PFAS adsorption morphologies, corresponding to their binding with the outer organosilane shell, the inner organosilane shell, and the kaolinite surface. Free energy calculations revealed a three-stage adsorption process synergistically governed by electrostatic attraction and hydrophobic interactions. The positively charged quaternary ammonium groups of the grafted DMOAP enable long-range electrostatic attraction, effectively “capturing” anionic PFAS species from water and drawing them toward the modified clay surface for subsequent binding. This study establishes a conceptual framework for designing high-affinity clay adsorbents by selecting functionalized organosilanes based on the specific physicochemical properties of target contaminants and grafting them via condensation with the hydroxyl groups on clay surfaces and edges.
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ANALYTICAL CHEMISTRY
·
2026
·Vol. 98
·期 30
·22495-22501
·
IF 7.3
Hou Wenhao,Xing Jiaqi,Zhu Siyu,Ju Yun,He Jing,Qiao Lina,Zhang Hong,Jiang Jie
Microdroplets are highly efficient microreactors, yet
conventional
mass spectrometry typically evaluates their reactivity as an ensemble
average, obscuring the independent catalytic roles of positively and
negatively charged microdroplets. In this study, we developed a microdroplet
separation mass spectrometry method. By separating mixed-charge microdroplet
plumes prior to MS sampling, this approach enables the independent,
online analysis of positively and negatively charged microdroplets.
The performance was validated by combining experiments and simulations.
Application of this methodology to perfluorooctanoic acid (PFOA) degradation
revealed that negatively charged microdroplets exhibit a higher degradation
efficiency than positive counterparts. Mechanistic investigations,
supported by radical trapping and density functional theory, reveal
that negative interfacial charge effectively stabilizes the transition
state, facilitating a hydroxyl radical (•OH)-driven degradation
pathway. This polarity-dependent enhancement proved universal across
varying reaction conditions and other perfluorinated compounds with
diverse chain lengths and terminal functional groups. Moreover, we
rationally modulated the microenvironment via negative voltage application
and Fenton’s reagent supplementation, boosting the PFOA degradation
from approximately 38% to 83%. These findings demonstrate that the
developed separation-MS method is a reliable tool for resolving mixed-charge
microdroplet behaviors and provides insights for reasonably elucidating
and optimizing charge-regulated microdroplet interfacial chemistry.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Lijuan Chang,Xianli Wang,Chengbin Liu,Hang Wen,Zhijie Zhang,Chunxia Yao
Perfluorooctanoic acid (PFOA) has attracted growing attention due to its widespread occurrence and harmful effects on humans. Owing to the strong C F bonds that confer inherent stability on PFOA, achieving efficient degradation via traditional photocatalysts is highly challenging. In this study, a UiO-66-NH 2 photocatalytic-persulfate (UiO-66-NH 2 /PS) integrated system was constructed to achieve high-efficiency PFOA removal, and its underlying mechanism was systematically revealed. A zirconium-based metal–organic framework, UiO-66-NH 2 , with readily tunable porosity was successfully synthesized via a solvothermal route, and its crystal structure, microstructure, and optical absorption behavior were confirmed through comprehensive characterizations. After optimization of the reaction parameters, the UiO-66-NH₂/PS system exhibited excellent PFOA degradation performance, with a markedly enhanced removal efficiency relative to the single UiO-66-NH 2 or persulfate system. The degradation efficiency of UiO-66-NH 2 /PS system in degrading PFOA was affected by ubiquitous anions and humic acid in water. Investigation of degradation pathways revealed that the cooperative action of photogenerated holes and SO₄• − /•OH radicals progressively cleaved the recalcitrant C F bonds, with short-chain perfluorocarboxylic acids (PFCAs) including perfluoroheptanoic acid (PFHpA, C 6 F 13 COOH), perfluorohexanoic acid (PFHxA, C 5 F 11 COOH), perfluoropentanoic acid (PFPeA, C 4 F 9 COOH), and perfluorobutyric acid (PFBA, C 3 F 7 COOH) identified as the main degradation intermediates. This study proposed a high-efficiency, economical and eco-friendly approach for the mineralization of PFOA, and meanwhile shed new light on the mechanism underlying the efficient degradation of PFOA by UiO-66-based photocatalysis combined with persulfate activation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Xiaoya Yuan,Lei Ouyang,Zhou Song,Xuelin Dong,Zhenli Zhu,Qin Shuai,Shenghong Hu
Perfluoroalkyl and polyfluoroalkyl substances (PFAS) present a serious risk to ecosystems and human health, underscoring the need for highly sensitive detection methods. Existing analytical approaches often lack the portability and rapid response required for on-site screening, and conventional surface-enhanced Raman spectroscopy (SERS) substrates exhibit limited affinity toward hydrophobic PFAS molecules. To overcome these limitations, we designed a superhydrophobic nano-Cu modified Ag foam that integrates hydrophobic enrichment with specific metal-carboxylate coordination for effective perfluorooctanoic acid (PFOA) capture and detection. The critical role of Cu 2+ as a bridging site for selective PFOA adsorption was elucidated. This design achieves a remarkably low detection limit of 0.1 μg L −1 for PFOA and enables discrimination between different PFAS categories. Moreover, it maintains excellent SERS activity after two months of storage, effectively addressing the issue of facile oxidation of Cu. The substrate was successfully applied to detect PFOA in various real water samples, demonstrating its potential as a practical and powerful platform for environmental PFAS monitoring.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yuxiang Nie,RuiPeng Lai,Huaicheng Bei,Xianyu Song,Dan Liu,Limeng Yin,Shuangliang Zhao,Honglai Liu
An MD–spectroscopy–XAI framework was developed for PFAS–HS interactions • Ensemble ML accurately predicted PFAS adsorption across 410 structures • Adsorption strength increased while diffusivity decreased with PFAS size • PFAS adsorption energy negatively correlated with molecular weight ( r = −0.72) • SHAP identified MolMR, Kappa3, size, and flexibility as key driver Understanding the adsorption behavior of PFAS on humic substances (HS) is critical for predicting their environmental fate and developing effective remediation strategies. Here, we integrate molecular dynamics (MD) simulations, experimental characterization, and explainable machine learning (XAI) to resolve PFAS interactions with HS at the molecular level. Based on 410 PFAS structures, MD-derived adsorption energies reveal a clear structure-dependent adsorption trend, with a strong negative correlation (Pearson's |r| > 0.72) between molecular weight and adsorption energy magnitude. Machine learning models show robust predictive performance (R 2 > 0.88), enabling accurate adsorption-energy prediction across structurally diverse PFAS. SHAP analysis reveals that PFAS adsorption onto HS is governed by a synergistic interplay of multiple molecular descriptors rather than any single molecular property. Molar refractivity, Kappa3, Number of hydrogen bond acceptors, and molecular weight emerge as the most influential descriptors, highlighting the coupled roles of electronic polarizability, molecular topology, conformational adaptability, and size in controlling adsorption. In contrast, descriptors associated with polarity and hydration tendency are more closely linked to migration behavior. Adsorption experiments and complementary spectroscopic and microscopic characterizations consistently confirmed stronger fluorine accumulation and greater compaction of the HS matrix induced by long-chain PFAS. Overall, the results converge on a unified molecular picture in which larger, more polarizable, and structurally adaptable PFAS are preferentially retained, whereas smaller and more hydration-favored PFAS remain comparatively mobile. This work provides a physics-informed and interpretable framework for predicting PFAS transport in heterogeneous organic environments. Download: Download high-res image (229KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Diwen Xiao,Wenyi Dong,Hongjie Wang,Jiahao Cao,Jie Liu,Yanhui Wang,Yang Wu,Fang Ma,Haifeng Yi
Semiconductor wastewater containing pollutants such as fluoride ions (F − ), per- and polyfluoroalkyl substances (PFAS) and heavy metals has become an increasingly severe issue. Coagulation is a conventional technique for treating semiconductor wastewater. However, existing coagulants face challenges in efficiently removing PFAS, along with issues such as high metal residues, poor settleability and low floc strength. Inspired by the insect-trapping mechanism of Drosera , we synthesized two silane-modified metal-based coagulants, with significantly enhanced performance. Among them, the Drosera -inspired zirconium-based coagulant (DZHC) outperformed the Drosera -inspired aluminum-based coagulant (DAHC) in terms of F − and PFAS removal efficiency, metal residue, settleability, floc size, Zeta potential and floc strength. Mechanistic analyses revealed that F − removal by DZHC occurs via ligand exchange between Zr-OH and F − , whereas DAHC requires initial Al F complexation followed by hydrolysis-polymerization to form coprecipitates. Additional mechanisms including electrostatic interactions, hydrogen bonding and polycondensation also contribute to defluoridation. The removal of copper citrate primarily relies on ligand exchange between metal hydroxyl groups and [Cu-citrate] − , assisted by electrostatic attraction from quaternary ammonium groups. Molecular dynamics simulations and density functional theory (DFT) calculations demonstrated that hydrophobic interactions from C18 chains on the coagulants dominate PFAS removal. In summary, this study provides a novel strategy for simplifying semiconductor wastewater treatment.
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Environmental Science-Water Research & Technology
·
2025
·
IF 3.1
Siyao Zhang,Lulei Zhang,Qinming Zhang,Chun Zhang,Guoqing Zhou,Lumei Gao,Nan Deng,Weidong Wu,Lingjie Meng
Per- and polyfluoroalkyl substances (PFAS) are increasingly recognized as persistent global contaminants with significant health implications. This study offers the first thorough assessment of 19 PFAS across 21 discharge points in Xi'an and Xianyang within the Wei River Basin, utilizing an advanced online solid-phase extraction with liquid chromatography-tandem mass spectrometry (SPE-LC-MS/MS). Notably, we observed distinct seasonal variations in ΣPFAS concentrations: dry water period (January 2024: 141.3-1930.7 ng/L, averaging 360.7 ng/L) > flat water period (May 2024: 7.9-2704.6 ng/L, averaging 245.4 ng/L) > abundant water period (September 2023: 22.0-637.4 ng/L, averaging 145.4 ng/L). Short-chain PFAS, especially perfluorobutanoic acid (PFBA) and Perfluorobutanesulfonic acid (PFBS), were predominant, with over 90% detection frequencies in all water periods. Only one critical finding was the elevated PFOS level at the SW19 discharge point, reaching 1427.0 ng/L during the flat water period—28 times higher than the US EPA's advisory limit for drinking water. Ecological risk assessments indicated SW19 exhibits high risks (RQ > 1) for PFOS during both flat and dry water periods, although the majority of PFAS discharge points are categorized as low or negligible risk. These results emphasize the urgent need for targeted source control in petrochemical and electronics industries, enhanced wastewater treatment technologies for short-chain PFAS, and long-term monitoring programs that account for hydrological changes. This study provides a methodological framework for monitoring multiple PFAS in complex watersheds and supports China's "New Pollutants Governance Action Plan."
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Diwen Xiao,Jiahao Cao,Hongjie Wang,Wenyi Dong,Fang Ma
Fluoride ions (F − ) and per- and polyfluoroalkyl substances (PFAS) in industrial wastewater pose a serious threat to the global environment. Adsorption is the most widely used treatment technology for F − and PFAS in the field of water pollution control. However, existing zirconium-based MOFs face challenges such as the inability to synergistically and efficiently adsorb PFAS, high preparation costs, limited adsorption capacity, and an insufficiently understood adsorption mechanism in multi-component pollution systems. Here, we prepared a novel cerium/zirconium/lanthanum tri-metallic MOF (denoted as Ce/Zr/La-M) by doping low-cost metals and loaded it onto a sponge modified with dimethyloctadecyl[3-(trimethoxysilyl)propyl]ammonium chloride (DTSACL), ultimately obtaining Ce/Zr/La-MSD. The practical adsorption capacity of Ce/Zr/La-MSD for F − is 255 mg/g, which is the highest reported value at similar initial concentrations, while the removal rates for PFAS (C 6 -C 8 ) and PFAS (C 4 ) exceed 96% and 84%, respectively.DFT calculations revealed that doping with La shifted the d-band center of the metals in the MOF closer to the Fermi level, enhancing the material's electron-donating capability. A series of characterization and kinetic simulation results demonstrated that the adsorption mechanism of F − by Ce/Zr/La-MSD involves electrostatic interactions, complexation effects, ion exchange and hydrogen bonding. The primary adsorption sites for PFBA, PFBS, PFOS, and PFHxS were the quaternary ammonium groups containing three carbon atoms, whereas the primary adsorption sites for PFOA and PFHxA were the C 18 chains on DTSACL. In summary, this study provides new insights for the rational design of multifunctional adsorbents and the interpretation of their mechanisms.
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危险品化学品经营许可证（带存储）