JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Xiaojing Tang,Guansheng Liu,Dongliang Wang,Hua Zhong
This study evaluates the methylene blue method for rapid and cost-effective analysis of perfluoroalkyl substances (PFAS). By employing three perfluorosulfonic acids (PFSAs) (perfluorooctanesulfonic acid (PFOS), perfluorohexanesulfonic acid (PFHxS) and perfluorobutanesulfonic acid (PFBS)), three perfluorocarboxylic acids (PFCAs) (perfluorooctanoic acid (PFOA), perfluorohexanoic acid (PFHxA) and perfluorobutanoic acid (PFBA)) and two non-fluorinated compounds (sodium 1-octanesulfonate (SOS) and octanoic acid (OA)), the impact of PFAS structure, specifically polar group type, carbon chain length and fluorine substitution, on the efficacy of the method was assessed. The results showed that PFSAs produced reliable calibration curves (R 2 > 0.99) across all pH levels due to strong dissociation of the -SO 3 H group. In contrast, PFCAs exhibited pH-sensitive performance in that PFOA (C8) showed good linearity (R² > 0.99) at pH ≥ 4, while shorter-chain PFHxA (C6) and PFBA (C4) had poor linearity for all of the pHs tested (1.6–10.0, R² < 0.95). Hydrophobicity-driven partitioning of methylene blue active substance (MBAS) into chloroform was critical, with long-chain PFAS (e.g., PFOS, PFOA) showing stable absorbance despite that the volume of washing solution increased up to 20 mL. The method was ineffective for SOS and OA, which are non-fluorinated analogs of PFOS and PFOA. The modified MB method developed in this study provides high-quality calibration curves for PFSAs and long-chain PFCAs, with a quantification limit as low as 0.03 mg/L, offering a rapid and cost-effective alternative to HPLC-MS for analysis of some PFAS compounds.
研究领域:
环境科学
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化学分析
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毒理学
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Zhaohuan Li,Yamei Hui,Miao Li,Han Li,Xiang Liu
The short-chain perfluoroalkyl and polyfluoroalkyl substances (PFAS) are produced and used in large quantities as substitutes for long-chain PFAS. Short-chain PFAS have strong migration capabilities due to their good water solubility and weak adsorption ability, posing increased risks to global groundwater safety. This study investigated the migration characteristics of short-chain PFAS in saturated porous media, their migration characteristics when coexisting with long-chain PFAS, and competitive effects. As shown in transport experiments, perfluorobutane sulfonate (PFBS) had stronger migration than perfluorobutyric acid (PFBA). Additionally, short-chain PFBA and PFBS showed accelerated migration in the presence of long-chain perfluorooctanoic acid (PFOA). Furthermore, molecular adsorption configurations were established, and adsorption energies were calculated. The absolute value of binding energy order was PFBS (|–3.4 eV|) < PFBA (|–3.91 eV|) < PFOA (|–4.02 eV|), indicating that PFBS had weaker adsorption on SiO 2 compared to PFBA and PFOA. Additionally, when PFOA was present, the binding energies of PFBA and PFBS were − 0.11 and − 0.46 eV, respectively. The difference between R values for PFBA/PFBS and tracer decreased in the PFBA/PFBS–PFOA system (0.152/0.015), compared with PFBA/PFBS pollution (0.232/0.166). The absolute values of binding energies of PFBA/PFBS also decreased, showing that the calculation results aligned with the experimental results. Overall, short-chain PFAS had faster migration rates and were prone to causing groundwater pollution, as inferred from both experiments and theoretical calculations. The results of this study are scientifically significant for better assessing and managing environmental risks of PFAS in soil. Environmental implication Previous studies have focused on adsorption and molecular dynamics simulation of PFAS in soil, microorganisms, and minerals. However, the molecular mechanism of long-chain PFAS on short-chain PFAS has not been addressed in binary pollution. The migration characteristics of short-chain PFAS and long-chain-short-chain PFAS binary pollution were quantitatively studied through breakthrough curve analysis. The adsorption binding energy and charge transfer of PFAS in natural quartz sand were calculated based on density functional theory, revealing molecular adsorption configurations and adsorption mechanisms.
研究领域:
环境科学
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环境化学
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土壤与地下水修复
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分子模拟
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污染迁移动力学
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高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 8
·2229-2239
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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
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材料科学
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高影响因子
Journal of Environmental Sciences
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2024
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IF 5.9
Shi-Ya Peng,Ya-Di Yang,Rong Tian,Naihao Lu
A key characteristic to be elucidated, to address the harmful health risks of environmental perfluorinated alkyl substances (PFAS), is their binding modes to serum albumin, the most abundant protein in blood. Hexafluoropropylene oxide-dimer acid (GenX or HFPO-DA) is a new industrial replacement for the widespread linear long-chain PFAS. However, the detailed interaction of new-generation short-chain PFAS with albumin is still lacking. Herein, the binding characteristics of bovine serum albumin (BSA) to GenX were explored at the molecular and cellular levels. It was found that this branched short-chain GenX could bind to BSA with affinity lower than that of legacy linear long-chain perfluorooctanoic acid (PFOA). Site marker competitive study and molecular docking simulation revealed that GenX interacted with subdomain IIIA to form BSA-GenX complex. Consistent with its weaker affinity to albumin protein, the cytotoxicity of branched short-chain GenX was less susceptible to BSA binding compared with that of the linear long-chain PFOA. In contrast to the significant effects of strong BSA-PFOA interaction, the weak affinity of BSA-GenX binding did not influence the structure of protein and the cytotoxicity of GenX. The detailed characterization and direct comparisons of serum albumin interaction with new generation short-chain GenX will provide a better understanding for the toxicological properties of this new alternative.
研究领域:
生物化学
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毒理学
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环境科学
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PubMed
高影响因子
WATER RESEARCH
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2024
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IF 11.4
Yue Zhi,Xiaoqing Zhao,Ao Shuai,Yonghui Jia,Xinyi Cheng,Shihong Lin,Feng Xiao,Le Han,Hongxiang Chai,Qiang He,Caihong Liu
Nanofiltration (NF) effectively removes per- and polyfluoroalkyl substances (PFAS) from water but struggles with short-chain PFAS (i.e., those containing less than 6 perfluorinated carbons) due to size exclusion inefficiency. In this study, we developed layer-by-layer assembled NF membranes with PDADMAC/PSS terminal bilayers varying in chain lengths, hydrophilicity, and charge, and systematically assessed their removal of 16 representative PFAS species. The mechanisms between long-chain and short-chain PFAS were investigated and optimal strategies for enhancing PFAS selectivity were developed. Results demonstrated that the (PDADMAC/PSS) 3 membrane achieved the highest removal (86.1%-98.1%) for short-chain PFAS, including PFBA-PFHpA (C4-C6), PFBS (C4), PFMOPrA (C3), PFMOBA (C4), and GenX (C5), while effectively removing (>99.9%) long-chain counterparts (≥C7). As feed water pH increased from 3.5 to 9.0, average PFAS rejection rose from 16.6% to 32.0%, revealing more negative charged membrane surface endow stronger electrostatic repulsion, particularly for short-chain anionic PFAS. In addition, we also tested the PFAS removal efficacy of (PDADMAC/PSS) 3 membrane using real sewage plant effluent. Compared to the pristine membrane, the (PDADMAC/PSS) 3 membrane exhibited improved removal for most PFAS, with removal efficiencies ranging from 82.5% for PFOA to 96.7% for PFOS. The most significant improvements were observed in C4 compounds like PFBA and PFBS (increased by 6.0-11.5%). Our study suggests that PFAS removal efficiency by NF highly depends on size exclusion, with short-chain anionic PFAS more likely affected by electrostatic repulsion. Membrane surface manipulation can enhance selectivity, aiding in predicting NF treatment effectiveness for specific PFAS compounds.
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Tao Sun,Fenghua Wang,Yangyang Xie,Xin Liu,Hui Yu,Ming Lv,Yanhui Zhang,Yuxin Xu
Poly- and perfluoroalkyl substances (PFAS) are ubiquitous in the environment and have raised global concern. However, little is known about the microbial response to biochar remediation of PFAS contaminated soil. An indoor experiment was conducted to investigate how microbial community changed when exposed to perfluorooctanoic acid (PFOA) pollution (1 mg/kg) and 3% (w/w) biochar amendment. Results showed that PFOA contamination decreased bacteria diversity and altered microbial composition. Phylum Actinobacteria and genera Gaiella , Blastococcus , Solirubrobacter , and Knoellia were the biomarkers in the PFOA treatments. PFOA pollution decreased the interaction between bacterial genera compared with the control group. PICRUST predictions showed that the C cycling functional genes of coxSML and malZ , N cycling genes of ureC , nirB , nasAB and nxrAB , P cycling genes of pstABC and ugpQ , genes dehH and dhaA encoding dehalogenase were enhanced, phoR and phnP were reduced by PFOA contamination. Biochar remediation restored the bacterial community structure and function to the control level, however, the interaction between bacterial genera was significantly decreased compared with uncontaminated level, illustrated as the reduced number of edges (from 538 to 245), network average degree (from 22 to 10), network density (from 0.477 to 0.217), the clustering coefficients (from 0.727 to 0.534) and the increased average path length (from 1.752 to 2.322). Our study found for the first time the decreased microbial interaction induced by biochar remediation of PFOA contaminated soil and provided a deeper insight into the response of microbial interaction to biochar amendment of recalcitrant compounds-PFAS contaminated soil.
研究领域:
环境科学
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微生物学
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土壤学
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高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2023
·Vol. 120
·期 27
·e2219179120
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IF 11.1
Yuanji Shi,Hongxin Mu,Jiaqian You,Chenglong Han,Huazai Cheng,Jinfeng Wang,Haidong Hu,Hongqiang Ren
The global ecological crisis of perfluoroalkyl and polyfluoroalkyl substances (PFASs) in drinking water has gradually shifted from long-chain to short-chain PFASs; however, the widespread established PFAS adsorption technology cannot cope with the impact of such hydrophilic pollutants given the inherent defects of solid–liquid mass transfer. Herein, we describe a reagent-free and low-cost strategy to reduce the energy state of short-chain PFASs in hydrophobic nanopores by employing an in situ constructed confined water structure in activated carbon (AC). Through direct (driving force) and indirect (assisted slip) effects, the confined water introduced a dual-drive mode in the confined water–encapsulated activated carbon (CW-AC) and completely eliminated the mass transfer barrier (3.27 to 5.66 kcal/mol), which caused the CW-AC to exhibit the highest adsorption capacity for various short-chain PFASs (C-F number: 3-6) among parent AC and other adsorbents reported. Meanwhile, benefiting from the chain length– and functional group–dependent confined water–binding pattern, the affinity of the CW-AC surpassed the traditional hydrophobicity dominance and shifted toward hydrophilic short-chain PFASs that easily escaped treatment. Importantly, the ability of CW-AC functionality to directly transfer to existing adsorption devices was verified, which could treat 21,000 bed volumes of environment-related high-load (~350 ng/L short-chain PFAS each) real drinking water to below the World Health Organization’s standard. Overall, our results provide a green and cost-effective in situ upgrade scheme for existing adsorption devices to address the short-chain PFAS crisis.
研究领域:
环境科学
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材料科学
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化学工程
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 11.3
Yu Xu,Siyuan Feng,Shujia Sun,Yaolong Yan,Wen Hao
Per- and polyfluoroalkyl substances (PFAS) are persistent contaminants that strongly accumulate at air–water interfaces, where they influence fate, transport, and treatment efficiency. However, experimental access to their dynamic interfacial effects remains limited. Here, camphor-driven Marangoni motors were employed as macroscopic probes to translate molecular adsorption of PFAS into measurable propulsion dynamics. Using perfluorooctanoic acid (PFOA) as a model PFAS and sodium dodecyl sulfate (SDS) as a hydrocarbon benchmark, systematic comparisons revealed distinct interfacial signatures. Increasing PFOA concentration induced a progression from continuous propulsion to oscillatory motion and confinement, with 0.4 mM PFOA suppressing the propulsion velocity by approximately 72% relative to the control. In contrast, SDS transitioned from fast propulsion to long-period oscillations and complete arrest, particularly in the presence of Ca²⁺. Quantitative analysis of speed, oscillation period, and peak velocity demonstrated that PFOA exerted more persistent suppression of Marangoni propulsion and retained oscillatory dynamics under ionic perturbation, highlighting its strong and resilient interfacial activity. Localized interactions between PFOA and camphor may modulate interfacial stress renewal in the camphor diffusion zone, supporting sustained oscillatory propulsion compared with SDS. This framework provides a physically transparent model linking amphiphile adsorption to macroscopic interfacial mobility and establishes motion metrics as diagnostic observables for probing amphiphile–interface interactions under non-equilibrium conditions, offering a low-cost platform for mechanistic insight into interfacial processes relevant to water and wastewater treatment.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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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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高影响因子
DESALINATION
·
2026
·
IF 9.9
Xuewu Zhu,Feiyue Ge,Guangjian Bao,Yixuan Li,Hong Peng,Yongshan Ma,Xinwei Kang,Daoji Wu,Jiyong Bian,Tianyu Wang
An alkaline interfacial environment alleviates the self-limiting effect of IP • Moderate NaOH suppresses amine protonation and promotes PA cross-linking. • The optimized membrane forms a dense and uniform polyamide selective layer. • The optimized membrane achieves excellent rejection of PFAS. • The selectivity between organic matter and mineral ions exceeds 200. Nanofiltration (NF) is an important membrane technology for industrial water treatment and advanced drinking water purification. Interfacial polymerization (IP) is widely used to fabricate polyamide (PA) NF membranes because of its tunability and scalability. However, the self-limiting effect in conventional IP, caused by the accumulation of acidic byproducts, constrains PA cross-linking and structural uniformity, limiting the rejection of emerging micropollutants such as per - and polyfluoroalkyl substances (PFAS). Here, the effects of aqueous NaOH concentration on interfacial reaction kinetics, PA microstructure, and membrane separation performance were systematically investigated. Moderate NaOH addition neutralized the HCl byproduct and suppressed piperazine protonation, promoting the formation of a dense and uniform PA network. By incorporating 1 wt% NaOH, the PA-OH-1 membrane achieved an optimized cross-linking density that facilitated 99.2% Na 2 SO 4 rejection and 99.4% natural organic matter removal, yielding an ion/organic selectivity coefficient above 200. Consistent with its dense structure, the membrane maintained high rejection (≥ 96%) for all nine PFAS species tested, with particular efficacy against short-chain perfluorobutanoic acid (PFBA) (99.7% rejection). In contrast, excessive NaOH induced alkaline hydrolysis, disrupted the PA network, altered surface morphology, and significantly deteriorated membrane performance. This work provides mechanistic insight into the structure-performance relationship of PA NF membranes under alkaline interfacial conditions and offers guidance for designing high-performance NF membranes for emerging contaminant removal. Download: Download high-res image (232KB) Download: Download full-size image
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Shi-Jie Jiang,Peng-Xiao Lv,Xing Chen,Ying-Hao Wang,Yan-Hui Chong,Qian Zhang,Jing-Lan Feng,Hai-Ming Guo
Due to their extensive use and widespread distribution, per - and polyfluoroalkyl substances (PFAS) pose significant risks human health and the environment. Development of efficient and environmentally benign adsorbents is urgently needed. In this study, three fluorine-free polymers (labeled QA2P-P , QA4P-P , and QA6P-P ) with cationic binding sites were constructed from quaternized pillar[5]arenes conveniently. These polymers exhibited excellent removal performance for three representative PFAS (perfluorooctanoic acid [PFOA], perfluoropentanoic acid [PFPeA], and ammonium perfluoro-2-propoxypropionate [GenX]). Notably, QA2P-P exhibited >99% removal efficiency for PFOA and GenX. Furthermore, QA2P-P reduced PFOA and GenX from 1 μg L −1 to <4 and < 10 ng L −1 , respectively. The maximum adsorption capacity of QA2P-P was 868.9 mg g −1 for PFOA, 399.6 mg g −1 for GenX, and 452.1 mg g −1 for PFPeA. These results positioned QA2P-P ahead of all previously reported fluorine-free materials and make it comparable to outstanding fluorinated adsorbents. Electrostatic and hydrophobic interactions worked together to enhance the removal capacity. All the polymers were easily synthesized, stable, and readily regenerated. The present research provided valuable guidance for the design of fluorine-free and efficient adsorbents for PFAS.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
·
IF 8.4
Houlong Yang,Muqiao Han,Wentian Zhang,Ming Yi,Lichao Xia,Fangang Meng,Yan Wang,Shanshan Zhao
Two-dimensional (2D) separation membranes have proved their superiorities in addressing global water scarcity and recycling resources. However, current 2D membranes usually suffer from swelling and irregular stacking issues, which result in poor separation performance. Herein, we developed novel mix-dimensional assembled MXene composite membranes with high permeability and selectivity by intercalating 1D carboxylated cellulose nanofibers (CNFs) into 2D lamellar MXene nanosheets. The effects of chain length of CNFs and MXene/CNFs mass ratios on the morphologies, physicochemical properties, and separation performances of composite membranes were systematically investigated. The optimized MXC-3-L membrane exhibited superior rejection to Congo red (CR, >99%) and remarkable separation efficiency of dye/salt. The separation factors for the CR/NaCl and CR/Na 2 SO 4 mixtures were 512.0 and 517.2, respectively. Moreover, the MXC-3-L membrane showed distinct rejections to perfluoroalkyl substances (PFAS) (>95%) with a nearly 8-fold increase of permeance in comparison with the commercial polyamide membrane. The 2D X-ray diffraction analysis verified that the intercalation of 1D CNFs into 2D MXene nanosheets via strong hydrogen bonding can regulate the nanochannel into more stable and regularly stacking lamellar structures, which plays a key role in high permeance and excellent molecular separation efficiency. In addition, 1D CNFs play an essential role as “threading” and “stitching”, shielding the defects between adjacent MXene nanosheets and improving the separation efficiencies. Our work provides new insights into design of defect-free and highly selective 2D materials-based membranes for enhanced wastewater treatment and molecular sieving.
研究领域:
材料科学
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环境科学
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化学工程
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高影响因子
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