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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高影响因子
SENSORS
·
2022
·Vol. 22
·期 5
·1778
·
IF 3.847
Tingting Zhang,Liyun Wu,Junchang Pei,Xuefeng Li,Haowen Li,Frank Inscore
We used surface-enhanced Raman spectroscopy (SERS) for the rapid and sensitive detection and quantification of caffeine in solution. Such a technique incorporated into a portable device is finding wide applications in trace chemical analysis in various fields, including law enforcement, medicine, environmental monitoring, and food quality control. To realize such applications, we are currently developing portable and handheld trace chemical analyzers based on SERS, which are integrated with a sensor embedded with activated gold nanoparticles in a porous glass matrix. In this study, we used this gold SERS-active substrate to measure aqueous solutions of the drug caffeine as a test chemical to benchmark sensor performance by defining sensitivity (lowest measured concentration (LMC) and estimated limit of detection (LOD)), determining concentration dependence and quantification capabilities by constructing calibration curves; by evaluating the effects of pH values of 3, 7, and 11; and by examining the reproducibility of the SERS measurements. The results demonstrate that the SERS sensor is sensitive, with caffeine detected at an LMC of 50 parts per billion (ppb) with an LOD of 0.63 ppb. The results further show that the sensor is very stable and can be used to make reproducible measurements, even under extremely acidic to basic pH conditions. Vibrational assignments of all observed SERS peaks are made and reported for the first time for caffeine on a gold substrate.Keywords:surface-enhanced Raman sensor;SERS;trace chemical detection;Au nanoparticles
研究领域:
分析化学
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环境科学
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材料科学
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WATER RESEARCH
·
2026
·
IF 12.4
Jiameng Liu,Tianchi Cao,Tong Zhang,Thilo Hofmann,Wei Chen
Per- and polyfluoroalkyl substances (PFAS) are widely recognized soil and groundwater contaminants of global concerns. Beyond directly compromising groundwater quality, PFAS may alter the fate and transport of coexisting contaminants, posing additional ecological and human health risks. In this study, we demonstrate that PFAS elevate the risk of colloid-facilitated contaminant transport in groundwater. Specifically, perfluorooctane sulfonate (PFOS), one of the most commonly detected PFAS in groundwater, increases the mobility of three soil colloids (Entisol, Inceptisol, and Mollisol), thereby promoting the transport of decabromodiphenyl ether associated with the colloids. In contrast, perfluorooctanoic acid (PFOA), another commonly detected PFAS, has negligible impact on the co-transport of colloids and contaminants. Using quartz crystal microbalance with dissipation, atomic force microscopy, and molecular dynamics simulations, we show that despite the fact that PFOS and PFOA have very similar molecular structures, PFOS adsorbs more strongly to aquifer materials and forms aggregates on sand grains, thereby creating steric repulsion that inhibits the attachment of soil colloids. Our findings reveal a previously unrecognized risk associated with PFAS, particularly near point sources and spill sites wherein PFAS concentrations are high, and underscore the need for a deeper understanding of the structure–activity relationships governing PFAS interfacial processes.
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JOURNAL OF VINYL & ADDITIVE TECHNOLOGY
·
2021
·Vol. 28
·期 4
·696-705
·
IF 1.993
Zhimin Fu,Zhanhong Yang,Lie Deng,Yao Rong,Jian Wu
The tris(hydroxymethyl)aminomethane (THAM) and its derivative (DHD 2-([1,3-dihydroxypropan-2-ylidene]amino)-2-(hydroxymethyl)propane-1,3-diol) have been used as organic thermal stabilizers for flexible poly(vinyl chloride) (PVC). According to dehydrochlorination and discoloration tests conducted at 180°C, THAM showed to be an excellent organic thermal stabilizer for flexible PVC, not only THAM stabilizer improved the thermal stability of PVC but also maintained the initial color of the PVC. The induction time and the thermal stability time were 52 and 55.5 min, respectively. DHD can also be used as an organic thermal stabilizer for flexible PVC; however, its thermal stabilizing efficiency was not satisfactory, but it has a good synergistic effect with traditional cadmium–zinc soap stabilizers. Besides, the experiments had been performed to investigate pentaerythritol (PER) and THAM, two substances with similar structure, but such a huge difference in thermal stabilizing efficiency for flexible PVC. THAM did improve the thermal stability of PVC, both in initial whiteness and long-term thermal stability. But PER has no thermal stabilizing efficiency for PVC when used alone. At the end of the article, the probable mechanism which can give an explanation for the stabilizing efficiency given by the THAM has been proposed.
研究领域:
材料科学
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高分子化学
·
热工程
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhixiang Xu,Jinrui Xiong,Caiqing Li,Siyuan Hu,Zihui Li,Yitao Ma,Siyuan Li,Bin Huang,Xiaomin Ren,Xuejun Pan
Per/polyfluoroalkyl substances (PFAS) are widespread in aquatic environments and pose significant risks to human health. Their roles in the spread of antibiotic resistance genes through conjugation were investigated in the laboratory. Results showed that PFAS including Perfluorooctanoic acid (PFOA), 6:2Cl-PFAES and 8:2Cl-PFAES at concentrations up to 100 µg/L can significantly enhance the RP4 plasmid-mediated conjugative transfer of antibiotic resistance genes (ARGs) within and across genera as much as 3.38-fold. Perfluorooctanoic acid (PFOA), a representative PFAS, was then selected to investigate the related mechanisms within genera by which PFAS promoted the conjugative transfer of ARGs. The phenotypic experiments demonstrated that PFOA could induce oxidative stress, enhance cell membrane permeability and promote the excretion of extracellular polymeric substances in Escherichia coli , resulting in the elevation of intercellular contact and conjugative transfer of ARGs. Moreover, quantitative polymerase chain reaction revealed that PFOA exposure regulated the expression of conjugation-related genes. In addition, PFOA has also been shown to alter microbial metabolic pathways, including amino acid metabolism, nucleotide metabolism, and membrane translocation, thus altering cellular energy allocation to influence the conjugative transfer of ARGs. This study deepened the understanding of PFAS in promoting the propagation of ARGs, hence improving awareness of the ecological and health risks of PFAS.
研究领域:
环境科学
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微生物学
·
毒理学
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WATER RESEARCH
·
2025
·
IF 12.4
Qinyu Wang,Zhonghao Chen,Xinrui Li,Kemeng Wang,Ke Wang,Yinjuan Chen,Zhugen Yang,Yanyan Zhang,Lei Wang
The phase-out of long chain per- and polyfluoroalkyl substances (PFAS) has accelerated the adoption of alternative emerging PFAS, posing a dual pollution challenge with persistent long-chain residues and their substitutes unclear fate in water treatment. Herein, we develop a scalable and closed-loop strategy producing aminated cellulose xerogel (CNPK) for PFAS removal. CNPK demonstrates excellent mechanical strength (1.96 MPa) and superior PFAS adsorption capacities (3.26 g g −1 HFPO-TrA, 1.82 g g −1 PFOA, 2.14 g g −1 HFPO-DA, 1.27 g g −1 PFHxA, 1.02 g g −1 PFBA and 1.01 g g −1 PFPrA) at pH 3. Its ability to absorb several times its own weight of PFAS is orders of magnitude higher than that of traditional adsorbents. In multi-component systems, the enhanced kinetics and affinity for short/ultra-short chain PFAS facilitate their near-complete removal. This is due to the preferential capture of long chains that provide additional van der Waals (vdW) interactions to accelerate short/ultra-chain adsorption. After five consecutive cycles, CNPK still achieves removal rates of 82%-99% for six types of PFAS and can be dissolved and reproduced. The proof-of-concept filter column achieves over 95% removal for short/ultra-short chain PFAS. The life cycle assessment (LCA) highlights xerogels having lower carbon footprint (161.28-161.71 kg CO 2 eq kg −1 PFAS) compared to most carbon-based adsorbents. Overall, this xerogel strategy tackles the urgent PFAS contamination through high-capacity enrichment under the principles of the circular economy.
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BIOORGANIC & MEDICINAL CHEMISTRY
·
2015
·
IF 2.793
Cheng-Ting Zi,Dan Yang,Fa-Wu Dong,Gen-Tao Li,Yan Li,Zhong-Tao Ding,Jun Zhou,Zi-Hua Jiang,Jiang-Miao Hu
A series of perbutyrylated glycosides of podophyllotoxin and its derivatives were synthesized and evaluated for their antitumor activity in vitro. Most of them exhibit cytotoxic activity against a panel of five human cancer cell lines (HL-60, SMMC-7721, A-549, MCF-7, SW480) using MTT assays . Among the synthesized compounds, epipodophyllotoxin α- d -galactopyranoside 8b , epipodophyllotoxin α- d -arabinopyranoside 8e , and podophyllotoxin β- d -glucopyranoside 11a show the highest potency of anticancer activity with their IC 50 values ranging from 0.14 to 1.69 μM. Structure activity relationship analysis indicates that the type of glycosidic linkage , the configuration at C-4 of the podophyllotoxin scaffold, and the substitution at 4′-position (OH vs OCH 3 ) can all have significant effect on the potency of their anticancer activity. Several compounds are more active than the control drugs Etoposide and Cisplatin , suggesting their potential as anticancer agents for further development.
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ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Xiao-Dong Cheng,Zheng Zhang,Yun-Ping Li
Green chromatography techniques using low-toxic mobile phase are getting increasingly attention in recent years. The core is developing stationary phases that possess adequate retention and separation under the mobile phase of high content water. Using thiol-ene click chemistry, an undecylenic acid-bonded silica stationary phase (UAS) was prepared in a facile manner. Elemental analysis (EA), solid-state 13 C NMR spectroscopy and Fourier transform infrared spectrometry (FT-IR) confirmed the successful preparation of UAS . The synthesized UAS was employed for per aqueous liquid chromatography (PALC), which uses little organic solvent during separation. Due to the hydrophilic carboxy, thioether group and hydrophobic alkyl chains of the UAS, various categories of compounds (including nucleobases , nucleosides , organic acids and basic compounds) with different properties can achieve enhanced separation under the mobile phase of high content water compared with commercial C18 and silica stationary phases. Overall, our present UAS stationary phase shows excellent separation ability toward highly polar compounds and meets the requirements of green chromatography.
研究领域:
分析化学
·
色谱技术
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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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ANALYTICA CHIMICA ACTA
·
2017
·
IF 4.95
Tong Chen,Ling Zhu,Huiyuan Lu,Guangsan Song,Yuanyuan Li,Hongbin Zhou,Ping Li,Wanning Zhu,Hechen Xu,Lijun Shao
The mixed phosphorylated/methacryloyl polysaccharide derivative was prepared and immobilized onto porous silica surface through the radical polymerization . The successful immobilization of polysaccharide on the silica support was confirmed by FT-IR spectra, elemental analysis and transmission electron microscopy (TEM), and so on. The new stationary phase (MCPP-SP) showed both hydrophilic interaction liquid chromatography (HILIC) and per aqueous liquid chromatography (PALC) characteristics. The chromatographic behaviors were evaluated by investigating the effects of water content, column temperature, mobile phase pH and salt concentration, and a typical PALC retention feature of MCPP-SP based column was observed at high percentage of water content. Compared with C18 column, using MCPP-SP column, separation of polar compounds including synthetic pigments and sulfa compounds in the PALC mode was successfully accomplished. The results demonstrated that MCPP-SP column exhibited stronger retention efficiency for various polar compounds. PALC as a green chromatography analytical method was suitable for the replacement of HILIC.
研究领域:
分析化学
·
色谱技术
·
绿色化学
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高影响因子
ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Fanke Tong,Ruitong Zhang,Deyan Li,Han Qu,Xiang Li,Qiang Gao,Delin Qi,Shubo Deng,Wei Wang
Per and polyfluoroalkyl substances (PFAS) have been classified as emerging pollutants requiring global control, and the development of highly efficient adsorbents is a key technological challenge hindering the effective treatment of PFAS. In this study, we prepared a novel fluorinated amino covalent organic framework (COF-FS-NH 2 ) via multimonomer hybrid synthesis and post-synthesis modification. The kinetic data of PFAS adsorption on COF-FS-NH 2 were well fitted using the pseudo-second-order model. Using the Langmuir model, the maximum adsorption capacities of COF-FS-NH 2 for perfluorooctanoic acid (PFOA), perfluoro-2,5-dimethyl-3,6-dioxanonanoic acid (HFPO-TA), perfluoro-2,5-dimethyl-3,6-dioxaheptanoic acid (C7 HFPO-TA), and perfluoro(2-methyl-3-oxahexanoic) acid (GenX) were found to be 0.331, 0.289, 0.319, and 0.210 mmol/g, respectively. PFAS adsorption mainly relied on the electrostatic interaction between the amino group of COF-FS-NH 2 and the anionic group of PFAS as well as the van der Waals forces. Compared with the conventional activated carbon and resin materials, COF-FS-NH 2 exhibited high selectivity and adsorption capacity for PFAS, with high removal percentage (> 80%) for the four PFAS at environmental concentration (10 μg/L). This study demonstrates that COF-FS-NH 2 has great potential for the efficient removal of PFAS from water, providing a new material strategy for practical water remediation.
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ANALYTICAL CHEMISTRY
·
2026
·
IF 7.3
Hang Du,Shuxia Zhang,Dacheng Hao,Sijia Li,Chang Guo,Leyu Wang
Abstract Per- and polyfluoroalkyl substances (PFASs), as a class of persistent organic pollutants, pose a great risk to the ecological environment and human health. The development of rapid and accurate assays for PFASs detection is therefore critically important, yet remains challenging. In this work, we designed a fluorescence sensor system based on single-atom catalysts (SACs) for the detection of PFASs. PFASs could block the atom-specific catalytic sites through hydrophobic–hydrophobic interaction and electrostatic interaction, attenuating the catalytic activity, which leads to the weakening of the colorimetric reaction of 3,3′,5,5′-tetramethylbenzidine (TMB). The resultant colored product (TMBOX) exhibits a substantially reduced fluorescence quenching effect on subsequently added fluorescent carbon dots (CDs). In other words, the bright fluorescence of CDs was well maintained in the presence of a trace amount of PFASs; otherwise, it was significantly quenched in the absence of PFASs. The sensor for PFOA was proposed based on Fe SACs with a detection limit of 1.8 ppb (4.4 nM). Furthermore, when various PFASs interact with a series of SACs, different fluorescence intensity changes could be observed due to the different affinities. Thus, three SACs (Fe, Co, and Cu SACs) were used as the sensing units to construct a fluorescence sensor array. When combined with linear discriminant analysis (LDA) and hierarchical cluster analysis (HCA), qualitative and quantitative detection of six structural PFASs was achieved. This study provides a novel strategy for rapid screening and multidimensional sensing analysis of organic pollutants in real environmental water samples.
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