查找使用阿拉丁产品的科研文献

Portable Hydrogel Kits Made with Bimetallic Nanozymes for Point-of-Care Testing of Perfluorooctanesulfonate

Xu Xu,Muyao Ma,Xinyue Zhou,Xin Zhao,Daming Feng,Lei Zhang

Perfluorooctanesulfonate (PFOS), an emerging organic contaminant, necessitates robust on-site detection strategies to safeguard human health and ecological balance. This study introduces a novel point-of-care testing (POCT) platform, combining a hydrogel kit with nanozymes and smartphone technology, for the highly sensitive detection of PFOS. The strategy utilizes copper-substituted cobalt-based Prussian blue analogue nanoboxes (CuCo-PBA NBs), which exhibit intricate hollow structures and remarkable peroxidase-like catalytic activity, efficiently catalyzing the oxidation of chromogenic substrates with hydrogen peroxide (H2O2). Density functional theory calculations elucidate the adsorption dynamics of H2O2 on CuCo-PBA NBs, identifying the factors that improve the catalytic efficiency. The colorimetric POCT platform, integrating the hydrogel kit with a smartphone interface, demonstrates practical utility and achieves a detection limit of 1.43 × 10–8 mol L–1 for PFOS. This research not only presents a new nanozyme design for PFOS detection in diverse matrices, such as lake water, whole blood, urine, and milk, but also paves the way for developing a portable and efficient POCT platform for a variety of emerging contaminants.

A mesoporous cationic thorium-organic framework that rapidly traps anionic persistent organic pollutants

Li Yuxiang,Yang Zaixing,Wang Yanlong,Bai Zhuanling,Zheng Tao,Dai Xing,Liu Shengtang,Gui Daxiang,Liu Wei,Chen Meng,Chen Lanhua,Diwu Juan,Zhu Lingyan,Zhou Ruhong,Chai Zhifang,Albrecht-Schmitt Thomas E.,Wang Shuao

Many environmental pollutants inherently exist in their anionic forms and are therefore highly mobile in natural water systems. Cationic framework materials that can capture those pollutants are highly desirable but scarcely reported. Here we present a mesoporous cationic thorium-based MOF (SCU-8) containing channels with a large inner diameter of 2.2 nm and possessing a high surface area of 1360 m 2  g −1 . The anion-exchange properties of SCU-8 were explored with many anions including small oxo anions like ReO 4 − and Cr 2 O 7 2− as well as anionic organic dyes like methyl blue and the persistent organic pollutant, perfluorooctane sulfonate (PFOS). Both fast uptake kinetics and great sorption selectivity toward PFOS are observed. The underlying sorption mechanism was probed using quantum mechanical and molecular dynamics simulations. These computational results reveal that PFOS anions are immobilized in SCU-8 by driving forces including electrostatic interactions, hydrogen bonds, hydrophobic interactions, and van der Waals interactions at different adsorption stages.

Uptake, elimination and biotransformation of N-ethyl perfluorooctane sulfonamide (N-EtFOSA) by the earthworms (Eisenia fetida) after in vivo and in vitro exposure

Shuyan Zhao,Bohui Wang,Lingyan Zhu,Tiankun Liang,Meng Chen,Liping Yang,Jingping Lv,Lifen Liu

N-ethyl perfluorooctane sulfonamide (N-EtFOSA) is commonly known as the active ingredient of sulfluramid. It can be degraded to perfluorooctane sulfonic acid (PFOS) in biota and environment. Earthworms ( Eisenia fetida ) were exposed with N-EtFOSA to examine the bioaccumulation, elimination and metabolism of N-EtFOSA by the earthworms after in vivo and in vitro exposure. N-EtFOSA could be biodegraded in quartz sands to perfluorooctane sulfonamide (FOSA) and PFOS. In the in vivo tests, in addition to parent N-EtFOSA, three metabolites, including perfluorooctane sulfonamide acetate (FOSAA), FOSA and PFOS also accumulated in earthworms as a result of N-EtFOSA biotransformation , with FOSA as the predominant metabolite. The bioaccumulation factor (BAF) and uptake rate coefficient ( k u ) of N-EtFOSA from sand were 20.4 and 2.41·d −1 , respectively. The elimination rate constants ( k e ) decreased in the order FOSAA (0.130·d −1 ) > N-EtFOSA (0.118·d −1 ) > FOSA (0.073·d −1 ) > PFOS (0.051·d −1 ). The biotransformation of N-EtFOSA in earthworm was further confirmed by the in vitro test involving incubation of earthworm homogenates with N-EtFOSA. This work provides evidence on the accumulation and transformation of N-EtFOSA in terrestrial invertebrates and will be helpful to explore the indirect sources of FOSA and PFOS in environmental biota.

Thermal defluorination behaviors of PFOS, PFOA and PFBS during regeneration of activated carbon by molten salt

Shen Zhichao,Zhan Lu,Xu Zhenming

Current study proposes a green regeneration method of activated carbon (AC) laden with Perfluorochemicals (PFCs) from the perspective of environmental safety and resource regeneration. The defluorination efficiencies of AC adsorbed perfluorooctanesulfonate (PFOS), perfluorooctanoic acid (PFOA) and perfluorobutanesulfonate (PFBS) using three molten sodium salts and one molten alkali were compared. Results showed that defluorination efficiencies of molten NaOH for the three PFCs were higher than the other three molten sodium salts at lower temperature. At 700°C, the defluorination efficiencies of PFOS and PFBS using molten NaOH reached to 84.2% and 79.2%, respectively, while the defluorination efficiency of PFOA was 35.3%. In addition, the temperature of molten salt, the holding time and the ratio of salt to carbon were directly proportional to the defluorination efficiency. The low defluorination efficiency of PFOA was due to the low thermal stability of PFOA, which made it difficult to be captured by molten salt. The weight loss range of PFOA was 75°C–125°C, which was much lower than PFOS and PFBS (400°C–500°C). From the perspective of gas production, fluorine-containing gases produced from molten NaOH-treated AC were significantly reduced, which means that environmental risks were significantly reduced. After molten NaOH treatment, the regenerated AC had higher adsorption capacity than that of pre-treated AC.

Fabrication of hydrolytically stable magnetic core-shell aminosilane nanocomposite for the adsorption of PFOS and PFOA

Ding Yu Xing,Yihua Chen,Jiaxin Zhu,Tongzhou Liu

Aminosilane materials, with their low cost and ease of modification, have exhibited great potential for the adsorption of perfluorinated compounds (PFCs) from water. However, this kind of material may be facing two drawbacks during its application: low resistance to hydrolysis and difficulties in separation from the water matrix. This work proposed a strategy of grafting N-(2-aminoethyl) aminopropyltrimethoxysilane (AE-APTMS) on the surface of magnetic γ-Fe 2 O 3 nanoparticles by full utilization of the sorption sites provided by the aminosilane and the magnetism by γ-Fe 2 O 3 . The FTIR and XRD results verified the formation of the magnetic AE-APTMS nanocomposite. The core-shell nanocomposite showed a superparamagnetic property and an isoelectric point at pH = 8.2. Particularly, compared to the aminopropyltriethoxysilane (APTES) nanocomposite, the AE-APTMS nanocomposite exhibited improved hydrolytic stability with 60% less loss of the amine groups during the 48 h adsorption process, as the longer alkyl chain hindered the aminosilane detachment. The AE-APTMS nanocomposite exhibited a rapid adsorption with the removal efficiency of 78% for perfluorooctane sulfonate (PFOS) and 65% for perfluorooctanoate (PFOA) due to the electrostatic interaction and hydrophobic interaction. The regeneration and reuse of the magnetic AE-APTMS nanocomposite were conveniently realized with the removal efficiency higher than 70% for both PFOS and PFOA even after 15 adsorption-desorption cycles. The stable magnetic aminosilane nanocomposite with the ease of separation may provide a new strategy to achieve the economical and effective removal of typical PFCs from water.

The colorimetry and smartphone determination of perfluorooctane sulfonate based on cytidine 5′-monophosphate-capped gold nanoclusters with peroxidase-like activity

Tian-Yuan Guo,Hong-Wei Li,Chun-Xia Zhang,Yuqing Wu

Besides being a luminescent material, cytidine 5′-monophosphate-capped gold nanoclusters (AuNCs@CMP) also show superior peroxidase-like activity which can promote TMB oxidation in the presence of H2O2, causing the solution to turn efficiently from pale to blue. However, the presence of perfluorooctane sulfonate (PFOS) in the above system inhibited TMB oxidation and bluing of the solution, consequently establishing a colorimetric platform of AuNCs/H2O2/TMB for PFOS determination. The results showed that it responded to PFOS over a wide range of 2.0–50 μM, with a limit of detection (LOD) as low as 150 nM. Furthermore, in-depth mechanism investigation revealed that, rather than the active site of the catalyst being occupied by PFOS, such a hypochromatic effect originated from depletion of the reactive oxygen species (ROS) by PFOS degradation, thereby also offering a unique strategy to scavenge the lethal toxicity of PFOS. In addition, the colorimetric response of AuNCs/H2O2/TMB to PFOS was extended to smartphone determination conveniently based on RGB values. Finally, the established platform was applied to PFOS determination both in soil extracts and in tap water with good recovery, which supplies a novel colorimetric platform for visual determination of PFOS in practice. The method has the advantages of being rapid, sensitive and highly selective, which highlight the design and construction of more systems for determination and elimination of lethal pollutants in environmental water.

Molecularly imprinted sensor based on CS/MXene/AuNPs synergy for ultra-trace detection of PFOS in water

Xuanxiu Da,Miao Zhou,Bolu Sun,Haoye Zou,Wenya Wang,Zhen Liu,Hongxia Shi,Jia Zhou,Lin Yang,Yonggang Wang

As a key compound widely used in textile, cosmetic, fire protection, and packaging industries, perfluorooctane sulfonic acid (PFOS) pollutes the environment via the hydrological cycle and enters the human body through the food chain, causing severe toxicity to reproductive, endocrine, and liver systems. Thus, highly sensitive detection of trace PFOS in water is crucial for protecting life and health. Based on this, a molecularly imprinted electrochemical sensor based on a chitosan/MXene/gold nanoparticle (CS/MXene/AuNPs) composite was developed for ultra-trace PFOS detection. MXene, with a high specific surface area and excellent conductivity, served as the substrate, enhancing electron transport via in situ AuNP reduction, while CS improved interfacial stability. Using PFOS as a template and pyrrole as the functional monomer, specific imprinted sites were constructed on the electrode via electropolymerization. Synergistic effects of MXene (conductive framework), AuNPs (catalyzing redox), and CS (immobilizing imprinted layer) boosted sensitivity. Results showed a linear range of 1.0 × 101–1.0 × 109 pg mL−1, detection limit of 7.9 pg mL−1 (S/N = 3), and 98.02–102.04% recovery in spiked samples. This strategy provides a selective and low-cost paradigm for monitoring persistent organic pollutants. Furthermore, it holds significant potential for supporting global environmental safety networks, aiding in pollution-induced disease control, and safeguarding ecological security, human health, and sustainable development.

Effects of Vitamin B12 on the Reductive Transformation of PFOS and F-53B by Nanoscale Zero-Valent Zinc

Perfluorooctane sulfonate (PFOS) and 6:2 chlorinated polyfluoroalkyl ether sulfonate (F-53B) are persistent per- and polyfluoroalkyl substances of concern in aquatic environments. This study compared their anaerobic reductive transformation by nanoscale zero-valent zinc (nZn0), with and without vitamin B12 (VB12). Solutions containing 1 mg/L PFOS or F-53B were treated with nZn0(278 mg/L) and, where indicated, 0.05 mmol/L VB12 (67.8 mg/L) at pH 8.5 and 30 °C for 20 days. After correction for losses observed in reagent-free blanks, PFOS loss was negligible with nZn0alone but reached approximately 34% with nZn0+ VB12, and the corresponding defluorination rate was 33.9%. In contrast, F-53B showed approximately 85% blank-corrected loss by day 6 with either nZn0alone or nZn0+ VB12, while defluorination rates reached 38.0% and 30.7%, respectively, indicating no enhancing benefit of VB12 for F-53B under the studied conditions. Nominal-mass LC-MS/MS features consistent with partially defluorinated and hydrogen-substituted products were observed, and tentative transformation pathways were proposed. These results demonstrated compound-specific effects of VB12 and emphasized the distinction among loss, transformation and defluorination when evaluating PFAS destruction.

Unveiling the neurodevelopmental toxicity of PFOA and PFOS: evidence from integration of in silico and in vitro study

Lili Xin,Rui Guo,Jiawei Sun,Yue Su,Jiahang Cai,Wanzhen Li,Zhongxiao Wan,Jianshu Wang

Perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) are well-known neurodevelopmental toxicants, but the potential molecular mechanism needs to be further clarified. This study aimed to investigate the underlying mechanism of PFOA and PFOS-induced neurodevelopmental toxicity by integrating network toxicology, transcriptomic data from autism spectrum disorder patients and in vitro study. Network toxicology identified 42 core targets that enriched in a total of 105 significant GO entries and 142 KEGG pathways. With the disease-context comparison from the transcriptomic, 10 hub targets and 22 common KEGG pathways were identified. Cellular senescence-associated responses including cellular senescence and cell cycle were proposed as one of the potential mechanisms underlying PFOA and PFOS co-exposure-induced neurodevelopmental toxicity. Molecular docking analysis showed that PFOA and PFOS elicits potential binding capacities with hub targets, with TP53 and MAPK 13 exhibiting lower binding energies with both PFASs, further predicting the potential role of these targets in PFASs-induced neurodevelopmental toxicity. After PFOA and PFOS co-treatment, reduced cell viability, a senescence-like phenotype characterized by cell cycle arrest and increased positive senescence β-galactosidase, upregulation of senescence-associated biomarkers including TP53, p53, p21 and IL-6 as well as the significant up-regulation of MAPK1, MAPK3, MAPK13 and MAPK14 genes were observed in human neuroblastoma SH-SY5Y cells. Thereafter, these findings suggested the multi-target and multi-pathway characteristic of PFOA and PFOS co-exposure-induced neurodevelopmental toxicity with cellular senescence-associated responses as one of the potential molecular mechanisms.

Fe2+-NTA synergized UV254 photolytic defluorination of perfluorooctane sulfonate (PFOS): Enhancing through intramolecular electron density perturbation via electron acquisition

Yihua Chen,Jiaxin Zhu,Hang Ma,Yurong Gu,Tongzhou Liu

Perfluorooctane sulfonate (PFOS) is a persistent organic pollutant posing a risk in environmental persistence, bioaccumulation and biotoxicity. This study was to reach a comprehensive and deeper understanding of PFOS elimination in a UV 254 photolytic treatment with the co-presence of Fe 2+ and nitrilotriacetic acid trisodium salt (NTA). PFOS defluorination was noticeably enhanced in the UV/Fe 2+ -NTA treatment compared with UV/NTA, UV/Fe 2+ and our previously studied UV/Fe 3+ treatments. UV–vis, FTIR, and UPLC/MS-MS results indicated the formation of PFOS-Fe 2+ -NTA complex in PFOS, Fe 2+ and NTA mixture. The transition energy gap of PFOS-Fe 2+ -NTA decreased below the excitation energy supplied by UV 254 irradiation, corresponding with red shift appearing in UV–vis scanning spectrum. This favored intramolecular electron transfer from Fe 2+ -NTA to PFOS under UV 254 irradiation to form electron-accepting PFOS. Molecular electrostatic potential and atom charge distribution analyses suggested electron density rearrangement and perturbation in the perfluorinated carbon chain of electron-accepting PFOS, leading to the decrease in bond dissociation energies. Intermediate products detection suggested the parallel defluorination pathways of PFOS desulfonation, middle carbon chain scission and direct C-F cleavage. NTA exhibited crucial functions in the UV/Fe 2+ -NTA treatment by holding Fe 2+ /Fe 3+ in soluble form as a chelant and favoring water activation to generate hydrated electrons (e aq − ) under UV irradiation as a photosensitizer. Fe 2+ acting as the conduit for electron transfer and the bridge of PFOS anion and NTA was thought functioning best at 200 µM in this study. The degree of UV/Fe 2+ -NTA -synergized PFOS defluorination also depended on e aq − yield and UV 254 photon flux. The structure dependence on the electron transfer process of PFOS and PFOA was explored incorporating molecular structure descriptors. Because of possessing greater potential to acquire electrons or less likeliness to donate its electrons than PFOA, PFOS exhibited faster defluorination kinetics in the published “reduction treatments” than “oxidation” ones. Whereas, PFOA defluorination kinetics were at similar level in both “reduction” and “oxidation” treatments.

Acute exposure to environmentally relevant concentrations of Chinese PFOS alternative F-53B induces oxidative stress in early developing zebrafish

Yongming Wu,Jing Huang,Mi Deng,Yuanxiang Jin,Huilin Yang,Yu Liu,Qinyan Cao,Jan A. Mennigen,Wenqing Tu

6:2 chlorinated polyfluorinated ether sulfonate (F-53B), a Chinese PFOS alternative, has recently been identified in the aquatic environment at concentrations similar to or higher than perfluorooctane sulfonate (PFOS). Although previous studies have shown that F-53B can trigger oxidative stress in fish, the underlying molecular mechanism is still largely unknown. In this study, zebrafish embryos were exposed to various concentrations of F-53B (0, 0.5, 20 and 200 μg/L) for 5 d to investigate oxidative stress responses and possible molecular mechanisms of action. Our results showed that F-53B accumulated in a concentration-dependent manner in zebrafish larvae. The contents of malondialdehyde (MDA) and reduced glutathione (GSH), as well as the activities, mRNA and protein levels of most of antioxidant enzyme genes involved in the phosphatidylinositol 3-kinase (PI3K)/Akt/Nrf2-ARE pathway were significantly reduced. Further in silico study indicated that F-53B binds tightly to PI3K, which may be related to the inhibition of Nrf2-regulated antioxidant functions by F-53B as a PI3K inhibitor. Combining in vivo and in silico studies, we elucidated the effects of F-53B on antioxidant system of zebrafish through the PI3K/Akt/Nrf2-ARE pathway, which increases our understanding of the molecular mechanism of F-53B on antioxidant responses in fish.

Molecularly imprinted resin modified with ionic liquid for dispersive filter extraction and determination of perfluoroalkyl acids in eggs

Yanke Lu,Hongyuan Yan,Pengfei Li,Yehong Han,Shigang Shen

Perfluoroalkyl acids (PFAAs) are emerging pollutants that endangers food safety. Developing methods for the selective determination of trace PFAAs in complex samples remains challenging. Herein, an ionic liquid modified porous imprinted phenolic resin-dispersive filter extraction-liquid chromatography-tandem mass spectrometry (IL-PIPR−DFE−LC-MS/MS) method was developed for the determination of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) in eggs. The new IL-PIPR adsorbent was prepared at room temperature , which avoids the disorder and instability of the template at high temperatures. The imprinting factor of IL-PIPR for PFOA and PFOS exceeded 7.3. DFE, combined with IL-PIPR (15 mg), was used to extract PFOA and PFOS from eggs within 15 min. The established method exhibits low limits of detection (0.01–0.02 ng/g) and high recoveries (84.7%–104.7%), which surpass those of previously reported methods. This work offers a new approach to explore advanced imprinted adsorbents for PFAAs, efficient sample pretreatment technique, and analytical method for pollutants in foods.