ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Kun Wang,Xin Xiao,Zhengzheng Liu,Jing Wang,Xiangyu Zhu,Enhui Wu,Christopher P. Higgins,Baoliang Chen
Though long recognized as synthetic precursors to other poly- and perfluoroalkyl substances (PFASs), most poly- and perfluoroalkyl sulfonyl halides (PASXs) cannot be directly measured and have generally received minimal attention. Inspired by the redox reaction between sulfonyl halide groups and p-toluenethiol in organic chemistry, we developed a novel nontarget analysis strategy for PASXs by intergrating derivatization and specific fragment-based liquid chromatography-high resolution mass spectrometry screening for m/z 82.961 [SO2F–] and m/z 95.934 [S2O2–]. By using this strategy, we discovered 11 PASXs, namely, perfluoroalkyl sulfonyl fluorides (5), polyfluoroalkyl sulfonyl fluorides (2), unsaturated perfluoroalkyl sulfonyl fluoride (1), and perfluoroalkyl sulfonyl chlorides (3) in soil samples collected from an abandoned fluorochemical manufacturing park. These average ∑PASXs concentrations were 1120 μg kg–1 (range: 9.7–9860 μg kg–1), which were very likely to be the key intermediates and undesired byproducts of electrochemical fluorination processes. Spatial variation in the mass ratio of ∑PASXs to ∑PFSAs (range: 0.7–795%) also indicates their different transportation pathways. More importantly, the decline of PASXs and increase of perfluoroalkyl sulfonates (when compared to a prior study at this site) suggest the continued hydrolysis of PASXs and the relatively fast environmental transformation rates in the abandoned fluorochemical park soils. Overall, these findings demonstrated the utility of a novel nontarget analysis strategy, which may change most PASXs from inferred precursors to measured intermediates and further could be adapted for structures, distribution, and transformation studies of PFASXs in other matrices.
研究领域:
环境科学
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分析化学
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化工工程
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DOI
PubMed
高影响因子
Frontiers in Chemistry
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2021
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IF 5.221
Wu Yalin,Bai Huahua,Zhou Qingxiang,Li Shuangying,Tong Yayang,Guo Jinghan,Zhou Boyao,Li Zhi,Zhan Yali,Liu Menghua,Li Yanhui,Qu Tongxu
The health threat from Sudan red dyes has been the subject of much attention in recent years and is crucial to design and establish reliable measurement technologies. In the present study, a new magnetic nanomaterial, polyamidoamine dendrimer-modified magnetic nanoparticles (Gn-MNPs), was synthesized and characterized. The nanomaterials had good adsorption capacity for Sudan dyes from natural waters. G1.5-MNPs possessed excellent adsorption capacity and a linear adsorption relationship over the range from 0.02 to 300 μg L−1 of Sudan dyes with relative coefficients all larger than 0.996. The sensitivity of the proposed method was excellent with detection limits over the range from 1.8 to 5.5 ng L−1 and the precision was less than 3.0%. G1.5-MNPs showed a remarkable application potential for the enrichment of trace environment pollutants in aqueous samples and the developed method based on this nanomaterial could be a robust and reliable alternative tool for routine monitoring of such pollutants.
研究领域:
环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Mei-Xia Ye,Xiao-Jun Luo,Yu Liu,Chu-Hong Zhu,Qun-Jie Feng,Yan-Hong Zeng,Bi-Xian Mai
The effects of sex and pregnancy on the bioaccumulation and tissue distribution of legacy and emerging per- and polyfluoroalkyl substances (PFASs) in Chinese water snakes were investigated. The bioaccumulation factor of PFASs showed a positive correlation with their protein–water partition coefficients (log KPW), and steric hindrance effects were observed when the molecular volume was > 357 Å3. PFAS levels in females were significantly lower than those in males. The chemical composition of pregnant females was significantly different from that of non-pregnant females and males. The maternal transfer efficiencies of perfluorooctane sulfonic acid were higher than those of other PFASs, and a positive correlation between the maternal transfer potential and log KPW was observed for other PFASs. Tissues with high phospholipid content exhibited higher concentrations of ∑PFASs. Numerous physiological changes occurred in maternal organ systems during pregnancy, leading to the re-distribution of chemicals among different tissues. The change in tissue distribution of PFASs that are easily and not-so-easily maternally transferred was in the opposite direction. The extent of compound transfer from the liver to the egg determined tissue re-distribution during pregnancy.
研究领域:
生态毒理学
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环境科学
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动物生理学
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DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Chu-Hong Zhu,Xiao-Jun Luo,Xi Chen,Peng-Peng Chen,Ke Lan Guan,Yan-Hong Zeng,Bi-Xian Mai
Amphibians are sensitive biomonitors of environmental pollutants. However, existing research on per- and polyfluoroalkyl substances (PFASs) between different species of amphibians is limited. In the present study, water, soil, tiger frog ( Hoplobatrachus chinensis ) and forest frog ( Rana chensinensis ) samples were collected from Qingyuan County, South China. The bioaccumulation, tissue distribution, and maternal transfer of 13 PFASs, including 9 perfluoroalkyl carboxylic acids (PFCAs) and 4 perfluoroalkyl sulfonic acids (PFSAs), in frogs were investigated. The ΣPFSA and ΣPFCA concentrations in frog tissues ranged from 0.25 – 36.5 and 0.75 – 226 ng/g wet weight (ww), respectively. The testis in the male frogs had the highest ΣPFCA and ΣPFSA concentrations of all tissues, while the eggs and liver exhibited the highest ΣPFSA and ΣPFCA concentrations in female frogs, respectively. The ΣPFSA and ΣPFCA concentrations were significantly higher in the tiger frogs than in the forest frogs, which could be due to the different exposure scenarios. Male frogs exhibited significantly higher ΣPFCA concentrations than female frogs, which could be due to sex-specific elimination rates for PFASs. Certain tissues exhibited a special affinity for certain PFASs, such as C14 PFCA for the testis; C8 PFSA for the skin, carcass, and eggs; and C10 PFCA for the liver and digestive tracts. Therefore, more in-depth studies are needed on the mechanism of the affinity of a certain tissue for PFASs with specific carbon chain lengths. Approximately 7.4 – 40.4% of PFASs were transferred from the maternal body to eggs, which could underestimate the maternal transfer efficiency of PFASs in frogs because the samples were collected in the early stage of frog breeding.
研究领域:
环境毒理学
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生态毒理学
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环境科学
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野生动物生物学
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生物化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
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2024
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IF 3.8
Xiao-Dong Cheng,Zheng Zhang,Xue-xin Dai,Yun-Ping Li
A 3 μm undecylenic acid-functionalized stationary phase (UAS) was prepared for the separation of nucleosides and nucleobases using per aqueous liquid chromatography (PALC) and hydrophilic interaction liquid chromatography (HILIC). The retention behaviors of nucleosides and nucleobases in PALC and HILIC modes were explored by adjusting parameters such as water content, buffer concentration, pH of the mobile phase and column temperature. The experimental data and separation chromatogram demonstrated that PALC could provide retention comparable to that of HILIC for nucleosides and nucleobases. Comparative studies using diluted adenosine solutions evaluated theoretical plates and peak shape for the same retention factors (between 0.25 and 5.0) in PALC and HILIC. There was no buffer component in the mobile phases used to operate the comparisons. HILIC mode is more efficient for adenosine than PALC mode at low retention factors. It's the exact opposite phenomenon for high retention factors. It is proposed that the mass transfer of adenosine between the UAS, the water-rich layer and the ACN-rich mobile phase in HILIC is relatively slow. Given the significant use of toxic ACN in HILIC, PALC emerges as a safer and more effective alternative for separating nucleosides and nucleobases.
研究领域:
分析化学
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生物化学
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产品关联
DOI
PubMed
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2025
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IF 6.1
Zifang Peng,Shijiao Hou,Qingyun He,Fangcheng Su,Lishun Ren,Congcong Pei,Dan Yin,Yanhao Zhang,Yanjie Huang,Shusheng Zhang,Zongwei Cai
p- Phenylenediamine (PPD) antioxidants and their quinone derivatives (PPDQs), as hot-spot novel contaminants in recent years, have been detected in air fine particulate matters (PM 2.5 ) in multiple regions. However, current research all discussed the pollution of PPDs and PPDQs based on the collected PM 2.5 samples at least in one day (23.5 h). In this work, an innovative study was conducted to investigate their precise daily pollution characteristics and health risks based on high-resolution collected PM 2.5 samples every 1.5 hours in one week in Zhengzhou, a megacity continuously suffers from serious air contamination in central China. The composition patterns and sources of PPDs and PPDQs were discovered and more serious contamination of them were both found at the day-time (07:00–19:00). Almost all daily time intervals with relatively high pollution levels of PPDs and PPDQs were commuting time for majority of workers, which was possibly because of increased rubber tire abrasion induced by huge traffic volume. The highest daily adults’ inhalation risks were also found in 11:30–13:00 and 16:00–17:30 for PPDs and PPDQs in PM 2.5 , respectively. Current study builds the relationship between pollution status of such novel pollutants and human activities, and possibly guides people in central China to take precautions to protect themselves from environmental toxicants at special daily time.
研究领域:
环境科学
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公共卫生
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DOI
PubMed
高影响因子
Green Synthesis and Catalysis
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2020
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IF 0
Bingmei Su,Lian Xu,Xinqi Xu,Lichao Wang,Aipeng Li,Juan Lin,Lidan Ye,Hongwei Yu
As an important building block for the synthesis of angiotensin-converting enzyme inhibitors, ethyl ( R )-2-hydroxyl-4-phenylbutanoate [( R )-HPBE] has attracted increasing attention. The key to industrial biosynthesis of ( R )-HPBE is a biocatalyst that efficiently reduces ethyl 2-oxo-4-phenylbutanoate (OPBE) with high R -enantioselectivity. This paper proposed a strategy for identifying key residues involved in enantioselectivity control based on per-residue free energy decomposition and sequence conservatism analysis. Using this strategy, 4 nonconservative sites with high energy contribution to binding of OPBE were chosen as engineering targets, generating variant Mu27 with 99% conversion and 98% ( R ) ee value at substrate loading of up to 500 mmol/L. MD simulations suggested the higher stability and formation probability of Mu27-OPBE proR prereaction state as key reasons for the excellent R -enantioselectivity of Mu27 towards OPBE. The success in this study provides a viable approach for rational design of alcohol dehydrogenases with high enantioselectivity towards unnatural substrates.
研究领域:
生物化学
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酶工程
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计算生物学
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DOI
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Zenghui Xie,Yuling Hu,Jiana Lin,Gongke Li,Qisheng Zhong
Long-term ingestion or exposure to food contaminated with per- and polyfluoroalkyl substances (PFASs) may cause potential harm to human health. Due to the low contents of PFASs in complex food matrices, it is of great significance to develop adsorbents with excellent properties to enrich PFASs before analysis. Herein, calix[4]arene (CX4) was used as building block to prepare ordered crystalline covalent organic frameworks (COFs). The perfect combination of the host-guest recognition ability of CX4 and the porosity of COFs makes the CX4-COFs selective and high adsorption capacity for linear molecular PFASs (261–1055 mg/g). The adsorption behavior and mechanism were verified by isotherm adsorption experiments and simulation calculations. The CX4-COFs were then used as adsorbents for membrane solid-phase extraction (M-SPE), combined with ultra-high performance liquid chromatography tandem mass spectrometry (UHPLC-MS/MS) to determine PFASs in food. The method has low detection limits (0.11–0.28 ng/kg) and good precision (1.3%−9.8%), and has been successfully applied to the simultaneous enrichment and determination of six PFASs in fish, shrimp and shellfish. Satisfactory recoveries (79.9%−118%) were obtained. This study provides a new strategy for preparing CX4-COFs containing macrocyclic molecules with different morphologies and expands the application of COFs as attractive enrichment media for sample pretreatment .
研究领域:
食品科学
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环境科学
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分析化学
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
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2022
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IF 8.943
Wenkai Liu,Bin Liu,Xin Li
The aim of this study was to investigate the feasibility and fouling mitigation mechanisms of UV/Fe(II) synergistically activated sulfite (S(IV)) (UFS) pretreatment to alleviate membrane fouling caused by HA-enhanced Ca 2+ scaling. After UFS treatment, hydrophobic substances and carboxyl groups structure were destroyed by the in-situ-generated SO•–4, resulted in a significant reduction of hydrophobic substances ratio and carboxyl group concentration. Due to the formation of more electropositive in-situ-generated Fe(III), the complexation between Ca 2+ and carboxyl groups was weakened so that the bulk crystallization size on the membrane surface was greatly reduced. The filter cake enhanced osmotic pressure effect (CEOP) and concentration polarization effect were hence alleviated, as well as the surface roughness . At the microcosmic perspective, as the energy barrier between the membrane and foulants was increased significantly after pretreatment, the anti -foulants adsorption ability of the membrane was enhanced. Correlation analysis showed that the carboxyl concentration and density, HPO ratio, larger particle size (>100 nm) ratio, the Ca 2+ concentration in the scaling layer and energy barrier all had a good correlation with the membrane resistance. This research not only provides an advanced oxidation technology that can effectively alleviate the synergistically-fouling effect of HA and Ca 2+ of nanofiltration process, but also proposes a guidance for the UV/Fe(II) synergistically activated sulfite.
研究领域:
环境科学
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水处理技术
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膜分离技术
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产品关联
DOI
PubMed
高影响因子
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