ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Yang Yang,Yifan Li,Qinhui Xie,Bo Jiang,Junbo Li,Yunfei Xie,Wei Ji
Biomimetic cytochrome P450 for chemical activation of environmental carcinogens is an efficient in vitro model for evaluating their mutagenicity and ultimately acquiring the metabolites that cannot be easily accessed by conventional routes of organic synthesis. Different kinds of mutagen derived from polyaromatic hydrocarbons (PAHs) by metalloporphyrin/oxidant model systems have been reported, but the underlying molecular mechanisms are poorly understood. Herein, we have for the first time demonstrated an effective surface-enhanced Raman scattering (SERS) protocol to study the dynamics and biomimetic metabolic behaviors of pyrene (Pyr) in the presence of various oxygen donors. Quantitative information on the relative concentration of Pyr and its metabolites in the biomimetic system can be extracted from the SERS spectra. On the basis of our results, we conclude that the oxidative metabolism of Pyr is highly influenced by the types and concentrations of oxygen donors, leading to the formation of 1-hydroxypyrene and dioxygenated products. Besides, the addition of an appropriate amount of an organic solvent can promote the formation of secondary oxidation products. These results offer valuable insights into the dynamics of PAHs metabolism and the regulation of their metabolic pathways in biomimetic activation. In comparison to traditional liquid chromatography–mass spectrometry, the present SERS approach is more suitable for high-throughput evaluation of the metabolic process and kinetics of PAHs. We anticipate that this approach will enable a more general and comprehensive tracking of metabolic dynamics and molecular mechanisms involved in the biomimetic activation of other xenobiotics, such as procarcinogens, promutagens, and drugs.
研究领域:
环境科学
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分析化学
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生物化学
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毒理学
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产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
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2011
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IF 3.65
Xiaofang Shen,Yan Cui,Yuehong Pang,He Qian
1-Hydroxypyrene (1-OHP) is a ubiquitous metabolite of polycyclic aromatic hydrocarbons (PAHs) and has been widely used as a biomarker for evaluation of human exposure to PAHs. In this paper, an electrochemical sensor consisted of graphene oxide nanoribbon (GON)/octa(3-aminopropyl)octasilae quioxane octahydrochloride (OA-POSS) framework films (GON/OA-POSS) modified electrode for pre-concentrating and sensing of 1-OHP was described. The GON/OA-POSS composite films were prepared by hierarchically layer-by-layer assembly via electrostatic interactions. GON, which has higher electrical conductivity than that of graphene oxide, offers residual π-conjugated systems for adsorption of 1-OHP via π–π stacking interaction. Meanwhile, OA-POSS nanocages make the GON layers frameworked to enhance contacting between GON and 1-OHP. When 1-OHP was pre-concentrated on GON/OA-POSS frameworks modified electrode, the response signal and adsorption stability was enhanced significantly. Differential pulse voltammetry was used for direct determination of 1-OHP. The electrochemical sensor calibration curve had a range of 0.1–12.55 μM ( R = 0.995) with a detection limit of 0.04 μM. The results showed that the GON/OA-POSS framework films modified electrode established a new way for simple and sensitive analysis of 1-OHP.
研究领域:
环境科学
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分析化学
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材料科学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF FOOD SCIENCE AND TECHNOLOGY
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2022
·Vol. 57
·期 8
·5376-5387
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IF 3.612
Hai Chi,Yujie Li,Guoqin Liu
Summary In this study, a new electrochemical strategy based on the fabrication of a molecularly imprinted sensor onto a MoS 2 -loaded peanut shell carbon complex with gold nanoparticles (AuNPs) and nitrogen-doped carbon dots (N-CDs) was proposed for the detection of benzo(a)pyrene (BaP). Molecularly imprinted polymer (MIP) films were prepared by cyclic voltammetry (CV) using 2-mercaptobenzimidazole (2-MBI) as a functional monomer in the presence of BaP. The surface morphologies, structural characteristics and electrochemical properties of the obtained MIP/AuNPs/N-CDs/PSBC/MoS 2 /GCE were investigated via scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive spectrometry (EDS), Fourier transform infrared spectrometry (FTIR), X-ray diffraction (XRD), UV–Vis spectrometry, fluorescence spectrometry, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). Under the optimised conditions, the detection range of the electrode towards BaP varied from 5 nM to 20 μM with a detection limit of 1.5 nM. The prepared electrochemical sensor also exhibited good stability, relevant reproducibility and high selectivity. The application of the sensor in the actual analysis of edible oil samples showed promising results, thereby being relevant as a biomimetic sensing platform for the detection of chemical hazards in food and environment.
研究领域:
分析化学
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环境科学
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食品科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Junfei Wu,Qin Zhang,Zhuojun He,Yingli Zhang,Yangli Chen,Hai-Bo Liu,Jing Wang
Tetracycline antibiotics (TCs) are widely distributed in the environment owing to excessive usage and incomplete metabolic breakdown, posing significant risks to ecosystems and human health. Herein, a bifunctional material, Cu-TATB-PCA, was prepared for simultaneous adsorption and detection of TCs. The material was constructed using Cu-MOF as the structural scaffold, with 1-pyrenecarboxylic acid (PCA) grafted via a postsynthetic ligand exchange (PSE) approach. The incorporated PCA moiety functions as both an active site for enhanced adsorption capacity and a fluorescent reporter for sensitive detection. Cu-TATB-PCA demonstrated a remarkable adsorption performance toward TCs, with a maximum adsorption capacity of 520.8 mg/g for oxytetracycline (OTC), 473.9 mg/g for chlortetracycline, and 469.5 mg/g for tetracycline (TC). The high adsorption capacity was mainly attributed to the dominant role of π-π interactions, which worked synergistically with coordination bonds, electrostatic interactions, and hydrogen bonds to collectively contribute to the adsorption process. In addition, Cu-TATB-PCA exhibited a highly sensitive fluorescent response toward TCs due to the mechanism of inner filter effect, which achieved a detection limit of 0.586 μM for TC and 0.776 μM for OTC. The streamlined and efficient material design paradigm paves the way for the development of bifunctional adsorption-detection materials and offers a promising avenue for future research endeavors in this field.
研究领域:
环境化学
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分析化学
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材料科学
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环境污染治理
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药物残留检测
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产品关联
DOI
高影响因子
Materials Science & Engineering C-Materials for Biological Applications
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2013
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IF 2.404
Xuan Zhang,Feng Gao,Xili Cai,Meixia Zheng,Fei Gao,Shulian Jiang,Qingxiang Wang
A stable and uniform organic–inorganic nanocomposite that consists of graphene (GR) and pyrenebutyric acid (PBA) was obtained by ultrasonication, which was characterized by scanning electron microscopy (SEM) and UV–vis absorption spectra. The dispersion was dropped onto a gold electrode surface to obtain GR–PBA modified electrode (GR–PBA/Au). Electrochemical behaviors of the modified electrode were characterized by cyclic voltammetry and electrochemical impedance spectroscopy using [Fe(CN) 6 ] 3 −/4 − as the electroactive probe. A novel DNA biosensor was constructed based on the covalent coupling of amino modified oligonucleotides with the carboxylic group on PBA. By using methylene blue (MB) as a redox-active hybridization indicator, the biosensor was applied to electrochemically detect the complementary sequence, and the results suggested that the peak currents of MB showed a good linear relationship with the logarithm values of target DNA concentrations in the range from 1.0 × 10 − 15 to 5.0 × 10 − 12 M with a detection limit of 3.8 × 10 − 16 M. The selectivity experiment also showed that the biosensor can well distinguish the target DNA from the non-complementary sequences.
研究领域:
分析化学
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生物传感器
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纳米医学
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分子诊断
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电化学
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基因检测
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DOI
高影响因子
CHEMOSPHERE
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2022
·
IF 8.943
Jibao Deng,Hefei Wang,Haisheng Zhan,Chenxi Wu,Yi Huang,Bing Yang,Ahmed Mosa,Wanting Ling
The capability of laccase to oxidate a broad range of polyphenols and aromatic substrates in vitro offers a new technological option for the remediation of polycyclic aromatic hydrocarbon (PAH) pollution with high cytotoxicity. However, laccase application in the remediation of PAH-contaminated sites mainly suffers from a low oxidation rate and high cost because of the difficulty in its recovery. In this study, laccases were immobilized on magnetic Fe 3 O 4 particles coated with chitosan (Fe 3 O 4 @SiO 2 -chitosan) to improve the operational stability and reusability in the treatment of PAH pollution. The enzyme fixation capacity reached 158 mg g −1 , and 79.1% of free laccase activities were reserved under the optimum immobilized condition of 4% glutaraldehyde, 1.0 mg mL −1 laccase, 2 h covalent bonding time, and 6 h fixation time. The degradation efficiencies of anthracene (ANT) and benzo[a]pyrene (B(a)P) by Fe 3 O 4 @SiO 2 -chitosan immobilized laccase in 48 h were 81.9% and 69.2%, respectively. Furthermore, it is very easy to magnetically recover the immobilized laccase from reaction systems and reuse it in a new batch. The relative activities of immobilized laccase were over 50% for the degradation of ANT and B(a)P in three catalytic runs, reaching the goal of substantially reducing cost in practice. According to the results from quantum calculations and mass spectrum analyses, the degradation products of ANT and B(a)P by laccase were anthraquinone and B(a)P-dione, respectively. The findings from this study provide valuable insight in promoting the application of immobilized laccase technology in the remediation of PAH contamination.
研究领域:
环境科学
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生物技术
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化学工程
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Mei Wang,Na Luo,Yanpeng Gao,Guiying Li,Taicheng An
Derivatives of polycyclic aromatic hydrocarbons (PAHs) pose significant threat to environment and human health due to their widespread and potential hazards. However, adverse effects and action mechanisms of PAH derivatives on human health have not been attempted yet. Herein, we chose pyrene and its derivatives (1-hydroxypyrene, 1-nitropyrene, and 1-methylpyrene) to investigate adverse effect mechanism to human lungs using in vitro and in vivo methods. Results showed that pyrene derivatives have higher lung health risks than original pyrene. They can activate AhR, subsequently affecting expression of downstream target genes CYP1A1 and CYP1B1. The binding energies of pyrene and its derivatives ranged from −16.07 to −27.25 kcal/mol by molecular dynamics simulations, implying that pyrene and its derivatives acted as agonists of AhR and increased adverse effects on lungs. Specifically, 1-nitropyrene exhibited stabler binding conformation and stronger AhR expression. In addition, sensitivity of pyrene and its derivatives to AhR activation was attributed to type and number of key amino acids in AhR, that is, pyrene (Leu293), 1-nitropyrene (Cys333, Met348, and Val381), 1-hydroxypyrene (Leu293 and Phe287), and 1-methylpyrene (Met348). In summary, we provide a universal approach for understanding action mechanisms of PAH derivatives on human health, and their adverse effects should be taken seriously.
研究领域:
环境健康
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毒理学
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分子生物学
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药理学
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产品关联
DOI
PubMed
高影响因子
POLYMER
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2021
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IF 4.43
Xinzhu Sun,Danman Guo,Yifeng Cao,Faxu Lin,Huahua Huang,Zhiyong Yang,Yongming Chen,Zhenguo Chi
A series of mechanoresponsive fluorescence composite films were prepared by doping pyrene (Py) and its derivatives including 1-hydroxypyrene (HPY), 1-pyrenemethanol (PYM) and 1-pyrenylboronic acid (PBA) into thermoplastic polyurethane (PU) via physical blending, respectively. The fluorescence property of the composite films was found to be influenced by the polar group of pyrene derivatives and the content of hard segment of PU. The doped PYM showed a stronger trend to aggregate in PU matrixes, relative to other dyes. Contrary to PU/Py and most of previously reported mechanoresponsive materials, the emission intensity of aggregated PYM molecules in both PU25/PYM and PU50/PYM films exhibited a stretching-enhanced-emission feature. When PU25/PYM was stretched up to 500%, the intensity ratio of its dual emission peaks at 490 and 400 nm increased from 2.3 to 5.3. This interesting mechanoresponsive behavior was related to the formation of strong hydrogen bonding between PYM and hard segment of PU matrixes proved by FT-IR spectrograph. Enhancing instead of reducing the emission intensity of dyes through stretching would be remarkable in the field of mechanoresponsive materials.
研究领域:
材料科学
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聚合物化学
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光学材料
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DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
·
IF 4.831
Zhen Liu,Yijie Shi,Chen Li,Wentong Hu,Zhiyi Yao
Polymyxin B (PMB) was an antibiotic with highly effective antibacterial effect but narrow safety interval, and its residues in food had attracted widespread attention. It was important to develop an accurate method for the rapid detection of PMB in animal foods. In this work, we had established a ratiometric sensing system based on the formation of supramolecular assemblies of pyrenyl probes, which were driven by the synergy of noncovalent forces such as multiple-electrostatic and π-π stacking interactions. Compared with the traditional fluorescence detection based on the single wavelength change, the present approach showing two-wavelength fluorescence response could reduce the interference of other factors making the experimental results more accurate. The sensor exhibited high sensitivity and selectivity with a low detection limit (28.3 nM). This method could be used to realize visual detection and had a visual detection limit of 1 μM. As we had learned yet, this was the first ratiometric sensor for PMB detection in aqueous solution. We believed all our preliminary would not only provide a complementary strategy for the detection of PMB, but also develop some new ideas for the construction of sensors for rapid antibiotic detection.
研究领域:
分析化学
·
纳米技术
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生物技术
·
食品安全
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DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2024
·
IF 8.5
Jing Zeng,Wenqin Wu,Xiao Chen,Shenling Wang,Huimin Wu,Ahmed A. El-Kady,Amnart Poapolathep,Alejandro Cifuentes,Elena Ibañez,Peiwu Li,Zhaowei Zhang
As emerging contaminants, microplastics threaten food and environmental safety. Dibutyl phthalate (DBP, released from microplastics) and benzo[ a ]pyrene (BaP, adsorbed on microplastics) coexisted in food and the environment, harming human health, requesting a sensitive and simultaneous testing method to monitor. To address current sensitivity, simultaneousness, and on-site portability challenges during dual targets in complex matrixes, CuCo 2 S 4 /Fe 3 O 4 nanoflower was designed to develop a smartphone-assisted photoelectrochemical point-of-care test (PEC POCT). The carrier transfer mechanism in CuCo 2 S 4 /Fe 3 O 4 was proven via density functional theory calculation. Under optimal conditions, the PEC POCT showed low detection limits of 0.126, and 0.132 pg/mL, wide linearity of 0.001–500, and 0.0005–50 ng/mL for DBP and BaP, respectively. The smartphone-assisted PEC POCT demonstrated satisfied recoveries (80.00%–119.63%) in real samples. Coherent results were recorded by comparing the PEC POCT to GC–MS (DBP) and HPLC (BaP). This novel method provides a practical platform for simultaneous POCT for food safety and environment monitoring.
研究领域:
食品安全
·
环境监测
·
分析化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Huili Zeng,Jingyi Huang,Minghuo Wu,Minjie Hu,Xiaojing Yang,Hao Zhou,Jingjing Zhan,Xuwang Zhang
As a representative polycyclic aromatic hydrocarbon (PAH), pyrene poses a significant threat to the environment and public health due to its persistence and potential toxicity. Extensive research has been conducted on biodegradation of pyrene, highlighting the crucial need to unravel its degradation mechanisms. Coastal and marine sediments are promising sources for discovering microbial candidates capable of degrading pyrene. In this study, three bacterial consortia, designated as BS, YS, and SS, were enriched from sediments collected from the Bohai Sea, Yellow Sea, and Liao River estuarine wetland, respectively. The bacterial consortia BS, YS, and SS demonstrated high pyrene degradation efficiencies, achieving 86.61 %, 80.39 %, and 75.70 % degradation at the concentration of 50 mg/L within 8 days, respectively. High-throughput sequencing of 16S rRNA gene amplicons revealed Pandoraea , Delftia , and Pseudomonas as the dominant populations in bacterial consortia BS, YS, and SS, respectively, with some species potentially being novel pyrene degraders. Further analysis included identifying pyrene degradation metabolites by LC-Q-TOF-MS (high-performance liquid chromatography tandem quadrupole time-of-flight mass spectrometry) and predicting functional genes through PICRUSt (Phylogenetic Investigation of Communities by Reconstruction of Unobserved Stats). Based on these results, the metabolic pathways for pyrene degradation by the bacterial consortia were proposed, which predominantly involved the dioxygenation pathway. Overall, these findings should offer valuable bacterial resources for facilitating the bioremediation of PAH-contaminated environments.
研究领域:
环境微生物学
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生物修复
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海洋生态学
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分子生物学
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产品关联
DOI
高影响因子
FOOD CHEMISTRY
·
2025
·
IF 9.8
Xinlian Zhao,Huihui Zhang,Shu Wang,Xinghe Zhang,Wu Zhong,Xingguo Wang,Pan Gao
Camellia oleifera seed oil (COSO) is highly susceptible to thermo-oxidative degradation due to its high content of unsaturated fatty acids, leading to nutrient loss and carcinogenic benzo[ a ]pyrene (BaP) formation. In this study, we employed a multimodal approach (Fourier transform infrared spectroscopy, FTIR; electron paramagnetic resonance, EPR; oxidation kinetics, α-tocopherol and BaP monitoring) to systematically compare four antioxidants (PG, TBHQ, BHT, VE) at industrially relevant concentrations. Results showed that TBHQ (0.2 g/kg) and PG (0.1 g/kg) optimally preserved α-tocopherols (6.70/4.58 mg/kg) and minimized BaP (1.40/1.46 μg/kg) during 15-day oxidation. FTIR revealed preferential stabilization of C H, cis-C=C, and C O bonds, while EPR confirmed superoxide radical (•O₂ − ) quenching via HAT/SET mechanisms. Kinetic analysis indicated higher activation energies for TBHQ (126.60 kJ/mol) and PG (92.63 kJ/mol), confirming enhanced stability. Mechanistically, TBHQ and PG function via phenolic hydroxyl H-transfer and quinonoid transformation. PG is a low-toxicity alternative to TBHQ for COSO stabilization.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）