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FOOD CHEMISTRY · 2024 · IF 8.5

Electromembrane extraction of multi-class prohibited/restricted veterinary drugs from food samples – Exploring liquid membrane composition

Junling He,Yong Tang,Chiliang Lin,Shaoyun Peng,Stig Pedersen-Bjergaard,Frederik André Hansen,Chen Zhou

Effective monitoring of veterinary drug residues in food is essential for legislation compliance and food safety, yet remains challenging due to low concentrations and complex matrices. This study introduced a miniaturized 96-well electromembrane extraction (EME) technique for pre-concentration and isolation 80 prohibited/restricted veterinary drugs from honey samples. Three liquid membranes were developed and characterized: V 1 (“V” for veterinary), a mixture of 2-undecanone and 0.5 % 2-nitro-p-cymene, was optimal for extraction of quinolones, tetracyclines, and β -agonists. V2, a mixture of 2-nitrophenyl octyl ether and a deep eutectic solution (formed upon mixing 6-methylcoumarin with thymol in a 1:1 w /w ratio) in a 1:1  v /v ratio, with the addition of 0.5 % di(2-ethylhexyl) phosphate (DEHP), was suitable for macrolides and sulfonamides extraction. V3, a deep eutectic solvent formed upon 1-decanoic acid and camphor in a 1:1 w /w ratio with 1 % DEHP, was suitable for aminoglycosides and β -lactams. Operational parameters were fine-tuned to achieve optimal extraction efficiencies, with recoveries ranging from 20.1–117.5 %, 20.3–91.9 %, and 20.1–118.8 % for V1, V2, and V3, respectively. High precision was observed for compounds with recoveries over 40 % (intra-day: 0.4–27.7 %; inter-day: 2.6–33.0 %), and matrix effects were generally within 80–120 %. This work established a theoretical framework for EME in food analysis, highlighting its potential as a powerful sample pretreatment method for the detection of veterinary drug residues. The results demonstrated the feasibility and advantages of using EME for ensuring food safety and regulatory compliance.

研究领域: 分析化学 · 食品科学 · 环境科学
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Food Chemistry-X · 2023 · IF 6.1

Novel filter-press single-step cleanup approach facilitated rapid screening and accurate quantification of 112 veterinary drugs in aquatic products

Jincheng Li,Ruidong Zhou,Guangxin Yang,Essy Kouadio Fodjo,Tengwang Feng,Huiwu Sun,Dongmei Huang,Cong Kong,Huan Liu

In this study, a novel filter-press cleanup column was developed as a single-step cleanup approach for the rapid screening and quantification of 112 veterinary drugs in fish samples. Fish muscle samples were extracted with acetonitrile and ethyl acetate, sequentially. After concentration and reconstitution, N -propylethylenediamine (PSA) sorbent, packed in filter-press column, allows rapid single-step cleanup operation, while UHPLC-Q-Orbitrap-HRMS provides high-precision mass information in multi-residue screening. Under optimum settings, the detection and quantification limits were validated at 0.5 and 2.0 μg·kg −1 , for all analytes, respectively. The ranges of recoveries were from 35.3 to 138.4%. Most of these target analytes (82%) could be measured with recoveries between 60 and 130%, and intra-day RSDs ranging from 1.9 to 26.1%. This method was further applied to evaluate the residual of veterinary drugs in fish samples from four cities in China, and results demonstrated its practicability for multi-residue monitoring veterinary residues for food safety administration.

CAS / MDL: 64-18-6
研究领域: 分析化学 · 食品科学 · 环境科学
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JOURNAL OF LUMINESCENCE · 2021 · IF 3.599

Red dual-emissive carbon dots for ratiometric sensing of veterinary drugs

He Li,Hong-Gang Ye,Rui Cheng,Jiazhuang Guo,Zhi-Bin Liang,Ge Li,Qing Li,Cai-Feng Wang,Su Chen

Carbon dots have been rapidly developed as a kind of luminescent nanomaterials . However, methods for the synthesis of long-wavelength-emissive carbon dots are still not mature enough. Meanwhile, developing a fast and highly sensitive method to detect residual veterinary drugs in food is particularly significant for food safety. Herein, we report the facile fabrication of red-emissive carbon dots (R-CDs) for ratiometric sensing of veterinary drugs. With use of sorbitol and o -phenylenediamine as precursors, R-CDs was prepared via a one-pot solvothermal approach. The resulting R-CDs show mainly excitation-independent and dual-emissive photoluminescence (PL) located at 597 and 645 nm. Meanwhile, the PL quantum yield (QY) of R-CDs without further surface treatment is 33% under 540 nm excitation. Interestingly, the R-CDs exhibit fast fluorescence response to malachite green oxalate (MG oxalate), 1-aminohydantoin hydrochloride (AHD) and pefloxacin , which are abused widely and retained easily in animals. Ratiometric sensing of these veterinary drugs were successfully performed taking the advantage of dual-emissive PL property; the detection limits of MG oxalate, AHD and pefloxacin were 0.79, 0.25 and 0.85 μM, respectively.

CAS / MDL: 64-17-5 95-54-5 50-70-4
研究领域: 食品安全 · 纳米材料科学 · 分析化学
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Food Bioscience · 2024 · IF 4.8

Application of silanized melamine sponges in matrix purification for rapid analysis of multiple pesticides and veterinary drugs in honey by UPLC-MS/MS

Baocheng Ji,Lanrui Yang,Mengxian Zhang,Peiyu Li,Zhuchen Hou,Jia Lv,Xu Xu,Wenbao Bi,Gaigai Xu,Yanhong Bai

In this study, a modified QuEChERS (Quick, Easy, Cheap, Effective, Rugged, and Safe) method based on two kinds of silanized melamine sponges coupled with ultra-high liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) were developed for the determination of multiple pesticides and veterinary drugs in honey. Quick and convenient matrix separation could be achieved with the developed silanized melamine sponges by simply soaking and squeezing. At three spiked levels, all recoveries of the monitored drugs ranged from 63.6% to 114.8%, with relative standard deviations less than 17.7%. No significant matrix influence was observed with matrix effects within −13.9%∼+15.1% for all monitored drugs. Good linearity with correlation coefficient (R 2 ) ≥0.991 was obtained in the range of 0.08–100 μg kg −1 for most drugs. The limits of detection and quantification ranged from 0.04 to 3.6 μg⋅kg −1 and from 0.08 to 9.8 μg⋅kg −1 , respectively. The results had shown the satisfactory matrix purification performance of silanized melamine sponges and indicated its good application prospect in the multiple determination of pesticides and veterinary drugs in various foods.

研究领域: 食品科学 · 分析化学
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FOOD CHEMISTRY · 2025 · IF 9.8

Monitoring of veterinary drug residues in mutton based on hyperspectral combined with explainable AI: A case study of OFX

Fujia Dong,Zhaoyang Ma,Ying Xu,Yingjie Feng,Yingkun Shi,Hui Li,Fukang Xing,Guangxian Wang,Zhongxiong Zhang,Weiguo Yi,Songlei Wang

Veterinary drug residues in meat seriously harm human health. Rapid and accurate detection of veterinary drug residues is necessary to minimize contamination. Taking ofloxacin (OFX) residues in mutton as an example, the near-infrared hyperspectral imaging combined with explainable AI was used to evaluate the importance of feature wavelengths in the convolutional neural network-stacked sparse auto-encoder (CNN-SSAE) model for chemical properties. Based on this, the qualitative (residue identification-residue level identification) and quantitative detection of OFX residues in mutton was realized. The results showed that the accuracy of CNN-SSAE in identifying residue and residue level of OFX was 100% and 93.65%, respectively, and the correlation coefficients for validation (R 2 P ) in quantitative detection of OFX residue was 0.8980. In addition, SHapley Additive exPlanation (SHAP) values were used to identify feature wavelengths that contribute the most in the CNN-SSAE model, which effectively explained the quality attribute information that spectral and chemical values may improve the predicted results in the model decision process. The reliability of the CNN-SSAE model was evaluated by statistical validation methods (F-test and T-test). Finally, the visualization diagram of OFX content distribution was established. This study provides a method reference for explainability detection of veterinary drug residues.

CAS / MDL: 82419-36-1
研究领域: 食品科学 · 人工智能 · 生物医学
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS · 2024 · IF 4

Rapid determination of residual pefloxacin in mutton based on hyperspectral imaging and data fusion

Hui Li,Fujia Dong,Yu Lv,Zhaoyang Ma,Yue Chen,Sichun Chen,Jinhua Xian,Yingjie Feng,Sijia Liu,Jiarui Cui,Xiuwei Yan,Songlei Wang

Non-destructive detection of veterinary drug residues in meat products is critical for ensuring food safety and human health. The feasibility of using visible near-infrared (Vis-NIR) and near-infrared (NIR) hyperspectral imaging (HSI) system combined with data fusion for the prediction of pefloxacin residues in mutton was investigated in this study. A partial least squares regression optimization model was developed by multivariate data processing methods. The results showed that the low-level fusion (LLF) produced better results with R 2 P = 0.907 and RMSEP = 0.462 as compared to individual data blocks. Furthermore, intermediate-level fusion (ILF) based on iterative retention of informative variables algorithm showed the best results with R 2 P = 0.940 and RMSEP = 0.375. Finally, the visualized distributions of Vis-NIR and NIR based on the optimal model combination were mapped. The results have demonstrated that a combination of HSI with data fusion may be applied to rapidly and non-destructively detect pefloxacin residues in mutton.

CAS / MDL: 70458-92-3
研究领域: 食品科学 · 光谱学 · 生物医学工程
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FOOD CHEMISTRY · 2021 · IF 7.514

Nontargeted screening method for veterinary drugs and their metabolites based on fragmentation characteristics from ultrahigh-performance liquid chromatography-high-resolution mass spectrometry

Wenying Liang,Fujian Zheng,Tiantian Chen,Xiuqiong Zhang,Yueyi Xia,Zaifang Li,Xin Lu,Chunxia Zhao,Guowang Xu

Nontargeted screening of both veterinary drugs and their metabolites is important for comprehensive safety evaluation of animal-derived foods. In this study, a novel nontargeted screening strategy was developed for veterinary drugs and their metabolites based on fragmentation characteristics from ultrahigh-performance liquid chromatography–high-resolution mass spectrometry. First, an in-house database of mass spectra including 3,710 veterinary drugs and their metabolites was constructed. Second, fragmentation characteristics of parent drugs and their metabolites in mass spectrometry were investigated and summarized. Then, a nontargeted screening procedure was established based on fragmentation characteristics to screen unknown parent drugs and their metabolites. Finally, the strategy was applied to 33 egg samples, and four veterinary drugs and three drug metabolites were determined and identified. These results showed that the developed strategy can realize suspect and nontargeted screening of veterinary drugs and their metabolites, and can also be applied to other animal-derived foods.

研究领域: 食品安全 · 分析化学
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FOOD CHEMISTRY · 2024 · IF 8.5

Eco-friendly chitosan microspheres as a novel one-step sorbent for the rapid purification and determination of pesticides and veterinary drug multi-residues in aquatic products with HPLC-MS/MS

Ruidong Zhou,Yupeng Wen,Wendi Huo,Cong Kong,Guangxin Yang,Huan Liu,Chaoying Zhang,Yingchun Mu,Dongmei Huang,Jincheng Li

A modified QuEChERS method was developed to determine multi-class pesticide and veterinary residues in aquatic products. Chitosan microspheres were conveniently synthesized and utilized as the cleanup adsorbent in the QuEChERS procedure, showcasing rapid filtration one-step pretreatment ability for the determination of drug multi-residues in aquatic products. Compared to conventional synthetic sorbents, chitosan microspheres not only have good purification performance, but also have renewable and degradable properties. This novel sorbent worked well in the simultaneous determination of 95 pesticides and veterinary drug residues in aquatic products after being combined with an improved one-step vortex oscillating cleanup method. We achieved recoveries ranging from 64.0% to 115.9% for target drugs in shrimp and fish matrix. The limits of detection and quantification were 0.5–1.0 and 1.0–2.0 μg kg −1 , respectively. Notably, hydrocortisone was detected with considerable frequency and concentration in the tested samples, underscoring the necessity for stringent monitoring of this compound in aquatic products.

CAS / MDL: 9012-76-4 64-18-6
研究领域: 分析化学 · 环境科学 · 食品安全
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

Determination of benzimidazoles in beef by molecularly imprinted boron nitride composite based dispersive solid phase microextraction and ultra performance liquid chromatography

Su Han Wang,Xiao Huan Zang,Shuai Hua Zhang,Jian Ping Wang

The main objective of this study was to synthesize the molecularly imprinted boron nitride material and develop a high efficient method for extraction of the residue of veterinary drug in food sample. During the experiments, the molecularly imprinted microspheres with 2-aminobenzimidazole as the template were polymerize on boron nitride to synthesize a type of new composite. Then it was used as absorbent to develop a dispersive solid phase microextraction method for purification of benzimidazole drugs in beef followed by determination with ultra performance liquid chromatography. This composite could simultaneously recognize 7 benzimidazoles with high absorption capacity (36.23–38.88 μg/mg) and high recovery (92.3%-97.1%), and could be reused for 5 times. This sample extraction method achieved high enrichment factors (21.5–37.9), so the limits of detection for determination of the 7 drugs in beef were in the range of 0.2–0.5 ng/g. This is the first study reporting the use of boron nitride based material for the extraction of residual veterinary drug in food sample.

CAS / MDL: 1321-74-0
研究领域: 分析化学 · 食品科学 · 药物分析
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES · 2016 · IF 2.687

Ion-exchange solid-phase extraction combined with liquid chromatography-tandem mass spectrometry for the determination of veterinary drugs in organic fertilizers

Zhiyong Zhao,Yanmei Zhang,Yanfang Xuan,Wei Song,Wenshuai Si,Zhihui Zhao,Qinxiong Rao

The analysis of veterinary drugs in organic fertilizers is crucial for an assessment of potential risks to soil microbial communities and human health. We develop a robust and sensitive method to quantitatively determine 19 veterinary drugs (amantadine, sulfonamides and fluoroquinolones) in organic fertilizers. The method involved a simple solid-liquid extraction step using the combination of acetonitrile and McIlvaine buffer as extraction solvent, followed by cleanup with a solid-phase extraction cartridge containing polymeric mixed-mode anion-exchange sorbents. Ultra-high performance liquid chromatography-tandem mass spectrometry (UHPLC–MS/MS) was used to separate and detect target analytes. We particularly focused on the optimization of sample clean-up step: different diluents and dilution factors were tested. The developed method was validated in terms of linearity, recovery, precision, sensitivity and specificity. The recoveries of all the drugs ranged from 70.9% to 112.7% at three concentration levels, with the intra-day and inter-day relative standard deviation lower than 15.7%. The limits of quantification were between 1.0 and 10.0   μg/kg for all the drugs. Matrix effect was minimized by matrix-matched calibration curves. The analytical method was successfully applied for the survey of veterinary drugs contamination in 20 compost samples. The results indicated that fluoroquinolones had higher incidence rate and mean concentration levels ranging from 31.9 to 308.7   μg/kg compared with other drugs. We expect the method will provide the basis for risk assessment of veterinary drugs in organic fertilizers.

研究领域: 环境科学 · 分析化学
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FOOD CHEMISTRY · 2024 · IF 8.5

One step cleanup of 160 pesticides and veterinary drugs in aquatic products using melamine-based automatic pressure filtration purification method combined with HPLC-MS/MS

Ruidong Zhou,Cong Kong,Yupeng Wen,Guangxin Yang,Wendi Huo,Chaoying Zhang,Huiwu Sun,Huan Liu,Dongmei Huang,Jincheng Li

A 15-channel pressure filtration purification method was presented for high throughput sample preparation of aquatic products. A cost-effective device was constructed and melamine sponge was selected as the cleanup sorbent. Upon interfacing with HPLC-MS/MS, the analytical procedure demonstrated its suitability for quantifying 160 pesticides and veterinary drug residues in aquatic products such as fish, shrimp, and crab. The method achieved sample recoveries ranging from 61.3 to 124.9 %. The detection limits were established between 0.5 and 1.0 μg/kg, while the quantitation limits were confirmed to be within the range of 1.0–2.0 μg/kg. The method was applied to quantify the pesticide and veterinary drug residues in mostly consumed aquatic products from five coastal provinces in China. The results showed significant differences between different aquatic products in the concentrations of pesticide and veterinary drug residues, implying the necessity of supervision for the accurate determination of pesticides and veterinary drugs.

CAS / MDL: 64-18-6
研究领域: 食品科学 · 分析化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

A Surface-Enhanced Raman Spectroscopy Platform Integrating Dual Signal Enhancement and Machine Learning for Rapid Detection of Veterinary Drug Residues in Meat Products

Yunpeng Wang,Chengming Li,Yang Yang,Chaochao Ma,Xiaojiao Zhao,Jiacheng Li,Lin Wei,Yang Li

The detection and quantification of veterinary drug residues in meat remain a significant challenge due to the complex background interference inherent to the meat matrix, which compromises the stability and accuracy of spectroscopic analysis. This study introduces an advanced label-free surface-enhanced Raman spectroscopy (SERS) platform for the precise identification and quantification of veterinary drugs. By employing a dual enhancement strategy involving sodium borohydride activation and calcium ion–deuterium oxide guidance, this platform achieves the efficient capture and signal amplification of drug molecules on highly active nanoparticles. High-quality SERS spectra were obtained for carprofen, doxycycline hydrochloride, chloramphenicol, and penicillin G sodium salt, enabling accurate classification and interference suppression. In addition, the application of machine learning algorithms, including PCA-LDA, heatmap, and decision tree modeling, allows for accurate differentiation of mixed drug samples. Quantitative analyses in meat samples were achieved through Raman intensity ratios and multivariate curve resolution-alternate least-squares (MCR-ALS) analysis, with results showing high consistency with high-performance liquid chromatography (HPLC) measurements. These findings highlight the potential of this SERS-based platform for accurate and rapid detection of multicomponent veterinary drug residues in complex food matrices.

研究领域: 食品安全 · 分析化学 · 生物信息学
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