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JOURNAL OF FOOD SCIENCE · 2019 ·Vol. 84 ·期 5 ·1138-1144 · IF 2.081

Developing and Validating a UPLC-MS Method with a StageTip-Based Extraction for the Biogenic Amines Analysis in Fish

Jingbo Zhang,Jing Hu,Shuai Wang,Xinping Lin,Huipeng Liang,Shengjie Li,Chenxu Yu,Xiuping Dong,Chaofan Ji

To effectively extract biogenic amines (BAs) from complex food matrices is an important issue. In this study, a stop-and-go-extraction tip (StageTip)-based method for simultaneous enrichment of six BAs including histamine, tyramine, putrescine, cadaverine, tryptamine, and β-phenylethylamine in fish samples was developed and optimized. This StageTip-based BAs extraction method required short extraction time, small sample size, and minimal consumption of organic solvents. In addition, an ultrahigh-performance liquid chromatography coupled with triple quadrupole mass spectrometer was used to identify and quantify BAs without derivatization. Target recovery efficiencies of BAs from spiked fish samples ranged from 84% to 110%. Linear regression models were established to determine BAs in the range of 0.4 to 3.0 mg/L ( R 2 > 0.995). Good repeatability was obtained with relative standard deviation of peak areas (1.17 to 5.61%) and retention time (0.09 to 0.20%). High sensitivity was achieved for the detection of six BAs (0.064 to 1.00 ng/L for the limit of detection, 0.10 to 5 ng/L for the limit of quantification). The proposed method had an obvious advantage in the analysis of BAs in complex food matrices such as fish tissues since it could reflect the subtle distribution of BAs from one fish fillet. Practical Application A StageTip-based BAs enrichment combined with UPLC-MS analysis method was developed and optimized, which was low - cost , environmentally friendly, and with good analytical performances. As such, it has the potential to become a powerful tool for the analysis of BAs in different complex food matrices.

研究领域: 食品科学 · 分析化学
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MICROCHIMICA ACTA · 2017 ·Vol. 184 ·期 7 ·2249-2254 · IF 4.58

Visual and photometric determination of histamine using unmodified gold nanoparticles

Huang Conghui,Wang Shuzhan,Zhao Wenfeng,Zong Chenghua,Liang Aiye,Zhang Qingquan,Liu Xiaojun

The authors describe a colorimetric approach for on-site monitoring of histamine based on the use of gold nanoparticles (AuNPs) that have a negatively charged surface due to the presence of adsorbed citrate ions. Histamine has two basic functional groups, an aliphatic amino group and an imidazole ring. Under the experimental conditions, the protonated aliphatic amino group drives the imidazole ring into close proximity to the AuNPs due to electrostatic attraction. This accelerates the replacement of citrate ions by the imidazole ring because of the strong affinity between imidazole and AuNPs. As a consequence, the two groups synergistically induce the aggregation of the AuNPs and trigger a visible color change from red to blue. The minimum visually detectable histamine concentration is 1.81 μM, which is comparable to the limit of detection (LOD) of the electrochemical approaches at a signal-to-noise ratio of 3:1. When using absorbance at 522 nm, the LOD is lowered to 38 nM. The method was applied to the determination of histamine in fish samples. Schematic of the detection scheme: Histamine induces gold nanoparticle aggregation and triggers a visible color change. The minimum visually detectable histamine concentration by bare eye is 1.81 μM. When using absorbance at 522 nm, the LOD is lowered to 38 nM.

研究领域: 分析化学 · 食品科学
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ANALYTICAL CHEMISTRY · 2015 · IF 5.636

Ultrasensitive and Highly Selective Detection of Bioaccumulation of Methyl-Mercury in Fish Samples via Ag0/Hg0 Amalgamation

Li Deng,Yan Li,Xiuping Yan,Jun Xiao,Cheng Ma,Jing Zheng,Shaojun Liu,Ronghua Yang

Methylmercury (CH3Hg+), the common organic source of mercury, is well-known as one of the most toxic compounds that is more toxic than inorganic or elemental mercury. In seabeds, the deposited Hg2+ ions are converted into CH3Hg+ by bacteria, where they are subsequently consumed and bioaccumulated in the tissue of fish, and finally, to enter the human diet, causing severe health problems. Therefore, sensitive and selective detection of bioaccumulation of CH3Hg+ in fish samples is desirable. However, selective assay of CH3Hg+ in the mercury-containing samples has been seriously hampered by the difficulty to distinguish CH3Hg+ from ionic mercury. We report here that metal amalgamation, a natural phenomenon occurring between mercury atoms and certain metal atoms, combining with DNA-protected silver nanoparticles, can be used to detect CH3Hg+ with high sensitivity and superior selectivity over Hg2+ and other heavy metals. In our proposed approach, discrimination between CH3Hg+ and Hg2+ ions was realized by forming Ag/Hg amalgam with a CH3Hg+-specific scaffold. We have found that Ag/Hg amalgam can be formed on a CH3Hg+-specific DNA template between silver atoms and mercury atoms but cannot between silver atoms and CH3Hg+. With a dye-labeled DNA strand, the sensor can detect CH3Hg+ down to the picomolar level, which is >125-fold sensitive over Hg2+. Moreover, the presence of 50-fold Hg2+ and 106-fold other metal ions do not interfere with the CH3Hg+ detection. The results shown herein have important implications for the fast, easy, and selective detection and monitoring of CH3Hg+ in environmental and biological samples.

CAS / MDL: 115-09-3
研究领域: 环境科学 · 分析化学 · 毒理学
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MICROCHIMICA ACTA · 2015 ·Vol. 182 ·期 9 ·1791-1796 · IF 3.741

Molecularly imprinted polymers for extraction of malachite green from fish samples prior to its determination by HPLC

Li Lu,Lin Zheng-zhong,Chen Xiao-mei,Zhang Hong-yuan,Lin Yi-dong,Lai Zhu-zhi,Huang Zhi-yong

Molecularly imprinted polymer (MIP) particles for malachite green (MG) were prepared by emulsion polymerization using methacrylic acid as the functional monomer, ethylene glycol dimethacrylate as the cross-linker, and a combination of Span-80 and Tween-80 as an emulsifier. The MIP particles were characterized by SEM micrographs and FT-IR spectra. Their binding capacity for MG was evaluated based on kinetic and isothermal adsorption experiments and compared to non-imprinted polymer particles. Analytical figures of merit include an adsorption equilibrium time of 15 min, an adsorption capacity of 1.9 mg∙g‾ 1 in acetonitrile-water (20:80), and an imprinting factor of 1.85. The MIP particles were successfully applied to the extraction of MG from fish samples spiked with MG and the other interfering substances prior to its determination of MG by HPLC. Spiked samples gave recoveries of MG that ranged from 86 to 104 %, much higher than that of the other interfering substance. Molecularly imprinted polymer particles for malachite green (MG) were prepared by emulsion polymerization. They show adsorption capacity of 1.9 mg∙g‾¹ with imprinting factor of 1.85, and were successfully applied to the extraction of MG from spiked fish samples.

研究领域: 分析化学 · 环境科学
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FOOD CHEMISTRY · 2025 · IF 9.8

Development of a semi-automated one-step purification method for determination of 63 pesticides in fish samples by HPLC-MS/MS using natural loofah sponge as a novel adsorbent

Yupeng Wen,Wendi Huo,Xinyuan Zhang,Yingchun Mu,Huan Liu,Chaoying Zhang,Lu Qiao,Jincheng Li

In this study, we developed a miniaturized semi-automatic purification method based on pressure-filtration purification for sensitive HPLC-MS/MS monitoring of pesticides in aquatic products. For the first time, loofah sponge was demonstrated and utilized as a novel green, low-cost, and effective one-step purification adsorbent for fish sample. The developed method consisted of two main steps: first, target analytes were extracted from fish samples using an acetonitrile-based QuEChERS extraction method. Subsequently, the extract was automatically purified through a pressure-filtration purification column in a centrifuge, followed by HPLC-MS/MS analysis. Under optimized experimental conditions, the method exhibited excellent linearity, with a range of 1.0 to 50.0 μg/kg and a correlation coefficient > 0.99. The detection and quantification limits were 0.5 and 1–2 μg/kg, respectively. Recoveries at spiked levels of 2.0, 5.0 and 30.0 μg/kg ranged from 69.95 to 104.88 %, with intra-day RSDs ranging from 0.58 to 15.01 % and inter-day RSDs ranging from 0.72 % to 14.32 %.

CAS / MDL: 631-61-8 64-19-7 64-18-6
研究领域: 食品科学 · 环境科学 · 分析化学
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FOOD CHEMISTRY · 2020 · IF 6.306

Histamine detection in fish samples based on indirect competitive ELISA method using iron-cobalt co-doped carbon dots labeled histamine antibody

Yi-Fang Li,Zheng-Zhong Lin,Cheng-Yi Hong,Zhi-Yong Huang

Due to complex matrixes and specific reagent deficiency, the rapid detection of histamine is still a challenge to date. Based on the high peroxidase-like activity of iron-cobalt co-doped carbon dots, an indirect competitive enzyme-linked immunosorbent assay (ic-ELISA) was established for histamine detection using the mimic enzyme labeled with histamine antibody (His-Ab). Through the competitive binding of the labeled His-Ab to solid-phase and sample antigens, histamine content was detected with a linear range of 2.5–150 μg mL −1 . The detection limit based on 3σ/K was 0.50 mg kg −1 , which was much lower than those of commercial His-kit and HPLC methods. The ic-ELISA method was applied to histamine detection in fish samples with the recovery of (103.4 ± 0.5)%, which was in accord with those of commercial His-kit and HPLC methods. The results indicated that the established ic-ELISA method was suitable for rapid detection of histamine in fish samples with high accuracy, sensitivity and stability.

研究领域: 食品科学 · 免疫学 · 分析化学
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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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FOOD CHEMISTRY · 2018 · IF 4.946

Visual determination of malachite green in sea fish samples

Nataliya A. Gavrilenko,Tatyana N. Volgina,Evgeniy V. Pugachev,Mikhail A. Gavrilenko

Polymethylmethacrylate matrix has been developed as an analytical device for visual and spectrophotometric determination of malachite green. Based on the studied effects of different pH levels, temperature, contact time and diverse ions, optimum analysis conditions have been established. For malachite green, the calibration graph was linear in the range of 0.5–30 mg·L −1 in the samples with the detection limit of 1 mg·kg −1 . The proposed simple method makes it possible to determine malachite green visually in the concentration range 8–30 mg·L −1 using a colour scale. The method has been implemented for determination of malachite green in various sea fish samples.

CAS / MDL: 1310-73-2 7647-01-0
研究领域: 分析化学 · 环境科学
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FOOD CHEMISTRY · 2017 · IF 4.529

Speciation analysis of six arsenic species in marketed shellfish: Extraction optimization and health risk assessment

Yuyu Jia,Lin Wang,Li Ma,Zhaoguang Yang

A comparative study between microwave assisted and sonication methods was carried out to extract arsenic (As) species in shellfish samples using different extractants. Six As species including arsenite [As(III)], arsenate [As(V)], monomethylarsonic acid (MMA), dimethylarsinic acid (DMA), arsenobetaine (AsB) and arsenocholine (AsC) were simultaneously separated and determined by the HPLC–ICP-MS method. The microwave assisted method exhibited higher efficiency than sonication, especially using diluted HNO 3 as extractant. By compromising extraction efficiency, pretreatment time and stability of As species, the microwave assisted method using 1% HNO 3 at 100   °C for 1.5   h was selected to extract As from real samples. The proposed method has been applied to extract and determine As species in shellfish samples. The result of correlation analysis indicated that the proportion of AsB in the shellfish samples was decreased with total As concentration increasing due to the biotransformation threshold from inorganic As to AsB.

研究领域: 环境科学 · 分析化学 · 食品安全
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2022 ·Vol. 415 ·期 18 ·4265-4275 · IF 4.478

PEG-modified halloysite as a hydrophilic interaction and cation exchange mixed-mode sorbent for solid-phase extraction of biogenic amines in fish samples

Wang Tingting,Chen Yihui,Hou Chunyan,Qiao Xiaoqiang

A novel type of PEG-modified halloysite was prepared and used as a hydrophilic interaction and cation exchange mixed-mode sorbent for solid-phase extraction of biogenic amines in fish samples. The eluates were analyzed by high-performance liquid chromatography-ultraviolet detection after the derivatization with benzoyl chloride. The developed sorbent was characterized by scanning electron microscopy, infrared spectroscopy, X-ray diffraction, zeta potential analyzer, and thermo-gravimetric analysis. After the optimization of various parameters influencing the extraction efficiency, the PEG-modified halloysite-based SPE method was evaluated. The adsorption capacities of putrescine, spermine, phenethylamine, and histamine were as high as 9.3, 8.5, 5.7, and 5.6 mg g −1 , respectively. Satisfactory reproducibility of sorbent preparation was obtained with within-batch and batch-to-batch relative standard deviations (RSDs) lower than 3.9% and 8.6%, respectively. The biogenic amine spiking recoveries in fish samples ranged from 84.3 to 105.5% with good RSDs lower than 7.8%. Intra-day and inter-day precision, expressed as RSDs, were better than 8.8%. The limits of detection of histamine, putrescine, phenethylamine, and spermine were 9.4, 1.9, 0.5, and 0.9 μg L −1 , respectively. This work provides a new hydrophilic interaction and cation exchange mixed-mode sorbent and is successfully applied to the extraction of trace biogenic amines from fish samples. Graphical Abstract

研究领域: 分析化学 · 食品科学
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES · 2018 · IF 2.441

Determination of semicarbazide in fish by molecularly imprinted stir bar sorptive extraction coupled with high performance liquid chromatography

Tang Tang,Fangdi Wei,Xu Wang,Yujie Ma,Yueyue Song,Yunsu Ma,Quan Song,Guanhong Xu,Yao Cen,Qin Hu

A novel molecularly imprinted stir bar (MI-SB) for sorptive extraction of semicarbazide (SEM) was prepared in present paper. The coating of the stir bar was characterized by scanning electron microscopy, Fourier-transform infrared spectroscopy, dynamic adsorption and static adsorption tests. The saturated adsorption of MI-SB was about 4 times over that of non-imprinted stir bar (NI-SB). The selectivity of MI-SB for SEM was much better than NI-SB. A method to determine SEM was established by coupling MI-SB sorptive extraction with HPLC-UV. The liner range was 1–100   ng/mL for SEM with a correlation coefficient of 0.9985. The limit of detection was about 0.59   ng/mL, which was below the minimum required performance limit of SEM in meat products regulated by European Union. The method was applied to the determination of SEM in fish samples with satisfactory results.

研究领域: 分析化学 · 食品安全
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FOOD CONTROL · 2022 · IF 6.652

Surface-enhanced Raman spectroscopy tandem with derivatized thin-layer chromatography for ultra-sensitive on-site detection of histamine from fish

Sihan Zhang,Qinzhen Fan,Jiaqi Guo,Xianhe Jiao,Xianming Kong,Qian Yu

Sensitive and rapid detection of histamine in fish sample was important for human health. A novel and facile method for on-site detecting histamine in fish was developed by tandem surface-enhanced Raman spectroscopy (SERS) with derivatized thin-layer chromatography. Histamine in tuna was firstly separated by TLC process on a diatomite plate, and then derivatized with fluorescamine (FSA). SERS is used for identification of histamine derivative by a portable Raman spectrometer. The operating conditions were optimized for improving the detection performance. Diatomite plate was suitable for separation and derivatization, 40 times concentrated Au colloid, 1 mM of FSA at pH = 8 were appropriate for the derivatization and SERS detection, and the limit of detection of histamine could achieve 9 ppb. The results indicated that the proposed method not only visualized the histamine on TLC plate but also improve the sensitivity in SERS, that could be employed for the on-site separating and detecting histamine from fish sample.

研究领域: 食品科学 · 分析化学
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