Citation: WEI Dan, GUO Ming, ZHANG Ju. Determination of 10 fluoroquinolones residues in aquatic products by accelerated solvent extraction, magnetic solid-phase extraction, and high-performance liquid chromatography-tandem mass spectrometry[J]. Chinese Journal of Chromatography, ;2020, 38(12): 1413-1422. doi: 10.3724/SP.J.1123.2020.05002 shu

Determination of 10 fluoroquinolones residues in aquatic products by accelerated solvent extraction, magnetic solid-phase extraction, and high-performance liquid chromatography-tandem mass spectrometry

WEI Dan ^1,, ,
GUO Ming ² ,
ZHANG Ju ¹

1.
College of Bioscience and Engineering, Hebei University of Economics and Business, Shijiazhuang 050000, China;
2.
Center of Analysis and Testing, Zhejiang Research Institute of Chemical Industry Co., Ltd, Hangzhou 310000, China

Corresponding author: WEI Dan, 1422547228@qq.com
Received Date: 15 May 2020

Fund Project: the Scientific Research Project of Zhejiang Provincial Education Department (No. Y201840776).

In the aquaculture industry, fluoroquinolones are widely used as effective therapeutic agents to prevent animal diseases. The wide bactericidal activity of fluoroquinolones strongly depends on their concentration. Abuse of fluoroquinolones is considered the main reason for the possible occurrence of residues in aquatic products. The increasing presence of residues in aquatic products may pose potential risks to human health. Therefore, it is important to develop an efficient, sensitive, and reliable method for the simultaneous determination of fluoroquinolones in aquatic products. In the analysis of fluoroquinolones, many HPLC methods with different detection techniques have been applied. Among the most common used techniques, HPLC-MS is possible for the determination of very low level analytes in matrix. For the determination of low concentrations of fluoroquinolone residues in aquatic products, preliminary extraction and purification steps are frequently needed to achieve low detection limits. Accelerated solvent extraction (ASE) is well suited for the determination of organic pollutants in solid samples. ASE has the advantages of a high degree of automation, sufficient extraction, high speed, and less solvent consumption, but it has the disadvantage of poor purification effects. Magnetic solid-phase extraction (MSPE) has attracted considerable attention on account of its benefits such as easy separation, less solvent consumption, and quick adsorption of antibiotic residues in liquid samples. The combination of ASE with MSPE makes it possible to sufficiently extract and further purify the target compounds from complex solid samples. Compared with the currently used purification methods of SPE and QuECHERS, MSPE has advantages such as no need of centrifugation and filtration, less solvent consumption, and low cost by appropriate choice of magnetic materials. In this study, a method based on ASE-MSPE-HPLC-MS/MS was developed for the simultaneous determination of sarafloxacin, ofloxacin, enrofloxacin, danofloxacin, lomefloxacin, pefloxacin, ciprofloxacin, enoxacin, norfloxacin, and difloxacin in yellow croaker, grass carp, black fish, prawn, and macrobrachium. As a magnetic purification sorbent, a graphene oxide nanoscale-coated zerovalent iron adsorbent composite (GO@nZVI), was facilely prepared at room temperature. GO and nZVI solutions were rapidly vortex-mixed at 25℃, and then, the magnetite precipitate was magnetically isolated to obtain GO@nZVI. Simpler than the usually used preparation methods, GO@nZVI can be fabricated without complicated multi-step synthesis, fussy operation and harsh conditions. nZVI nanomaterials have strong multiple interactions (hydrogen bonding, electrostatic interaction or their combination) with GO composite only with appropriate adjustment of pH values. The synthesized magnetic purification sorbents were characterized by scanning electron microscopy (SEM), Fourier transform infrared (FT-IR) spectroscopy, and X-ray diffraction (XRD), indicating the successful formation of GO@nZVI. The magnetic material was used to purify and extract ten fluoroquinolone residues in aquatic products via MSPE, followed by ASE. In ASE step, the analytes were extracted from the aquatic products using methanol for 5 min at 70℃, under an extractive pressure of 10.34 MPa for three cycles. The extract was purified by MSPE using GO@nZVI. The target compounds were separated on an Agilent ZORBAX Eclipse Plus C18 column (100 mm×3.0 mm, 1.8 μm) with gradient elution, and analyzed in multiple reaction monitoring (MRM) mode with positive electrospray ionization (ESI⁺). Under the optimized conditions, good linearities were obtained for the ten fluoroquinolones in the range of 1-100 μg/kg, with correlation coefficients above 0.99. LODs (S/N=3) and LOQs (S/N=10) were 0.02-0.29 μg/kg and 0.07-0.98 μg/kg, respectively. At three spiked levels, the recoveries of the fluoroquinolones were between 81.6% and 105.8%, with RSDs between 4.2% and 13.6%. Overall, the major advantages of this combined ASE-MSPE-HPLC-MS/MS method are facile preparation of the magnetic purification material, automated and simple operation, high sensitivity, short extraction time, and less solvent consumption. This sensitive, repetitive method could be successfully employed for the determination of ten fluoroquinolone residues in aquatic products, with good recoveries.
1. [1]
2. [2]
3. [3]
4. [4]
5. [5]
6. [6]
7. [7]
8. [8]
9. [9]
10. [10]
11. [11]
12. [12]
13. [13]
14. [14]
15. [15]
16. [16]
17. [17]
18. [18]
19. [19]
20. [20]
21. [21]
22. [22]
23. [23]
24. [24]
25. [25]
26. [26]
27. [27]
1. [1]
  Yanhui Zhong , Ran Wang , Zian Lin . Analysis of Halogenated Quinone Compounds in Environmental Water by Dispersive Solid-Phase Extraction with Liquid Chromatography-Triple Quadrupole Mass Spectrometry. University Chemistry, 2024, 39(11): 296-303. doi: 10.12461/PKU.DXHX202402017
2. [2]
  Zunxiang Zeng , Yuling Hu , Yufei Hu , Hua Xiao . Analysis of Plant Essential Oils by Supercritical CO₂Extraction with Gas Chromatography-Mass Spectrometry: An Instrumental Analysis Comprehensive Experiment Teaching Reform. University Chemistry, 2024, 39(3): 274-282. doi: 10.3866/PKU.DXHX202309069
3. [3]
  Lihui Jiang , Wanrong Dong , Hua Yang , Yongqing Xia , Hongjian Peng , Jun Yuan , Xiaoqian Hu , Zihan Zeng , Yingping Zou , Yiming Luo . Study on Extraction of p-Hydroxyacetophenone. University Chemistry, 2024, 39(11): 259-268. doi: 10.12461/PKU.DXHX202402056
4. [4]
  Mingyang Men , Jinghua Wu , Gaozhan Liu , Jing Zhang , Nini Zhang , Xiayin Yao . 液相法制备硫化物固体电解质及其在全固态锂电池中的应用. Acta Physico-Chimica Sinica, 2025, 41(1): 2309019-. doi: 10.3866/PKU.WHXB202309019
5. [5]
  Chongjing Liu , Yujian Xia , Pengjun Zhang , Shiqiang Wei , Dengfeng Cao , Beibei Sheng , Yongheng Chu , Shuangming Chen , Li Song , Xiaosong Liu . Understanding Solid-Gas and Solid-Liquid Interfaces through Near Ambient Pressure X-Ray Photoelectron Spectroscopy. Acta Physico-Chimica Sinica, 2025, 41(2): 100013-. doi: 10.3866/PKU.WHXB202309036
6. [6]
  Gaoyan Chen , Chaoyue Wang , Juanjuan Gao , Junke Wang , Yingxiao Zong , Kin Shing Chan . Heart to Heart: Exploring Cardiac CT. University Chemistry, 2024, 39(9): 146-150. doi: 10.12461/PKU.DXHX202402011
7. [7]
  Xiaowu Zhang , Pai Liu , Qishen Huang , Shufeng Pang , Zhiming Gao , Yunhong Zhang . Acid-Base Dissociation Equilibrium in Multiphase System: Effect of Gas. University Chemistry, 2024, 39(4): 387-394. doi: 10.3866/PKU.DXHX202310021
8. [8]
  Shuang Yang , Qun Wang , Caiqin Miao , Ziqi Geng , Xinran Li , Yang Li , Xiaohong Wu . Ideological and Political Education Design for Research-Oriented Experimental Course of Highly Efficient Hydrogen Production from Water Electrolysis in Aerospace Perspective. University Chemistry, 2024, 39(11): 269-277. doi: 10.12461/PKU.DXHX202403044
9. [9]
  Chunai Dai , Yongsheng Han , Luting Yan , Zhen Li , Yingze Cao . Ideological and Political Design of Solid-liquid Contact Angle Measurement Experiment. University Chemistry, 2024, 39(2): 28-33. doi: 10.3866/PKU.DXHX202306065
10. [10]
  Jiao CHEN , Yi LI , Yi XIE , Dandan DIAO , Qiang XIAO . Vapor-phase transport of MFI nanosheets for the fabrication of ultrathin b-axis oriented zeolite membranes. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 507-514. doi: 10.11862/CJIC.20230403
11. [11]
  Zhiwen HU , Weixia DONG , Qifu BAO , Ping LI . Low-temperature synthesis of tetragonal BaTiO₃ for piezocatalysis. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 857-866. doi: 10.11862/CJIC.20230462
12. [12]
  Haiyang Zhang , Yanzhao Dong , Haojie Li , Ruili Guo , Zhicheng Zhang , Jiangjiexing Wu . Exploring the Integration of Chemical Engineering Principle Experiment with Cutting-Edge Research Achievements. University Chemistry, 2024, 39(10): 308-313. doi: 10.12461/PKU.DXHX202405035
13. [13]
  Zhuoming Liang , Ming Chen , Zhiwen Zheng , Kai Chen . Multidimensional Studies on Ketone-Enol Tautomerism of 1,3-Diketones By ¹H NMR. University Chemistry, 2024, 39(7): 361-367. doi: 10.3866/PKU.DXHX202311029
14. [14]
  Zian Lin , Yingxue Jin . Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry (MALDI-MS) for Disease Marker Screening and Identification: A Comprehensive Experiment Teaching Reform in Instrumental Analysis. University Chemistry, 2024, 39(11): 327-334. doi: 10.12461/PKU.DXHX202403066
15. [15]
  Qin Hu , Liuyun Chen , Xinling Xie , Zuzeng Qin , Hongbing Ji , Tongming Su . Ni掺杂构建电子桥及激活MoS₂惰性基面增强光催化分解水产氢. Acta Physico-Chimica Sinica, 2024, 40(11): 2406024-. doi: 10.3866/PKU.WHXB202406024
16. [16]
  Bingliang Li , Yuying Han , Dianyang Li , Dandan Liu , Wenbin Shang . One-Step Synthesis of Benorilate Guided by Green Chemistry Principles and in vivo Dynamic Evaluation. University Chemistry, 2024, 39(6): 342-349. doi: 10.3866/PKU.DXHX202311070
17. [17]
  Fang Niu , Rong Li , Qiaolan Zhang . Analysis of Gas-Solid Adsorption Behavior in Resistive Gas Sensing Process. University Chemistry, 2024, 39(8): 142-148. doi: 10.3866/PKU.DXHX202311102
18. [18]
  Yue Zhao , Yanfei Li , Tao Xiong . Copper Hydride-Catalyzed Nucleophilic Additions of Unsaturated Hydrocarbons to Aldehydes and Ketones. University Chemistry, 2024, 39(4): 280-285. doi: 10.3866/PKU.DXHX202309001
19. [19]
  Liangzhen Hu , Li Ni , Ziyi Liu , Xiaohui Zhang , Bo Qin , Yan Xiong . A Green Chemistry Experiment on Electrochemical Synthesis of Benzophenone. University Chemistry, 2024, 39(6): 350-356. doi: 10.3866/PKU.DXHX202312001
20. [20]
  Guojie Xu , Fang Yu , Yunxia Wang , Meng Sun . Introduction to Metal-Catalyzed β-Carbon Elimination Reaction of Cyclopropenones. University Chemistry, 2024, 39(8): 169-173. doi: 10.3866/PKU.DXHX202401060

Get Citation

PDF

XML

Metrics

PDF Downloads(28)
Abstract views(2373)
HTML views(265)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142