Abstract
Objective:This study aimed to develop a method of rapid detection of tetracyclines including tetracycline, oxytetracycline, aureomycin and doxycyclin in aquatic products with deep eutectic solvents (DES) extraction and ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS).Methods:Different parameters of DES, such as the types of solvents, molar ratio of solvents, water content, and pH value were optimized.Results:The optimum deep eutectic solvent conditions for the medicament analysis of four tetracyclines in aquatic products were choline chloride-glycerol combination(molar ratio 1∶4) with 90% moisture content and 0.1% formic acid. Under the control of these condition, the four types of tetracyclines could be significantly separated, with a linear correlation of 0.999 4 in the mass concentration range of 5.0~200.0 ng/mL and LOD of 20.0 μg/kg. The recovery of each target component ranged from 82.2% to 102.8%, and the RSD was less than 10%. The analytical method developed was used to detect four kinds of tetracyclines in different samples including 13 batches of commercially available aquatic products, one quality control (QC) sample, and one international proficiency testing sample. The result indicated that oxytetracycline and doxycycline could be detected in one batch of shrimp sample from the market with a concentration of 64.8 μg/kg, and 25.4 μg/kg, respectively, while the content of tetracyclines in QC sample and international proficiency testing sample were all within the limits of given characteristic values.Conclusion:The novel DES-UPLC-MS/MS method developed is feasible to both the qualitative and quantitative analysis of the tetracyclines in aquatic products, which an advantage of simple pre-processing and high accuracy and efficiency.
Publication Date
7-7-2022
First Page
40
Last Page
45
DOI
10.13652/j.issn.1003-5788.2022.02.007
Recommended Citation
Zi-xiong, LIU; Guo-dan, XIE; Gui-liang, TAN; Hong-tao, ZHENG; Hai, DONG; and Jing-hui, HUANG
(2022)
"Rapid determination of drug residues of four kinds of tetracyclines using DES-UPLC-MS/MS in aquatic products,"
Food and Machinery: Vol. 38:
Iss.
2, Article 7.
DOI: 10.13652/j.issn.1003-5788.2022.02.007
Available at:
https://www.ifoodmm.cn/journal/vol38/iss2/7
References
[1] ABBOTT A P,CAPPER G,DAVIES D L,et al.Novel solvent properties of choline chloride/urea mixtures[J].Chemical Communications,2003,9(1):70-71.
[2] ZHANG K G,LIU C,LI S Y,et al.Vortex-assisted liquid-liquid microextraction based on a hydrophobic deep eutectic solvent for the highly efficient determination of Sudan I in food samples[J].Analytical Letters,2020,53(8):1 204-1 217.
[3] 刘慧强,陈美婷,王韦达,等.低共熔溶剂萃取超高效液相色谱法检测调味油中酸性橙Ⅱ、碱性橙21和碱性橙22[J].分析试验室,2018,37(8):932-936.LIU Hui-qiang,CHEN Mei-ting,WANG Wei-da,et al.Determination of acid orange II,alkaline orange 21 and alkaline orange 22 in flavoured oil by deep eutectic solvent extraction combined with ultra high performance liquid chromatography[J].Chinese Journal of Analysis Laboratory,2018,37(8):932-936.
[4] ZHU Shu-qiang,ZHOU Jia,JIA Hong-fang,et al.Liquid-liquid microextraction of synthetic pigments in beverages using a hydrophobic deep eutectic solvent[J].Food Chemistry,2018,243:351-356.
[5] 张康迪,刘伟.基于低共熔溶剂的液相微萃取-高效液相色谱法测定大豆油中的TBHQ[J].河南工业大学学报(自然科学版),2017,38(5):32-36.ZHANG Kang-di,LIU Wei.Deep eutectic solvent based solvent microextraction-HPLC method for determination of TBHQ in soybean oil[J].Journal of Henan University of Technology(Natural Science Edition),2017,38(5):32-36.
[6] ZHAO Jing,MENG Zhao-rui,ZHAO Ze-xin,et al.Ultrasound-assisted deep eutectic solvent as green and efficient media combined with functionalized magnetic multi-walled carbon nanotubes as solid-phase extraction to determine pesticide residues in food products[J].Food Chemistry,2020,310:125863.1-125863.8.
[7] SHISHOV A,GORBUNOV A,BARANOVSKII E,et al.Microextraction of sulfonamides from chicken meat samples in three-component deep eutectic solvent[J].Microchemical Journal,2020,158:105274.
[8] 王漫漫,赵晶,郭春晓,等.DES-HPLC法同时测定桂枝中香豆素、桂皮酸和桂皮醛的含量[J].沈阳药科大学学报,2018,35(11):956-960.WANG Man-man,ZHAO Jing,GUO Chun-xiao,et al.DES-HPLC to simutaneously determine the contents of coumarin,cinnamic acid and cinnamaldehyde in Cinnamomi Ramulus[J].Journal of Shenyang Pharmaceutical University,2018,35(11):956-960.
[9] WANG Gen,CUI Qi,YIN Lu-jun,et al.Efficient extraction of flavonoids from flos sophorae immaturus by tailored and sustainable deep eutectic solvent as green extraction media[J].Journal of Pharmaceutical and Biomedical Analysis,2019,170:285-294.
[10] KOUTSOUKOS S,TSIAKA T,TZANI A,et al.Choline chloride and tartaric acid,a natural deep eutectic solvent for the efficient extraction of phenolic and carotenoid compounds[J].Journal of Cleaner Production,2019,241:118384.
[11] 王程娅,郑绪东,雷萍,等.低共熔溶剂微萃取—高效液相色谱法测定烟叶中β-胡萝卜素[J].理化检验(化学分册),2019,55(8):912-915.WANG Cheng-ya,ZHENG Xu-dong,LEI Ping,et al.HPLC Determination of beta carotene in tobacco leaves with deep eutectic solvent microextraction[J].Physical Testing and Chemical Analysis(Part B:Chemical Analysis),2019,55(8):912-915.
[12] 陈冉,李德慧,阮桂发,等.基于绿色低共熔溶剂法高效提取鸡骨草中的黄酮和皂苷[J].天然产物研究与开发,2019,31(9):1 632-1 640.CHEN Ran,LI De-hui,RUAN Gui-fa,et al.Green and efficient extraction of flavoniods and saponins from Abrus cantoniensis Hance by deep eutectic solvents[J].Natural Product Research and Development,2019,31(9):1 632-1 640.
[13] 田富林,黄文晶,王展,等.植物多酚提取研究进展[J].食品与机械,2020,36(9):211-216.TIAN Fu-lin,HUANG Wen-jing,WANG Zhan,et al.Research progress on the extraction of plant polyphenols[J].Food & Machinery,2020,36(9):211-216.
[14] 赵桐桐,张冬昊,郭振福,等.低共熔溶剂液相微萃取技术测定5种杀菌剂农药残留分析方法[J].现代食品科技,2019,35(8):281-286.ZHAO Tong-tong,ZHANG Dong-hao,GUO Zhen-fu,et al.A liquid-phase microextraction method based on deep eutectic solvents determination for five Kinds of fungicides residues[J].Modern Food Science and Technology,2019,35(8):281-286.
[15] LIU Yong-jing,XU Wen,ZHANG Hua,et al.Hydrophobic deep eutectic solvent-based dispersive liquid-liquid microextraction for the simultaneous enantiomeric analysis of five β-agonists in the environmental samples[J].Electrophoresis,2019,40(21):2 828-2 836.
[16] DI Xin,ZHAO Xiao-jun,GUO Xiao-li.Hydrophobic deep eutectic solvent as a green extractant for high-performance liquid chromatographic determination of tetracyclines in water samples[J].Journal of Separation Science,2020,43(15):3 129-3 135.
[17] HU Xi-zhou,ZHANG Lu-yun,XIA Hong,et al.Dispersive liquid-liquid microextraction based on a new hydrophobic deep eutectic solvent for the determination of phenolic compounds in environmental water samples[J].Journal of Separation Science,2021,44(7):1 510-1 520.
[18] 中华人民共和国农业部.四环素类药物水产养殖使用规范:SC/T 1085—2006[S].北京:中国农业出版社,2006:1.Ministry of Agriculture of the PRC.Specification for the application of tetracyclines in aquaculture:SC/T 1085—2006[S].Beijing:China agriculture press,2006:1.
[19] 梅英杰,史新宇,董瑾,等.超高效液相色谱—串联质谱法同时检测鸡肉中氯霉素、四环素、金霉素和土霉素[J].食品与发酵工业,2017,43(8):240-245.MEI Ying-jie,SHI Xin-yu,DONG Jin,et al.Determination of chloramphenicol,tetracycline,chlortetracycline and oxytetracycline in chicken by ultra performance liquid chromatography-tandem mass spectrometry[J].Food and Fermentation Industries,2017,43(8):240-245.
[20] 刑俊生,张彬,李倩.食品虾仁中土霉素、四环素、金霉素含量测定方法的建立[J].中国药事,2017,31(10):1 199-1 204.XING Jun-sheng,ZHANG Bin,LI Qian.Establishment of the method to determine terramycin,tetracycline and chlorotetracycline in shrimp meat[J].Chinese Pharmaceutical Affairs,2017,31(10):1 199-1 204.
[21] 石春红,曹向英,曹美萍.超高效液相色谱—串联质谱法分析动物源性食品中4种四环素类药物残留[J].食品安全质量检测学报,2019,10(10):3 126-3 131.SHI Chun-hong,CAO Xiang-ying,CAO Mei-ping.Determination of 4 kinds of tetracycline drugs residues in food of animal origin by ultra performance liquid chromatography-tandem mass spectrometry[J].Journal of Food Safety and Quality,2019,10(10):3 126-3 131.
[22] CHEN Jian,WEI Zhen,CAO Xian-ying.QuEChERS pretreatment combined with ultra-performance liquid chromatography-tandem mass spectrometry for the determination of four veterinary drug residues in marine products[J].Food Analytical Methods,2019,12(5):1 055-1 066.
[23] 王志昱,张桂芳,张晓瑜,等.QuEChERS-高效液相色谱—质谱联用法同时检测鸡胗和鸡肝中15种喹诺酮类和四环素类抗生素[J].肉类研究,2020,34(3):51-57.WANG Zhi-yu,ZHANG Gui-fang,ZHANG Xiao-yu,et al.Simultaneous determination of 15 quinolones and tetracyclines antibiotics in chicken gizzard and liver by QuEChERS-high performance liquid chromatography-mass Spectrometry[J].Meat Research,2020,34(3):51-57.