LI Lichun, LIU Shugui, LIN Jiawei, et al. Response Surface Optimization of the QuEChERS Combined with UHPLC-MS/MS Method for Determination of Tetracyclines in Muscle of Channa argus[J]. Science and Technology of Food Industry, 2023, 44(21): 216−226. (in Chinese with English abstract). doi: 10.13386/j.issn1002-0306.2022120266.
Citation: LI Lichun, LIU Shugui, LIN Jiawei, et al. Response Surface Optimization of the QuEChERS Combined with UHPLC-MS/MS Method for Determination of Tetracyclines in Muscle of Channa argus[J]. Science and Technology of Food Industry, 2023, 44(21): 216−226. (in Chinese with English abstract). doi: 10.13386/j.issn1002-0306.2022120266.

Response Surface Optimization of the QuEChERS Combined with UHPLC-MS/MS Method for Determination of Tetracyclines in Muscle of Channa argus

More Information
  • Received Date: January 03, 2023
  • Available Online: October 24, 2023
  • A quick, easy, cheap, effective, rugged and safe pre-treatment method (QuEChERS) was established to evaluate the risk of tetracycline residues in the muscle of Channa argus. The Box-Behnken design (BBD) response surface optimization method was used to optimize the extraction and purification conditions. The samples were extracted with 10 mL acetonitrile (containing 1% formic acid) and 2 mL 0.1 mol/L Na2EDTA-Mcllvaine buffer solution, and the extracts were purified by 150 mg primary secondary amine(PSA)and 200 mg C18, and detected with Ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS). The result showed that the calibration curve was linear in the range of 0.50~100 ng/mL, with high correlation coefficients (r≥0.999). The limits of detection (LOD) and quantification (LOQ) were 0.25~0.75 μg/kg and 0.84~2.00 μg/kg, respectively. The average recoveries of tetracycline, oxytetracycline, chlortetracycline and doxycycline at three different spiked levels in the muscle of Channa argus were 89.5%~118%, with relative standard deviations (RSDs) of 1.11%~8.88%. This method is simple, sensitive and accurate, and can be used for the rapid quantitative determination of tetracyclines in Channa argus.
  • [1]
    李俊锁, 邱月明, 王超. 兽药残留分析[M]. 上海:上海科学技术出版社, 2002:365−390

    LI J S, QIU Y M, WANG C. Analysis of veterinary drug residues [M]. Shanghai:Shanghai Scientific & Technical Publishers, 2002:365−390.
    [2]
    LI S, SHI WZ, LIU W, et al. A duodecennial national synthesis of antibiotics in China's major rivers and seas (2005-2016)[J]. Sci Total Environ,2018,615:906−917. doi: 10.1016/j.scitotenv.2017.09.328
    [3]
    ZHANG M, LIU Y S, ZHAO J L, et al. Occurrence, fate and mass loadings of antibiotics in two swine wastewater treatment systems[J]. Sci Total Environ,2018,639:1421−1431. doi: 10.1016/j.scitotenv.2018.05.230
    [4]
    罗方园, 潘根兴, 李恋卿, 等. 洪泽湖沉积物中四环素土霉素及相关抗性基因的分布特征及潜在风险分析[J]. 农业环境科学学报,2017,36(2):369−375 doi: 10.11654/jaes.2016-1237

    LUO F Y, PAN G X, LI L Q, et al. The distribution characteristics and potential risk of tetracycline, oxytetracycline, and their corresponding gene pollution in sediment of Hongze Lake[J]. Journal of Agro-Environment Science,2017,36(2):369−375. doi: 10.11654/jaes.2016-1237
    [5]
    LEI J, HU X L, YIN D Q, et al. Occurrence, distribution and seasonal variation of antibiotics in the Huangpu River, Shanghai , China[J]. Chemosphere, 2011, 82(6):822−828.
    [6]
    Commossion Regulation No. 508/99 (1999). Official journal of European Community[Z]. 139 March, No. L60.
    [7]
    GOTO T, ITO Y, YAMADA S, et al. High-throughput analysis of tetracycline and penicillin antibiotics in animal tissues using electrospray tandem mass spectrometry with selected reaction monitoring transition[J]. Journal of Chromatography A,2005,1100:193−19. doi: 10.1016/j.chroma.2005.09.056
    [8]
    ORLANDO E A, SIMIONATO A V. Extraction of tetracycline antibiotic residues from fish filet:Comparison and optimization of different procedures using liquid chromatography with fluorescence detection[J]. Journal of Chromatography A,2013,1307:111−118. doi: 10.1016/j.chroma.2013.07.084
    [9]
    GB 31650-2019 食品安全国家标准 食品中兽药最大残留限量[S]. 北京:中国农业出版社, 2020

    GB 31650-2019 National food safety standard maximum residue limits of veterinary drugs in foods [S]. Beijing:China Agriculture Press. 2020.
    [10]
    张启华, 张志军, 田华. 蜂蜜中四环素族抗生素残留量的薄层色谱测定法[J]. 分析测试学报, 1998, 17(4):54−56

    ZHANG Q H, ZHANG Z J, TIAN H. Determination of the residues of tetracyclines antibiotics in honey by thin-layer chromatofraphy[J]. Journal of Instrumental Analysis, 1998, 17 (4):54−56.
    [11]
    张琰图, 章竹君, 孙永华. 高效液相色谱化学发光法检测牛奶中残留四环素类化合物的研究[J]. 化学学报,2006,64(24):2461−2466 doi: 10.3321/j.issn:0567-7351.2006.24.013

    ZHANG Y T, ZHANG Z J, SUN Y H. Determination of tetracyclines residues in milk using high-performance liquid chromatography with chemiluminescence detection[J]. Acta Chimical Sinca,2006,64(24):2461−2466. doi: 10.3321/j.issn:0567-7351.2006.24.013
    [12]
    CHEN Y, KONG D Z, LIU L Q, et al. Development of an ELISA and immunochromatographic assay for tetracycline, oxytetracycline, and chlortetracycline residues in milk and honey based on the class-specific monoclonal antibody[J]. Food Anal Methods,2016,9:905−914. doi: 10.1007/s12161-015-0262-z
    [13]
    檀尊社, 陆恒, 邵伟, 等. 胶体金免疫层析法快速检测水产品中四环素类药物残留[J]. 西北农业学报,2010,19(8):32−37 doi: 10.3969/j.issn.1004-1389.2010.08.007

    TAN Z S, LU H, SHAO W, et al. Nanocolloidal gold-based immunoassay for rapid detection of tetracycline residue in aquatic products[J]. Acta Agriculture Boreali-occidentalis Sinica,2010,19(8):32−37. doi: 10.3969/j.issn.1004-1389.2010.08.007
    [14]
    刘丽, 蔡志斌, 张英. 高效液相色谱法测定水产品中土霉素、四环素、金霉素[J]. 中国卫生检验杂志,2007,17(8):1405−1406 doi: 10.3969/j.issn.1004-8685.2007.08.077

    LIU L, CAI Z B, ZHANG Y. Detection of three antibiotics in aquatic products by HPLC[J]. Chinese Journal of Health Laboratory Technology,2007,17(8):1045−1046. doi: 10.3969/j.issn.1004-8685.2007.08.077
    [15]
    刘艳华, 张纯萍, 门立强, 等. 液相色谱-串联质谱法测定鸡肌肉组织中的四环素类药物残留[J]. 色谱,2006,24(2):171−173 doi: 10.3321/j.issn:1000-8713.2006.02.015

    LIU Y H, ZHANG C P, MEN L Q, et al. Determination of tetracycline antibiotics residues in chicken muscle by liquid chromatography-tandem mass spectrometry[J]. Chinese Journal of Chromatography,2006,24(2):171−173. doi: 10.3321/j.issn:1000-8713.2006.02.015
    [16]
    ABBASI M M, NEMATI M, BABAEI H, et al. Solid-phase extraction and simultaneous determination of tetracycline residues in edible cattle tissues using an HPLC-FL method[J]. Iranian Journal of Pharmaceutical Research, 2012, 11(3):781−787.
    [17]
    WANG G N, ZHANG L, SONG Y P, et al. Application of molecularly imprinted polymer-based matrix solid-phase dispersion for determination of fluoroquinolones, tetracyclines, and sulfonamides in meat[J]. Journal of Chromatography B,2017,1065−1066:104−111. doi: 10.1016/j.jchromb.2017.09.034
    [18]
    ZHOU J H, XUE X F, LI Y, et al. Multiresidue determination of tetracycline antibiotics in propolis by using HPLC-UV detection with ultrasonic-assisted extraction and two-step solid phase extraction[J]. Food Chemistry,2009,115:1074−1080. doi: 10.1016/j.foodchem.2008.12.031
    [19]
    LIU Y, YANG H L, YANG S, et al. High-performance liquid chromatography using pressurized liquid extraction for the determination of seven tetracyclines in egg, fish, and shrimp[J]. Journal of Chromatography B,2013(917-918):11−17.
    [20]
    CRISTINABLASCO, DICORCIA A, YOLANDAPICO. Determination of tetracyclines in multi-specie animal tissues by pressurized liquid extraction and liquid chromatography-tandem mass spectrometry[J]. Food Chemistry,2009,116:1005−1012. doi: 10.1016/j.foodchem.2009.03.055
    [21]
    ALBERO B, SANCHEZ-BRUNETE C, GARCIA-VALCARCEL A I, et al. Ultrasound-assisted extraction of emerging contaminants from environmental samples[J]. Trends in Analytical Chemistry,2015,71:110−118. doi: 10.1016/j.trac.2015.03.015
    [22]
    CHEMAT F, ROMBAUT N, SICAIRE A, et al. Ultrasound assisted extraction of food and natural products. Mechanisms, techniques, combinations, protocols, and applications. A review[J]. Ultrasonics Sonochemistry,2017,34:540−560. doi: 10.1016/j.ultsonch.2016.06.035
    [23]
    王 飞, 宓捷波, 李淑静, 等. 改良的QuEChERS 样本前处理/高效液相色谱-串联质谱法检测猪肉中四环素类兽药的残留[J]. 分析测试学报,2017,2(36):272−275

    WANG F, MI J B, LI S J, et al. Determination of tetracyclines residues in pork by high-performance liquid chromatography-tandem mass spectrometry with modified QuEChERS sample pretreatment[J]. Journal of Instrumental Analysis,2017,2(36):272−275.
    [24]
    GRANDE-MARTINEZA M, MORENO-GONZALEZB D, ARREBOLA-LIEBANASA F J, et al. Optimization of a modified QuEChERS method for the determination of tetracyclines in fish muscle by UHPLC-MS/MS[J]. Journal of Pharmaceutical and Biomedical Analysis,2018,155:27−32. doi: 10.1016/j.jpba.2018.03.029
    [25]
    TOLGYESI A, BEKESI L T, FEKETE V S. Determination of tetracyclines in pig and other meat samples using liquid chromatography coupled with diode array and tandem mass spectrometric detectors[J]. Meat Science,2014,96:1332−1339. doi: 10.1016/j.meatsci.2013.11.011
    [26]
    MARAN J P, MANIKANDAN S, THIRUGNANASAMBANDHAM K, et al. Box-Behnken design-based statistical modeling for ultrasound-assisted extraction of corn silk polysaccharide[J]. Carbohydrate Polymers,2013,92 (1):604−611. doi: 10.1016/j.carbpol.2012.09.020
    [27]
    CURRIE L, HORWITZ W. IUPAC recommendations for defining and measuring detection and quantification limits[J]. Anal Magazine. 1994, 22:M24–26.
    [28]
    CHATTERJEE N S, UTTARA S, BANERJEE K, et al. Multiresidue analysis of multiclass pesticides and polyaromatic hydrocarbons in fatty fish by gas chromatography-tandem mass spectrometry and evaluation of matrix effect[J]. Food Chemistry,2016,196:1−8. doi: 10.1016/j.foodchem.2015.09.014
    [29]
    DIAO P P, CHEN Q, WANG R, et al. Phenolic endocrine-disrupting compounds in the Pearl River Estuary:Occurrence, bioaccumulation and risk assessment[J]. Sci Total Environ,2017,584−585:1100−1107. doi: 10.1016/j.scitotenv.2017.01.169
    [30]
    RAMASWAMY B R, KIM J, ISOBE T, et al. Determination of preservative and antimicrobial compounds in fish from Manila Bay, the Philippines using ultra-high performance liquid chromatography-tandem mass spectrometry, and assessment of human dietary exposure[J]. Journal of Hazardous Materials,2011,192:1739−1745. doi: 10.1016/j.jhazmat.2011.07.006
    [31]
    OMAR T F T, ARIS A Z, . YUSOFF F M, et al. Occurrence and level of emerging organic contaminant in fish and mollusk from Klang River estuary, Malaysia and assessment on human health risk[J]. Environmental Pollution,2019,248:763−773. doi: 10.1016/j.envpol.2019.02.060
    [32]
    LI R J, LIU T J, CUI S H, et al. Residue behaviors and dietary risk assessment of dinotefuran and its metabolites in Oryza sativa by a new HPLC-MS/MS method[J]. Food Chemistry,2017,235:188−193. doi: 10.1016/j.foodchem.2017.04.181
    [33]
    CAARASCO-PANCORBO A, CASADO-TERRONES S, SEGURA-CARRETERO A, et al. Reversed-phase high-performance liquid chromatography coupled to ultraviolet and electrospray time-of-flight mass spectrometry on-line detection for the separation of eight tetracyclines in honey samples[J]. Journal of Chromatography A,2008,1195:107−116. doi: 10.1016/j.chroma.2008.05.003
    [34]
    CRISTOFANI E, CHIARA ANTONINI, TOVO G, et al. A confirmatory method for the determination of tetracyclines in muscle using high-performance liquid chromatography with diode-array detection[J]. Analytica Chimica Acta,2009,637:40−46. doi: 10.1016/j.aca.2008.10.029
    [35]
    WALSH J R, WALKER L V, WEBBER J J. Determination of tetracyclines in bovine and porcine muscle by high-performance liquid chromatography using solid-phase extraction[J]. Journal of Chromatography A,1992,596(2):211−216. doi: 10.1016/0021-9673(92)85009-I
    [36]
    OKA H, ITO Y, MATSUMOTO H. Chromatographic analysis of tetracycline antibiotics in foods[J]. Journal of Chromatography A,2000,882(1-2):109−113. doi: 10.1016/S0021-9673(99)01316-3
    [37]
    WEI Y M, ZHANG Y, XU J, et al. Simultaneous quantification of several classes of antibiotics in water, sediments, and fish muscles by liquid chromatography-tandem mass spectrometry[J]. Frontiers of Environmental Science & Engineering,2014,8:357–371.
    [38]
    VARGASMAMANI M C, AMAYAFARFAN J, REYESREYES F G, et al. Simultaneous determination of tetracyclines in pharmaceuticals by CZE using experimental design[J]. Talanta,2006,70(2):236−243. doi: 10.1016/j.talanta.2006.02.048
    [39]
    MELO A, AGUIAR A, MANSILHA C, et al. Optimisation of a solid-phase microextraction/HPLC/Diode Array method for multiple pesticide screening in lettuce[J]. Food Chemistry,2012,130:1090–1097. doi: 10.1016/j.foodchem.2011.07.137
    [40]
    MILLER J N, MILLER J C. Statistics and chemometrics for analytical chemistry[M]. fifth, Pearson Education Limited, England, 2005.
    [41]
    CARLOS P V, STEPHEN L, TREVOR W, et al. Mixture-amount design and response surface modeling to assess the effects of flavonoids and phenolic acids on developmental performance of Anastrepha ludens[J]. Journal of Chemical Ecology,2014,40(3):297−306. doi: 10.1007/s10886-014-0404-6
    [42]
    MONTEIRO S H, FRANCISCO J G, CAMPION T F, et al. Multiresidue antimicrobial determinationin Nile tilapia ( Oreochromis niloticus) cage farming by liquid chromatographytandem mass spectrometry[J]. Aquaculture,2015,447:37–43. doi: 10.1016/j.aquaculture.2015.07.002
    [43]
    PEREIRA-LOPES R, CAZORLA-REYES R, ROMERO-GONZALEA R, et al. Multiresidue determination of veterinary drugs inaquaculture fish samples by ultra high performance liquid chromatographycoupled to tandem mass spectrometry[J]. J. Chromatogr. B , 2012,895:39–47.
  • Cited by

    Periodical cited type(3)

    1. 杨林雷,沈真辉,罗祥英,李荣平,李荣春. 食用菌麦角硫因的研究进展. 生物工程学报. 2025(02): 574-587 .
    2. 何鑫怡,周子艺,陈媛媛,赵吉春,李富华,明建. 麦角硫因生物活性及其在食品工业中的应用. 食品与发酵工业. 2023(10): 285-292 .
    3. 木开代斯·买合木提,陈建,焦春伟,谢意珍. L-麦角硫因生物合成与应用研究进展. 天然产物研究与开发. 2022(04): 713-721 .

    Other cited types(1)

Catalog

    Article Metrics

    Article views (75) PDF downloads (8) Cited by(4)

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return