LC-MS/MS를 이용한 퇴비 및 액비 중 항생제 동시 분석법 개발
Development of Simultaneous Analytical Method of Veterinary Antibiotics in Manure using Liquid Chromatography Coupled with Tandem Mass Spectrometry
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초록
전국의 퇴비 및 액비 시료에서 대상 항생제 9종(ceftiofur, clopidol, florfenicol, sulfamethazine, sulfamethoxazole, sulfathiazole, tetracycline, tiamulin, tylosin)을 pH 6 McIlvaine buffer를 사용하여 아세트산 함유 아세토니트릴, Na2Cit.5H2O, Na3Cit.2H2O로 추출 후 C18과 PSA로 정제하여 LC-MS/MS로 분석하는 모니터링을 수행하였다. 그 중5종의 항생제 sulfamethazine, sulfathiazole, tylosin, tiamulin 및 clopidol이 국내 퇴·액비 시료에서 검출되었으며 제안한 분석법은 퇴·액비 중 잔류 항생제 모니터링을 위한빠르고 간편한 시험법이라 사료 된다. 본 실험을 통하여 퇴비및 액비 중 축산 항생제의 잔류 현황을 파악하여 모니터링 자료를 확보하였고 이를 활용하여 검출된 항생제들이 안전한토양 및 생태 환경 유지 및 관리의 기초 자료와 더불어 환경기준 예비 항목 및 설정(안)을 위한 기초자료로 제공 및 다양하게 활용될 수 있을 것으로 판단된다.
Abstract
BACKGROUND: The current study was to monitor of 9 veterinary antibiotics (ceftiofur, clopidol, florfenicol, sulfamethazine, sulfamethoxazole, sulfathiazole, tetracycline, tiamulin, and tylosin) inmanure using liquid chromatographytandem mass spectrometry (LC-MS/MS) in positive and negative electrospray ionization mode. METHODS AND RESULTS: Sample preparation was carried out usingMcllvaine buffer and citrate salts to adjust the pH of the sample followed by purification with dispersive solid phase extraction (d-SPE). Separation of analytes during LC-MS/MS analysis was conducted using an Eclipse Plus C18 column and the mobile phase was in gradient mode with, 0.1% formic acid and 5 mM ammonium formate inmethanol (A) and 0.1% formic acid and 5 mM ammonium formate in distilled water (B). The linearity of the matrix-matched calibrations of all tested antibioticswas good, with R2determination coefficients ≥ 0.9920. The limit of detection (LOD) and quantifications (LOQ) were 0.1-67.0 μg/kg and 0.4-200.0 μg/kg, respectively. Analysis of 13 solid and liquid manure samples taken from the Republic of Korea revealed concentrations less than 0.7 μg/kg for tiamulin, 1497.6 μ g/kg for sulfamethazine. CONCLUSION: To monitor 9 veterinary antibiotics from manure samples in 13 provincial areas throughout the Republic of Korea, an analytical method was developed. The developedmethodwas fully validated and successfully applied for monitoring various veterinary antibiotics in manure samples.
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