Browse > Article
http://dx.doi.org/10.15681/KSWE.2016.32.6.670

Determination of Veterinary Antibiotic Residues: IV. Comparable Analytical Methods with EPA Methods 1694_A Review  

Kim, Chansik (Watershed and Total Load Management Research Division, Water Environment Research Department, National Institute of Environmental Research)
Ryu, Hong-Duck (Watershed and Total Load Management Research Division, Water Environment Research Department, National Institute of Environmental Research)
Chung, Eu Gene (Watershed and Total Load Management Research Division, Water Environment Research Department, National Institute of Environmental Research)
Kim, Yongseok (Watershed and Total Load Management Research Division, Water Environment Research Department, National Institute of Environmental Research)
Rhew, Doug Hee (Watershed and Total Load Management Research Division, Water Environment Research Department, National Institute of Environmental Research)
Publication Information
Journal of Korean Society on Water Environment / v.32, no.6, 2016 , pp. 670-699 More about this Journal
Abstract
In this study, 16 antibiotics were selected from among the top 30 veterinary antibiotics sold in South Korea in 2014, as well as from among the pharmaceuticals targeted by EPA method 1694, in order to review analytical methods for the detection of trace levels of antibiotics in environmental samples: surface water, soils, animal origin foods, and manures. LC-MS/MS was heavily used. In the chromatography for the detection of the selected antibiotics, the $C_{18}$ column was mostly used at the temperature of $30{\sim}40^{\circ}C$. Water and methanol/acetonitrile were commonly chosen as a nonpolar and a polar mobile phase, respectively. Gradient elution was applied to separate multiclass antibiotics. Volatile additives, such as formic acid, acetic acid, and ammonium acetate were mixed with the mobile phase to improve the ionization efficiency of analytes and the sensitivity in MS detection. Electrospray ionization (ESI) was widely used in the LC-MS/MS and positive ionization was preferred to determine the selected antibiotics. A protonated $[M+H]^+$ molecule was selected as a precursor ion, and its two transitions were analyzed, one for quantitative measurement and the other for confirmation. This study reviewed linearity of the calibration curve, recovery, repeatability, method detection limits (MDLs), and method quantification limits (MQLs) for each target compound used to validate the developed analytical methods.
Keywords
Analytical methods; EPA method 1694; HPLC-MS/MS; Veterinary antibiotics;
Citations & Related Records
Times Cited By KSCI : 1  (Citation Analysis)
연도 인용수 순위
1 Yang, S., Cha, J., and Carlson, K. (2004). Quantitative Determination of Trace Concentrations of Tetracycline and Sulfonamide Antibiotics in Surface Water Using Solid-Phase Extraction and Liquid Chromatography/Ion Trap Tandem Mass Spectrometry, Rapid Communications in Mass Spectrometry, 18(18), pp. 2131-2145.   DOI
2 Zhou, L. J., Ying, G. G., Liu, S., Zhao, J. L., Chen, F., Zhang, R. Q., Peng, F. Q., and Zhang, Q. Q. (2012). Simultaneous Determination of Human and Veterinary Antibiotics in Various Environmental Matrices by Rapid Resolution Liquid Chromatography-Electrospray Ionization Tandem Mass Spectrometry, Journal of Chromatography A, 1244, pp. 123-138.   DOI
3 Zhou, L. J., Ying, G. G., Liu, S., Zhang, R. Q., Lai, H. J., Chen, Z. F., and Pan, C. G. (2013). Excretion Masses and Environmental Occurrence of Antibiotics in Typical Swine and Dairy Cattle Farms in China, Science of the Total Environment, 444, pp. 183-195.   DOI
4 National Institute of Environmental Research (NIER). (2010). Environmental Examination･Inspection QA/QC Handbook, 2nd ed, 11-1480083-000291-01, National Institute of Environmental Research, pp. 21-25.
5 Lindsey, M. E., Meyer, M., and Thurman, E. M. (2001). Analysis of Trace Levels of Sulfonamide and Tetracycline Antimicrobials in Groundwater and Surface Water Using Solid-Phase Extraction and Liquid Chromatography/Mass Spectrometry, Analytical Chemistry, 73(19), pp. 4640-4646.   DOI
6 Bohm, D. A., Stachel, C. S., and Gowik, P. (2012). Validation of a Multi-Residue Method for the Determination of Several Antibiotic Groups in Honey by LC-MS/MS, Analytical and Bioanalytical Chemistry, 403(10), pp. 2943-2953.   DOI
7 Aguilera-Luiz, M. M., Vidal, J. M., Romero-Gonzalez, R., and Frenich, A. G. (2012). Multiclass Method for Fast Determination of Veterinary Drug Residues in Baby Food by Ultra- High-Performance Liquid Chromatography-Tandem Mass Spectrometry, Food Chemistry, 132(4), pp. 2171-2180.   DOI
8 Avisar, D., Primor, O., Gozlan, I., and Mamane, H. (2010). Sorption of Sulfonamides and Tetracyclines to Montmorillonite Clay, Water, Air, & Soil Pollution, 209(1-4), pp. 439-450.   DOI
9 Ben, W., Qiang, Z., Adams, C., Zhang, H., and Chen, L. (2008). Simultaneous Determination of Sulfonamides, Tetracyclines and Tiamulin in Swine Wastewater by Solid-Phase Extraction and Liquid Chromatography-Mass Spectrometry, Journal of Chromatography A, 1202(2), pp. 173-180.   DOI
10 United Nations, Department of Economic and Social Affairs, Population Division. (2015). World Population Prospects: The 2015 Revision, Key Findings and Advance Tables. Working Paper No. ESA/P/WP.241, United Nations, New York, pp. 2-3.
11 United States Department of Agriculture (USDA). (2016). http://www.ars.usda.gov/Main/docs.htm? docid=6750&page=1.
12 Malintan, N. T. and Mohd, M. A. (2006). Determination of Sulfonamides in Selected Malaysian Swine Wastewater by High-Performance Liquid Chromatography, Journal of Chromatography A, 1127(1), pp. 154-160.   DOI
13 Nebot, C., Iglesias, A., Regal, P., Miranda, J., Cepeda, A., and Fente, C. (2012). Development of a Multi-class Method for the Identification and Quantification of Residues of Antibiotics, Coccidiostats and Corticosteroids in Milk by Liquid Chromatography-Tandem Mass Spectrometry, International Dairy Journal, 22(1), pp.78-85.   DOI
14 Neu, H. C. (1992). The Crisis in Antibiotic Resistance, Science, 257(5073), pp. 1064-1073.   DOI
15 Locatelli, M. A. F., Sodre, F. F., and Jardim, W. F. (2011). Determination of Antibiotics in Brazilian Surface Waters Using Liquid Chromatography-Electrospray Tandem Mass Spectrometry, Archives of Environmental Contamination and Toxicology, 60(3), pp. 385-393.   DOI
16 Lopes, R. P., Reyes, R. C., Romero-Gonzalez, R., Vidal, J. L. M., and Frenich, A. G. (2012). Multiresidue Determination of Veterinary Drugs in Aquaculture Fish Samples by Ultra High Performance Liquid Chromatography Coupled to Tandem Mass Spectrometry, Journal of Chromatography B, 895, pp. 39-47.
17 Martinez-Carballo, E., Gonzalez-Barreiro, C., Scharf, S., and Gans, O. (2007). Environmental Monitoring Study of Selected Veterinary Antibiotics in Animal Manure and Soils in Austria, Environmental Pollution, 148(2), pp. 570-579.   DOI
18 McArdell, C. S., Molnar, E., Suter, M. J. F., and Giger, W. (2003). Occurrence and Fate of Macrolide Antibiotics in Wastewater Treatment Plants and in the Glatt Valley Watershed, Switzerland, Environmental Science & Technology, 37(24), pp. 5479-5486.   DOI
19 United States Environmental Protection Agency (U. S. EPA). (1996). Method 8321A Solvent Extractable Nonvolatile Compounds by High Performance Liquid Chromatography/Thermospray/Mass Spectrometry (HPLC/TS/MS) or Ultraviolet (UV) Detection, U.S. Environmental Protection Agency.
20 United States Environmental Protection Agency (U. S. EPA). (1984). Method 610: Polynuclear Aromatic Hydrocarbons, U.S. Environmental Protection Agency.
21 United States Environmental Protection Agency (U. S. EPA). (2007). Method 1694: Pharmaceuticals and Personal Care Products in Water, Soil, Sediment, and Biosolids by HPLC/MS/MS, EPA-821-R-08-002, U.S. Environmental Protection Agency, Washington, DC.
22 Salvia, M. V., Vulliet, E., Wiest, L., Baudot, R., and Cren-Olive, C. (2012). Development of a Multi-Residue Method Using Acetonitrile-Based Extraction Followed by Liquid Chromatography-Tandem Mass Spectrometry for the Analysis of Steroids and Veterinary and Human Drugs at Trace Levels in Soil, Journal of Chromatography A, 1245, pp. 122-133.   DOI
23 Prat, M. D., Benito, J., Compano, R., Hernandez-Arteseros, J. A., and Granados, M. (2004). Determination of Quinolones in Water Samples by Solid-Phase Extraction and Liquid Chromatography with Fluorimetric Detection, Journal of Chromatography A, 1041(1), pp. 27-33.   DOI
24 Pfeifer, Y., Cullik, A., and Witte, W. (2010). Resistance to Cephalosporins and Carbapenems in Gram-Negative Bacterial Pathogens, International Journal of Medical Microbiology, 300(6), pp. 371-379.   DOI
25 Pozo, O. J., Guerrero, C., Sancho, J. V., Ibanez, M., Pitarch, E., Hogendoorn, E., and Hernandez, F. (2006). Efficient Approach for the Reliable Quantification and Confirmation of Antibiotics in Water Using On-Line Solid-Phase Extraction Liquid Chromatography/Tandem Mass Spectrometry, Journal of Chromatography A, 1103(1), pp. 83-93.   DOI
26 Schlusener, M. P., Con Arb, M. A., and Bester, K. (2006). Elimination of Macrolides Tiamulin and, Salinomycin During Manure Storage, Archives of Environmental Contamination and Toxicology, 51(1), pp. 21-28.   DOI
27 Hirsch, R., Ternes, T. A., Haberer, K., Mehlich, A., Ballwanz, F., and Kratz, K. L. (1998). Determination of Antibiotics in Different Water Compartments via Liquid Chromatography-Electrospray Tandem Mass Spectrometry, Journal of Chromatography A, 815(2), pp. 213-223.   DOI
28 Nakata, H., Kannan, K., Jones, P. D., and Giesy, J. P. (2005). Determination of Fluoroquinolone Antibiotics in Wastewater Effluents by Liquid Chromatography-Mass Spectrometry and Fluorescence Detection, Chemosphere, 58(6), pp. 759-766.   DOI
29 Korea Ministry of Government Legislation. (2015). Act On The Management and Use of Livestock Excreta, 13526, Korea Ministry of Government Legislation.
30 Li, J. D., Cai, Y. Q., Shi, Y. L., Mou, S. F., and Jiang, G. B. (2007). Determination of Sulfonamide Compounds in Sewage and River by Mixed Hemimicelles Solid-Phase Extraction Prior to Liquid Chromatography-Spectrophotometry, Journal of Chromatography A, 1139(2), pp. 178-184.   DOI
31 Ho, Y. B., Zakaria, M. P., Latif, P. A., and Saari, N. (2012). Simultaneous Determination of Veterinary Antibiotics and Hormone in Broiler Manure, Soil and Manure Compost by Liquid Chromatography-Tandem Mass Spectrometry, Journal of Chromatography A, 1262, pp. 160-168.   DOI
32 Ho, Y. B., Zakaria, M. P., Latif, P. A., and Saari, N. (2014). Occurrence of Veterinary Antibiotics and Progesterone in Broiler Manure and Agricultural Soil in Malaysia, Science of the Total Environment, 488, pp. 261-267.
33 Hong, Y., Sharma, V. K., Chiang, P. C., and Kim, H. (2015). Fast-Target Analysis and Hourly Variation of 60 Pharmaceuticals in Wastewater Using UPLC-High Resolution Mass Spectrometry, Archives of Environmental Contamination and Toxicology, 69(4), pp. 525-534.   DOI
34 Iglesias, A., Nebot, C., Miranda, J. M., Vazquez, B. I., and Cepeda, A. (2012). Detection and Quantitative Analysis of 21 Veterinary Drugs in River Water Using High-pressure Liquid Chromatography Coupled to Tandem Mass Spectrometry, Environmental Science and Pollution Research, 19(8), pp. 3235-3249.   DOI
35 United States Environmental Protection Agency (U. S. EPA). (2010). Method 1668A Interlaboratory Validation Study Report, EPA-820-R-10-004, U.S. Environmental Protection Agency, Washington, DC.
36 United States Food and Drug Administration (U. S. FDA). (2015). http://www.fda.gov/AnimalVeterinary/SafetyHealth/AntimicrobialResistance/NationalAntimicrobialResistanceMonitoringSystem/default.html.
37 Yang, J. F., Ying, G. G., Zhao, J. L., Tao, R., Su, H. C., and Chen, F. (2010). Simultaneous Determination of Four Classes of Antibiotics in Sediments of the Pearl Rivers Using RRLC-MS/MS, Science of the Total Environment, 408(16), pp. 3424-3432.   DOI
38 Hou, J., Wan, W., Mao, D., Wang, C., Mu, Q., Qin, S., and Luo, Y. (2015). Occurrence and Distribution of Sulfonamides, Tetracyclines, Quonolones, Macrolides, and Nitrofurans in Livestock Manure and Amended Soils of Northern China, Environmental Science and Pollution Research, 22(6), pp. 4545-4554.   DOI
39 Hur, J., Jawale, C., and Lee, J. H. (2012). Antimicrobial Resistance of Salmonella Isolated from Food Animals: A Review, Food Research International, 45(2), pp. 819-830.   DOI
40 Seifrtova, M., Novakova, L., Lino, C., Pena, A., and Solich, P. (2009). An Overview of Analytical Methodologies for the Determination of Antibiotics in Environmental Waters. Analytica Chimica Acta, 649(2), pp. 158-179.   DOI
41 Tang, Y. Y., Lu, H. F., Lin, H. Y., Shih, Y. C., and Hwang, D. F. (2012). Multiclass Analysis of 23 Veterinary Drugs in Milk by Ultraperformance Liquid Chromatography-Electrospray Tandem Mass Spectrometry, Journal of Chromatography B, 881, pp. 12-19.
42 Tao, Y., Yu, G., Chen, D., Pan, Y., Liu, Z., Wei, H., Peng, D., Huang, L., Wang, Y., and Yuan, Z. (2012). Determination of 17 Macrolide Antibiotics and Avermectins Residues in Meat with Accelerated Solvent Extraction by Liquid Chromatography-Tandem Mass Spectrometry, Journal of Chromatography B, 897, pp. 64-71.   DOI
43 Tolls, J. (2001). Sorption of Veterinary Pharmaceuticals in Soils: A Review, Environmental Science & Technology, 35(17), pp. 3397-3406.   DOI
44 Li, W., Shi, Y., Gao, L., Liu, J., and Cai, Y. (2012). Occurrence of Antibiotics in Water, Sediments, Aquatic Plants, and Animals from Baiyangdian Lake in North China, Chemosphere, 89(11), pp. 1307-1315.   DOI
45 Li, Z., Chang, P. H., Jean, J. S., Jiang, W. T., and Wang, C. J. (2010). Interaction Between Tetracycline and Smectite in Aqueous Solution, Journal of Colloid and Interface Science, 341(2), pp. 311-319.   DOI
46 Lim S. K., Lee, J. E., Lee, H. S., Nam, H. M., Moon, D. C., Jang, G. C., Park, Y. J., Jung, Y. G., Jang, S. C., and Wee, S. H. (2014). Trends in Antimicrobial Sales for Livestock and Fisheries in Korea During 2003-2012, Korean Journal of Veterinary Research, 54(2), pp. 81-86. [Korean Literature]   DOI
47 Karthikeyan, K. G. and Meyer, M. T. (2006). Occurrence of Antibiotics in Wastewater Treatment Facilities in Wisconsin, USA, Science of the Total Environment, 361(1), pp. 196-207.   DOI
48 Jacobsen, A. M. and Halling-Sorensen, B. (2006). Multi-Component Analysis of Tetracyclines, Sulfonamides and Tylosin in Swine Manure by Liquid Chromatography-Tandem Mass Spectrometry, Analytical and Bioanalytical Chemistry, 384(5), pp. 1164-1174.   DOI
49 Kaklamanos, G., Vincent, U., and von Holst, C. (2013). Analysis of Antimicrobial Agents in Pig Feed by Liquid Chromatography Coupled to Orbitrap Mass Spectrometry, Journal of Chromatography A, 1293, pp. 60-74.   DOI
50 Kartal, S. N. (2003). Removal of Copper, Chromium, and Arsenic from CCA-C Treated Wood by EDTA Extraction, Waste Management, 23(6), pp. 537-546.   DOI
51 Kim, Y., Lim, S., Han, M., and Cho, J. (2012). Sorption Characteristics of Oxytetracycline, Amoxicillin, and Sulfathiazole in Two Different Soil Types, Geoderma, 185, pp. 97-101.
52 Carretero, V., Blasco, C., and Pico, Y. (2008). Multi-Class Determination of Antimicrobials in Meat by Pressurized Liquid Extraction and Liquid Chromatography-Tandem Mass Spectrometry, Journal of Chromatography A, 1209(1), pp. 162-173.   DOI
53 Boscher, A., Guignard, C., Pellet, T., Hoffmann, L., and Bohn, T. (2010). Development of a Multi-Class Method for the Quantification of Veterinary Drug Residues in Feedingstuffs by Liquid Chromatography-Tandem Mass Spectrometry, Journal of Chromatography A, 1217(41), pp. 6394-6404.   DOI
54 Bonnet, R. (2004). Growing Group of Extended-Spectrum ${\beta}$-Lactamases: the CTX-M Enzymes, Antimicrobial Agents and Chemotherapy, 48(1), pp. 1-14.   DOI
55 Bronzwear, S. L. A. M., Cars, O., Buchholz, U., Molstad, S., Goettsch, W., Veldhuijzen, I. K., Kool, J. L., Sprenger, M. J., and Degener, J. E. (2002). A European Study on The Relationship of Antimicrobial Use and Antimicrobial Resistance, Emerging Infectious Diseases, 8(3), pp. 278-282.   DOI
56 Castiglioni, S., Bagnati, R., Calamari, D., Fanelli, R., and Zuccato, E. (2005). A Multiresidue Analytical Method Using Solid-Phase Extraction and High-Pressure Liquid Chromatography Tandem Mass Spectrometry to Measure Pharmaceuticals of Different Therapeutic Classes in Urban Wastewaters, Journal of Chromatography A, 1092(2), pp. 206-215.   DOI
57 Kolpin, D. W., Furlong, E. T., Meyer, M. T., Thurman, E. M., Zaugg, S. D., Barber, L. B., and Buxton, H. T. (2002). Pharmaceuticals, Hormones, and Other Organic Wastewater Contaminants in US Streams, 1999-2000: A National Reconnaissance, Environmental Science & Technology, 36(6), pp. 1202-1211.   DOI
58 Babic, S., Asperger, D., Mutavdzic, D., Horvat, A. J., and Kastelan-Macan, M. (2006). Solid Phase Extraction and HPLC Determination of Veterinary Pharmaceuticals in Wastewater, Talanta, 70(4), pp. 732-738.   DOI
59 Behera, S. K., Kim, H. W., Oh, J. E., and Park, H. S. (2011). Occurrence and Removal of Antibiotics, Hormones and Several Other Pharmaceuticals in Wastewater Treatment Plants of the Largest Industrial City of Korea, Science of the Total Environment, 409(20), pp. 4351-4360.   DOI
60 Dasenaki, M. E. and Thomaidis, N. S. (2010). Multi-Residue Determination of Seventeen Sulfonamides and Five Tetracyclines in Fish Tissue Using a Multi-Stage LC-ESI-MS/MS Approach Based on Advanced Mass Spectrometric Techniques, Analytica Chimica Acta, 672(1), pp. 93-102.   DOI
61 Centers for Disease Control and Preventation (CDC). (2013). Antibiotic Resistance Threats in the United States, 2013, Center for Disease Control and Prevention, US Department of Health and Human Services, Atlanta, Georgia, pp. 13-17.
62 Centers for Disease Control and Preventation (CDC). (2015). http://www.cdc.gov/narms/about/index.html.
63 Freitas, A., Barbosa, J., and Ramos, F. (2014). Multi-Residue and Multi-Class Method for the Determination of Antibiotics in Bovine Muscle by Ultra-High-Performance Liquid Chromatography Tandem Mass Spectrometry, Meat Science, 98(1), pp. 58-64.   DOI
64 Dolliver, H., Gupta, S., and Noll, S. (2008). Antibiotic Degradation During Manure Composting. Journal of Environmental Quality, 37(3) pp. 1245-1253.   DOI
65 EU Commission. (2002). Commission Decision EC 2002/657 of 12 August 2002 Implementing Council Directive 96/23/EC Concerning the Performance of Analytical Methods and the Interpretation of Results, Official Journal of European Communities, L 221, pp. 8-36.
66 Fiese, E. F. and Steffen, S. H. (1990). Comparison of the Acid Stability of Azithromycin and Erythromycin A, Journal of Antimicrobial Chemotherapy, 25(suppl A), pp. 39-47.
67 Gao, L., Shi, Y., Li, W., Niu, H., Liu, J., and Cai, Y. (2012). Occurrence of antibiotics in eight sewage treatment plants in Beijing, China, Chemosphere, 86(6), pp. 665-671.   DOI
68 Gbylik-Sikorska, M., Posyniak, A., Sniegocki, T., and Zmudzki, J. (2015). Liquid Chromatography-Tandem Mass Spectrometry Multiclass Method for the Determination of Antibiotics Residues in Water Samples from Water Supply Systems in Food-Producing Animal Farms, Chemosphere, 119, pp. 8-15.   DOI
69 Goossens, H., Ferech, M., Vander Stichele, R., Elseviers, M., and ESAC Project Group. (2005). Outpatient Antibiotic Use in Europe and Association with Resistance: a Cross-National Database Study, The Lancet, 365(9459), pp. 579-587.   DOI
70 Gorissen, B., Reyns, T., Devreese, M., De Backer, P., Van Loco, J., and Croubels, S. (2015). Determination of Selected Veterinary Antimicrobials in Poultry Excreta by UHPLC-MS/MS, for Application in Salmonella Control Programs, Analytical and Bioanalytical Chemistry, 407(15), pp. 4447-4457.   DOI
71 Hao, C., Lissemore, L., Nguyen, B., Kleywegt, S., Yang, P., and Solomon, K. (2006). Determination of Pharmaceuticals in Environmental Waters by Liquid Chromatography/Electrospray Ionization/Tandem Mass Spectrometry, Analytical and Bioanalytical Chemistry, 384(2), pp. 505-513.
72 Gros, M., Rodriguze-Mozaz, S., and Barcelo, D. (2013). Rapid Analysis of Multiclass Antibiotic Residues and Some of Their Metabolites in Hospital, Urban Wastewater and River Water by Ultra-High-Performance Liquid Chromatography Coupled to Quadrupole-Linear Ion Trap Tandem Mass Spectrometry, Journal of Chromatography A, 1292, pp. 173-188.   DOI
73 Han, R. W., Zheng, N., Yu, Z. N., Wang, J., Xu, X. M., Qu, X. Y., Li, S. L., Zhang, Y. D., and Wang, J. Q. (2015). Simultaneous Determination of 38 Veterinary Antibiotic Residues in Raw Milk by UPLC-MS/MS, Food Chemistry, 181, pp. 119-126.   DOI