Abstract
Currently, there is increasing awareness regarding the effect of antibiotics on various organisms in the ecosystem even though they may occur at relatively low concentration. Thus, their concentration needs to be quantified precisely in various matrices including ground water, surface water, and municipal wastewater. The use of liquid chromatography together with high-resolution mass spectrometry (HR-LC-MS/MS) has enhanced the reliability, accessibility, and accuracy with which antibiotics can be detected. In the present study, a HR-LC-MS/MS-based method was developed for four antibiotics (ciprofloxacin, norfloxacin, azithromycin, and sulfamethoxazole). Initially, various mobile phases and LC columns were evaluated. The effect of solution pH, drying time of cartridge, and solvent used in the concentration step on recovery of antibiotics during solid-phase extraction (SPE) was also evaluated. Subsequently, the recovery of antibiotics from influent and effluent wastewater samples, obtained from a wastewater treatment plant (WWTP) in India, was determined based on the matrix spike method. The results revealed that for these wastewater samples even the use of structurally similar, isotopically labelled (deuterated) standards could not adequately improve the recovery of target antibiotics.
This is a preview of subscription content, log in via an institution to check access.
Access this chapter
Tax calculation will be finalised at checkout
Purchases are for personal use only
References
Annesley TM (2003) Ion suppression in mass spectrometry. Clin Chem 49:1041–1044. https://doi.org/10.1373/49.7.1041
Balakrishna K, Rath A, Praveenkumarreddy Y, Guruge KS, Subedi B (2016) A review of the occurrence of pharmaceuticals and personal care products in Indian water bodies. Ecotoxicol Environ Saf 137:113–120. https://doi.org/10.1016/j.ecoenv.2016.11.014
Berridge JC (1985) Techniques for the automated optimization of HPLC separation. Wiley
Bevan R, Harrison P, Youngs L, Whelan M, Goslan E, Macadam J, Holmes P, Persich T (2012) A review of latest endocrine disrupting chemicals research implications for drinking water. Institute of Environment and Health (IEH), UK
Bonfiglio R, Bonfiglio R, King R, King R, Olah T, Olah T, Merkle K, Merkle K (1999) The effects of sample preparation methods on the variability of the electrospray ionization response for model drug compounds. Rapid Commun Mass Spectrom 13:1175–1185. https://doi.org/10.1002/(SICI)1097-0231(19990630)13:12<1175:AID-RCM639>3.0.CO;2-0
Comero S, Loos R, Carvalho R, Anto DC, Locoro G, Tavazzi S, Paracchini B, Ghiani M, Lettieri T, Blaha L, Jarosova B, Voorspoels S, Servaes K, Haglund P, Fick J, Lindberg RH, Schwesig D, Gawlik BM, António DC, Comero S, Locoro G, Tavazzi S, Paracchini B, Ghiani M, Lettieri T, Blaha L, Jarosova B, Voorspoels S, Servaes K, Haglund P, Fick J, Lindberg RH, Schwesig D, Gawlik BM (2013) EU-wide monitoring survey on emerging polar organic contaminants in wastewater treatment plant effluents. Water Res 47:6475–6487. https://doi.org/10.1016/j.watres.2013.08.024
Diwan V, Tamhankar AJ, Khandal RK, Sen S, Aggarwal M, Marothi Y, Iyer RV, Sundblad-Tonderski K, Stålsby-Lundborg C (2010) Antibiotics and antibiotic-resistant bacteria in waters associated with a hospital in Ujjain, India. BMC Public Health 10:1–8. https://doi.org/10.1186/1471-2458-10-414
EPA (2007) Method 1694: pharmaceuticals and personal care products in water soil, sediment, and biosolids by HPLC/MS/MS. EPA Method. https://doi.org/10.1002/etc.3451
Gómez MJ, Petrović M, Fernández-Alba AR, Barceló D (2006) Determination of pharmaceuticals of various therapeutic classes by solid-phase extraction and liquid chromatography-tandem mass spectrometry analysis in hospital effluent wastewaters. J Chromatogr A 1114:224–233. https://doi.org/10.1016/j.chroma.2006.02.038
Gros M, Petrović M, Barceló D (2006) Development of a multi-residue analytical methodology based on liquid chromatography-tandem mass spectrometry (LC-MS/MS) for screening and trace level determination of pharmaceuticals in surface and wastewaters. Talanta 70:678–690. https://doi.org/10.1016/j.talanta.2006.05.024
Gros M, RodrÃguez-Mozaz S, Barceló 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. J Chromatogr A 1292:173–188. https://doi:10.1016/j.chroma.2012.12.072
Hernandez-Ruiz S, Abrell L, Wickramasekara S, Chefetz B, Chorover J (2012) Quantifying PPCP interaction with dissolved organic matter in aqueous solution: combined use of fluorescence quenching and tandem mass spectrometry. Water Res 46:943–954. https://doi.org/10.1016/j.watres.2011.11.061
Huber MM, Göbel A, Joss A, Hermann N, Löffler D, McArdell CS, Ried A, Siegrist H, Ternes TA, Von Gunten U (2005) Oxidation of pharmaceuticals during ozonation of municipal wastewater effluents: a pilot study. Environ Sci Technol 39:4290–4299. https://doi.org/10.1021/es048396s
ICH (1994) Validation of analytical procedures: text and methodology Q2(R1) [WWW Document]. Int Conf Harmon. https://www.ich.org/fileadmin/Public_Web_Site/ICH_Products/Guidelines/Quality/Q2_R1/Step4/Q2_R1__Guideline.pdf. Accessed on 9th Aug 2017
Karthikeyan KG, Meyer MT (2006) Occurrence of antibiotics in wastewater treatment facilities in Wisconsin, USA. Sci Total Environ 361:196–207. https://doi.org/10.1016/j.scitotenv.2005.06.030
Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ (2008) The effect of signal suppression and mobile phase composition on the simultaneous analysis of multiple classes of acidic/neutral pharmaceuticals and personal care products in surface water by solid-phase extraction and ultra performance liquid chromatogra. Talanta 74:1299–1312. https://doi.org/10.1016/j.talanta.2007.08.037
Kasprzyk-Hordern B, Dinsdale RM, Guwy AJ (2007) Multi-residue method for the determination of basic/neutral pharmaceuticals and illicit drugs in surface water by solid-phase extraction and ultra performance liquid chromatography-positive electrospray ionisation tandem mass spectrometry. J Chromatogr A 1161:132–145. doi:10.1016/j.chroma.2007.05.074
King R, Bonfiglio R, Fernandez-Metzler C, Miller-Stein C, Olah T (2000) Mechanistic investigation of ionization supression in electrospray ionization. J Am Soc Mass Spectrom 11:942–950. https://doi.org/10.1016/S1044-0305(00)00163-X
Lacey C, McMahon G, Bones J, Barron L, Morrissey A, Tobin, JM (2008) An LC-MS method for the determination of pharmaceutical compounds in wastewater treatment plant influent and effluent samples. Talanta 75:1089–1097. doi:10.1016/j.talanta.2008.01.011
Lin AY-CC, Tsai Y-TT (2009) Occurrence of pharmaceuticals in Taiwan’s surface waters: impact of waste streams from hospitals and pharmaceutical production facilities. Sci Total Environ 407:3793–3802. https://doi.org/10.1016/j.scitotenv.2009.03.009
Liu R, Zhou J, Wilding A (2004) Simultaneous determination of endocrine disrupting phenolic compounds and steroids in water by solid-phase extraction–gas chromatography–mass spectrometry. J Chromatogr A 1022:179–189. doi:10.1016/j.chroma.2003.09.035
Mallet CR, Lu Z, Mazzeo JR (2004) A study of ion suppression effects in electrospray ionization from mobile phase additives and solid-phase extracts. Rapid Commun Mass Spectrom 18:49–58. https://doi.org/10.1002/rcm.1276
Matuszewski BK, Constanzer ML, Chavez-Eng CM (2003) Strategies for the assessment of matrix effect in quantitative bioanalytical methods based on HPLC-MS/MS. Anal Chem 75:3019–3030. https://doi.org/10.1021/ac020361s
Mohapatra S, Huang C-H, Mukherji S, Padhye LP (2016) Occurrence and fate of pharmaceuticals in WWTPs in India and comparison with a similar study in the United States. Chemosphere 159:526–535. https://doi.org/10.1016/j.chemosphere.2016.06.047
Mutavdžić Pavlovic D, Pinušić T, Periša M, Babić S (2012) Optimization of matrix solid-phase dispersion for liquid chromatography tandem mass spectrometry analysis of 12 pharmaceuticals in sediments. J Chromatogr A 1258:1–15. https://doi.org/10.1016/j.chroma.2012.08.025
Nelson ED, Do H, Lewis RS, Carr SA (2011) Diurnal variability of pharmaceutical, personal care product, estrogen and alkylphenol concentrations in effluent from a tertiary wastewater treatment facility. Environ Sci Technol 45:1228–1234. doi:10.1021/es102452f
Oaks JL, Gilbert M, Virani MZ, Watson RT, Meteyer CU, Rideout BA, Shivaprasad HL, Ahmed S, Chaudhry MJI, Arshad M, Mahmood S, Ali A, Khan AA (2004) Diclofenac residues as the cause of vulture population decline in Pakistan. Nature 427:630–633. https://doi.org/10.1038/nature02317
Padhye LP, Yao H, Kung’u FT, Huang C-H (2014) Year-long evaluation on the occurrence and fate of pharmaceuticals, personal care products, and endocrine disrupting chemicals in an urban drinking water treatment plant. Water Res 51:266–276. doi:10.1016/j.watres.2013.10.070
Pan B, Ning P, Xing B (2009) Part V-Sorption of pharmaceuticals and personal care products. Environ Sci Pollut Res Int 16:106–116. https://doi.org/10.1007/s11356-008-0052-x
Park J, Yamashita N, Park C, Shimono T, Takeuchi DM, Tanaka H (2017) Removal characteristics of pharmaceuticals and personal care products: comparison between membrane bioreactor and various biological treatment processes. Chemosphere 179:347–358. https://doi.org/10.1016/j.chemosphere.2017.03.135
Sterner J, Johnston M, Nicol G, Ridge D (2000) Signal suppression in electrospray ionization Fourier transform mass spectrometry of multi-component samples. J Mass Spectrom 35:385–391. https://doi.org/10.1002/(SICI)1096-9888(200003)35:3<385:AID-JMS947>3.0.CO;2-O
Sun Q, Li M, Ma C, Chen X, Xie X, Yu CP (2016) Seasonal and spatial variations of PPCP occurrence, removal and mass loading in three wastewater treatment plants located in different urbanization areas in Xiamen, China. Environ Pollut 208:371–381. https://doi.org/10.1016/j.envpol.2015.10.003
Ternes TA (1998) Occurrence of drugs in german sewage treatment plants and rivers. Water Res 32:3245–3260. https://doi.org/10.1016/S0043-1354(98)00099-2
Tolls J (2001) Sorption of veterinary pharmaceuticals in soils: a review. Environ Sci Technol 35:3397–3406. https://doi.org/10.1021/es0003021
Van Boeckel TP, Gandra S, Ashok A, Caudron Q, Grenfell BT, Levin SA, Laxminarayan R (2014) Global antibiotic consumption 2000 to 2010: an analysis of national pharmaceutical sales data. Lancet Infect Dis 14:742–750. doi:10.1016/S1473-3099(14)70780-7
Vanderford BJ, Pearson RA, Rexing DJ, Snyder SA (2003) Analysis of endocrine disruptors, pharmaceuticals, and personal care products in water using liquid chromatography/tandem mass spectrometry. Anal Chem 75:6265–6274. doi:10.1021/ac034210g
Watkinson AJ, Murby EJ, Costanzo SD (2007) Removal of antibiotics in conventional and advanced wastewater treatment: implications for environmental discharge and wastewater recycling. Water Res 41:4164–4176. doi:10.1016/j.watres.2007.04.005
Weigel S, Kallenborn R, Hühnerfuss H (2004) Simultaneous solid-phase extraction of acidic, neutral and basic pharmaceuticals from aqueous samples at ambient (neutral) pH and their determination by gas chromatography-mass spectrometry. J Chromatogr A 1023:183–195. https://doi.org/10.1016/j.chroma.2003.10.036
Xu W, Zhang G, Li X, Zou S, Li P, Hu Z, Li J (2007) Occurrence and elimination of antibiotics at four sewage treatment plants in the Pearl River Delta (PRD), South China. Water Res 41:4526–4534. https://doi.org/10.1016/j.watres.2007.06.023
Zhang ZL, Zhou JL (2007) Simultaneous determination of various pharmaceutical compounds in water by solid-phase extraction-liquid chromatography-tandem mass spectrometry. J Chromatogr A 1154:205–213. https://doi.org/10.1016/j.chroma.2007.03.105
Zorita S, Mårtensson L, Mathiasson L (2009) Occurrence and removal of pharmaceuticals in a municipal sewage treatment system in the south of Sweden. Sci Total Environ 407:2760–2770. https://doi.org/10.1016/j.scitotenv.2008.12.030
Acknowledgements
We acknowledge IRCC, IIT Bombay, for providing partial financial support. The LC-MS/MS facility in Sophisticated Analytical Instrument Facility (SAIF), IIT Bombay, was used for analysis of the antibiotics. Department of Science and Technology (DST), New Delhi, is acknowledged for providing INSIPRE fellowship to Sanjeeb Mohapatra.
Author information
Authors and Affiliations
Corresponding author
Editor information
Editors and Affiliations
Rights and permissions
Copyright information
© 2018 Springer Nature Singapore Pte Ltd.
About this chapter
Cite this chapter
Mohapatra, S., Padhye, L.P., Mukherji, S. (2018). Challenges in Detection of Antibiotics in Wastewater Matrix. In: Gupta, T., Agarwal, A., Agarwal, R., Labhsetwar, N. (eds) Environmental Contaminants. Energy, Environment, and Sustainability. Springer, Singapore. https://doi.org/10.1007/978-981-10-7332-8_1
Download citation
DOI: https://doi.org/10.1007/978-981-10-7332-8_1
Published:
Publisher Name: Springer, Singapore
Print ISBN: 978-981-10-7331-1
Online ISBN: 978-981-10-7332-8
eBook Packages: Earth and Environmental ScienceEarth and Environmental Science (R0)