journal article Open Access Dec 10, 2018

Caffeine vs. carbamazepine as indicators of wastewater pollution in a karst aquifer

View at Publisher Save 10.5194/hess-22-6371-2018
Abstract
Abstract. This paper presents the analysis of caffeine and carbamazepine
transport in the subsurface as a result of wastewater release in the Sorek
creek over the outcrops of the carbonate, Yarkon-Taninim, aquifer in Israel.
Both caffeine and carbamazepine were used as indicators of sewage
contamination in the subsurface. While carbamazepine is considered
conservative, caffeine is subject to sorption and degradation. The objective
of the study was to quantify differences in their transport under similar
conditions in the karst aquifer. Water flow and pollutant transport in a
“vadose zone–aquifer” system were simulated by a quasi-3-D dual
permeability numerical model. The results of this study show that each of
these two pollutants can be considered effective tracers for characterization
and assessment of aquifer contamination. Carbamazepine was found to be more
suitable for assessing the contamination boundaries, while caffeine can be
used as a contaminant tracer only briefly after contamination occurs. In
instances where there are low concentrations of carbamazepine which appear as
background contamination in an aquifer, caffeine might serve as a better
marker for detecting new contamination events, given its temporal nature. The
estimated caffeine degradation rate and the distribution coefficient of a
linear sorption isotherm were 0.091 d−1 and
0.1 L kg−1, respectively, which imply a
high attenuation capacity. The results of the simulation indicate that by the
end of the year most of the carbamazepine mass (approximately 95 %)
remained in the matrix of the vadose zone, while all of the caffeine was
completely degraded a few months after the sewage was discharged.
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References
49
[1]
Ahmed, W., Goonetilleke, A., and Gardner, T.: Detection and quantification of faecal pollution in environmental waters using alternative Faecal indicators: A Brief Review, Water, 39, 46–49, 2008.
[2]
Arye, G., Dror, I., and Berkowitz, B.: Fate and transport of carbamazepine in soil aquifer treatment (SAT) infiltration basin soils, Chemosphere, 82, 244–252, https://doi.org/10.1016/j.chemosphere.2010.09.062, 2011. 10.1016/j.chemosphere.2010.09.062
[3]
Sorption and biodegradation of organic micropollutants during river bank filtration: A laboratory column study

C. Bertelkamp, J. Reungoat, E.R. Cornelissen et al.

Water Research 10.1016/j.watres.2013.10.068
[4]
Bradley, P. M., Barber, L. B., Kolpin, D. W., McMahon, P. B., and Chapelle, F. H.: Biotransformation of Caffeine, Cotinine, and Nicotine in sream sediments: Implications for use as wastewater indicators, Environ. Toxicol. Chem., 26, 1116, https://doi.org/10.1897/06-483R.1, 2007. 10.1897/06-483r.1
[5]
Bueno, M. J. M., Hernando, M. D., Herrera, S., Gómez, M. J., Fernández-Alba, A. R., Bustamante, I., and García-Calvo, E.: Pilot survey of chemical contaminants from industrial and human activities in river waters of spain, Int. J. Environ. An. Chem., 90, 321–343, https://doi.org/10.1080/03067310903045463, 2010. 10.1080/03067310903045463
[6]
Buerge, I. J., Poiger, T., Müller, M. D., and Buser, H.-R.: Caffeine, an Anthropogenic Marker for Wastewater Contamination of Surface Waters, Environ. Sci. Technol., 37, 691–700, https://doi.org/10.1021/es020125z, 2003. 10.1021/es020125z
[7]
Chen, M., Ohman, K., Metcalfe, C., Ikonomou, M. G., Amatya, P. L., and Wilson, J.: Pharmaceuticals and endocrine disruptors in wastewater treatment effluents and in the water supply system of Calgary, Alberta, Canada, Water Qual. Res. J. Can., 41, 351–364, 2006. 10.2166/wqrj.2006.039
[9]
Conn, K. E. and Siegrist, R. L.: Occurrence and fate of trace organic contaminants in onsite wastewater treatment systems and implications for water quality management, Completion Rep no. 210, (Colorado State Universyty), available at: https://mountainscholar.org/bitstream/handle/10217/69222/CR_210.pdf?sequence=1 (last access: 6 December 2018), 2009.
[10]
Dafny, E., Burg, A. and Gvirtzman, H.: Effects of Karst and geological structure on groundwater flow: The case of Yarqon-Taninim Aquifer, Israel, J. Hydrol., 389, 260–275, https://doi.org/10.1016/j.jhydrol.2010.05.038, 2010. 10.1016/j.jhydrol.2010.05.038
[11]
Doherty, J.: PEST: Model independent parameter estimation, Fifth edition, user manual, Watermark Numer. Comput., https://doi.org/10.1016/B978-0-08-098288-5.00031-2, 2004. 10.1016/b978-0-08-098288-5.00031-2
[12]
Dvory, N. Z., Livshitz, Y., Kuznetsov, M., Adar, E., and Yakirevich, A.: The effect of hydrogeological conditions on variability and dynamic of groundwater recharge in a carbonate aquifer at local scale, J. Hydrol., 535, 480–494, https://doi.org/10.1016/j.jhydrol.2016.02.011, 2016. 10.1016/j.jhydrol.2016.02.011
[13]
Dvory, N. Z., Kuznetsov, M., Livshitz, Y., Gasser, G., Pankratov, I., Lev, O., Adar, E., and Yakirevich, A.: Modeling sewage leakage and transport in carbonate aquifer using carbamazepine as an indicator, Water Res., 128, 157–170, https://doi.org/10.1016/j.watres.2017.10.044, 2018a. 10.1016/j.watres.2017.10.044
[14]
Dvory, N. Z., Ronen, A., Livshitz, Y., Adar, E., Kuznetsov, M., and Yakirevich, A.: Quantification of groundwater recharge from an ephemeral stream into a Mountainous karst aquifer, Water, 10, 1–16, https://doi.org/10.3390/w10010079, 2018b. 10.3390/w10010079
[15]
Fenz, R., Blaschke, A. P., Clara, M., Kroiss, H., Mascher, D., and Zessner, M.: Quantification of sewer exfiltration using the anti-epileptic drug carbamazepine as marker species for wastewater, Water Sci. Technol., 52, 209–217, https://doi.org/10.2166/wst.2005.0321, 2005. 10.2166/wst.2005.0321
[16]
Ferrer, I. and Thurmann, E. M.: EPA Method 1694: Agilent's 6410A LC/MS/MS Solution for pharmaceuticals and personal care products in water, soil, sediment, and biosolids by HPLC/MS/MS Application Note, Group, 12, 2008.
[17]
Ferreira, A. P.: Caffeine as an environmental indicator for assessing urban aquatic ecosystems, Cad. Saúde Pública, Río Janeiro, 21, 1884–1892, https://doi.org/10.1590/S0102-311X2005000600038, 2005. 10.1590/s0102-311x2005000600038
[18]
Gardinali, P. R. and Zhao, X.: Trace determination of caffeine in surface water samples by liquid chromatography–atmospheric pressure chemical ionization–mass spectrometry (LC–APCI–MS), Environ. Int, 28, 521–528, 2002. 10.1016/s0160-4120(02)00080-6
[19]
Gasser, G., Rona, M., Voloshenko, A., Shelkov, R., Tal, N., Pankratov, I., Elhanany, S., and Lev, O.: Quantitative evaluation of tracers for quantification of wastewater contamination of potable water sources, Environ. Sci. Technol., 44, 3919–3925, https://doi.org/10.1021/es100604c, 2010. 10.1021/es100604c
[20]
Gerke, H. H. and van Genuchten, M. T.: A dual-porosity model for simulating the preferential movement of water and solutes in structured porous media, Water Resour. Res., 29, 305–319, https://doi.org/10.1029/92WR02339, 1993. 10.1029/92wr02339
[21]
Geyer, T., Birk, S., Licha, T., Liedl, R., and Sauter, M.: Multitracer test approach to characterize reactive transport in karst aquifers, Ground Water, 45, 36–45, https://doi.org/10.1111/j.1745-6584.2006.00261.x, 2007. 10.1111/j.1745-6584.2006.00261.x
[22]
GMS 6.0: Groundwater modeling system, Brigham Young University, 2002.
[23]
Godfrey, E., Woessner, W. W., and Benotti, M. J.: Pharmaceuticals in on-site sewage effluent and ground water, Western Montana, Ground Water, 45, 263–271, https://doi.org/10.1111/j.1745-6584.2006.00288.x, 2007. 10.1111/j.1745-6584.2006.00288.x
[24]
Harbaugh, B. A. W., Banta, E. R., Hill, M. C., and Mcdonald, M. G.: MODFLOW-2000, The U.S. Geological Survey modular graound-water model – User guide to modularization concepts and the ground-water flow process, U.S. Geol. Surv., 130, available at: https://pubs.usgs.gov/of/2000/0092/report.pdf (last access: 6 December 2018), 121 pp., 2000. 10.3133/ofr200092
[25]
Hebig, K. H., Groza, L. G., Sabourin, M. J., Scheytt, T. J., and Ptacek, C. J.: Transport behavior of the pharmaceutical compounds carbamazepine, sulfamethoxazole, gemfibrozil, ibuprofen, and naproxen, and the lifestyle drug caffeine, in saturated laboratory columns, Sci. Total Environ., 590–591, 708–719, https://doi.org/10.1016/j.scitotenv.2017.03.031, 2017. 10.1016/j.scitotenv.2017.03.031
[26]
Hillebrand, O., Nödler, K., Licha, T., Sauter, M., and Geyer, T.: Caffeine as an indicator for the quantification of untreated wastewater in karst systems, Water Res., 46, 395–402, https://doi.org/10.1016/j.watres.2011.11.003, 2012a. 10.1016/j.watres.2011.11.003
[27]
Hillebrand, O., Nödler, K., Licha, T., Sauter, M., and Geyer, T.: Identification of the attenuation potential of a karst aquifer by an artificial dualtracer experiment with caffeine, Water Res., 46, 5381–5388, https://doi.org/10.1016/j.watres.2012.07.032, 2012b. 10.1016/j.watres.2012.07.032
[28]
Hillebrand, O., Nödler, K., Sauter, M., and Licha, T.: Multitracer experiment to evaluate the attenuation of selected organic micropollutants in a karst aquifer, Sci. Total Environ., 506–507, 338–343, https://doi.org/10.1016/j.scitotenv.2014.10.102, 2015. 10.1016/j.scitotenv.2014.10.102
[29]
Klabunde, C. T.: Potential impacts on groundwater quality in a fractured sedimentary bedrock aquifer from biosolids application on agricultural fields, 2016.
[30]
Knee, K. L., Gossett, R., Boehm, A. B., and Paytan, A.: Caffeine and agricultural pesticide concentrations in surface water and groundwater on the north shore of Kauai (Hawaii, USA), Mar. Pollut. Bull., 60, 1376–1382, https://doi.org/10.1016/j.marpolbul.2010.04.019, 2010. 10.1016/j.marpolbul.2010.04.019
[31]
Kolpin, D. W., Skopec, M., Meyer, M. T., Furlong, E. T., and Zaugg, S. D.: Urban contribution of pharmaceuticals and other organic wastewater contaminants to streams during differing flow conditions, Sci. Total Environ., 328, 119–130, https://doi.org/10.1016/j.scitotenv.2004.01.015, 2004. 10.1016/j.scitotenv.2004.01.015
[32]
Kuznetsov, M., Yakirevich, A., Pachepsky, Y. A., Sorek, S., and Weisbrod, N.: Quasi 3D modeling of water flow in vadose zone and groundwater, J. Hydrol., 450–451, 140–149, https://doi.org/10.1016/j.jhydrol.2012.05.025, 2012. 10.1016/j.jhydrol.2012.05.025
[33]
Lapworth, D. J., Baran, N., Stuart, M. E., Manamsa, K., and Talbot, J.: Persistent and emerging micro-organic contaminants in Chalk groundwater of England and France, Environ. Pollut., 203, 214–225, https://doi.org/10.1016/j.envpol.2015.02.030, 2015. 10.1016/j.envpol.2015.02.030
[34]
Levy, Y., Shapira, R. H., Chefetz, B., and Kurtzman, D.: Modeling nitrate from land surface to wells' perforations under agricultural land: success, failure, and future scenarios in a Mediterranean case study, Hydrol. Earth Syst. Sci., 21, 3811–3825, https://doi.org/10.5194/hess-21-3811-2017, 2017. 10.5194/hess-21-3811-2017
[35]
Lin, A. Y. C., Lin, C. A., Tung, H. H., and Chary, N. S.: Potential for biodegradation and sorption of acetaminophen, caffeine, propranolol and acebutolol in lab-scale aqueous environments, J. Hazard. Mater., 183, 242–250, https://doi.org/10.1016/j.jhazmat.2010.07.017, 2010. 10.1016/j.jhazmat.2010.07.017
[36]
Liu, Y., Blowes, D. W., Groza, L., Sabourin, M. J., and Ptacek, C. J.: Acesulfame-K and pharmaceuticals as co-tracers of municipal wastewater in a receiving river, Environ. Sci. Process. Impacts, 16, 2789–2795, https://doi.org/10.1039/C4EM00237G, 2014. 10.1039/c4em00237g
[37]
Manamsa, K., Lapworth, D. J., and Stuart, M. E.: Temporal variability of micro-organic contaminants in lowland chalk catchments: New insights into contaminant sources and hydrological processes, Sci. Total Environ., 568, 566–577, https://doi.org/10.1016/j.scitotenv.2016.01.146, 2015. 10.1016/j.scitotenv.2016.01.146
[38]
Martínez-Hernández, V., Meffe, R., Herrera López, S., and de Bustamante, I.: The role of sorption and biodegradation in the removal of acetaminophen, carbamazepine, caffeine, naproxen and sulfamethoxazole during soil contact: A kinetics study, Sci. Total Environ., 559, 232–241, https://doi.org/10.1016/j.scitotenv.2016.03.131, 2016. 10.1016/j.scitotenv.2016.03.131
[39]
Martínez-Hernández, V., Meffe, R., Kohfahl, C., and de Bustamante, I.: Investigating natural attenuation of pharmaceuticals through unsaturated column tests, Chemosphere, 177, 292–302, https://doi.org/10.1016/j.chemosphere.2017.03.021, 2017. 10.1016/j.chemosphere.2017.03.021
[40]
Metcalfe, C. D., Beddows, P. A., Bouchot, G. G., Metcalfe, T. L., Li, H., and Van Lavieren, H.: Contaminants in the coastal karst aquifer system along the Caribbean coast of the Yucatan Peninsula, Mexico, Environ. Pollut., 159, 991–997, https://doi.org/10.1016/j.envpol.2010.11.031, 2011. 10.1016/j.envpol.2010.11.031
[41]
Neuman, S. P.: Universal scaling of hydraulic conductivities and dispersivities in geologic media, Water Resour. Res., 26, 1749–1758, https://doi.org/10.1029/WR026i008p01749, 1990. 10.1029/wr026i008p01749
[42]
Regnery, J., Wing, A. D., Alidina, M., and Drewes, J. E.: Biotransformation of trace organic chemicals during groundwater recharge: How useful are first-order rate constants?, J. Contam. Hydrol., 179, 65–75, https://doi.org/10.1016/j.jconhyd.2015.05.008, 2015. 10.1016/j.jconhyd.2015.05.008
[43]
Seiler, R. L., Zaugg, S. D., Thomas, J. M., and Howcrof, D. L.: Caffeine and Pharmaceuticals as Indicators of Waste Water Contamination in Wells, Groundwater, 37, 405–410, https://doi.org/10.1111/j.1745-6584.1999.tb01118.x, 1999. 10.1111/j.1745-6584.1999.tb01118.x
[44]
Swartz, C. H., Reddy, S., Benotti, M. J., Yin, H., Barber, L. B., Brownawell, B. J., and Rudel, R. A.: Steroid estrogens, nonylphenol ethoxylate metabolites, and other wastewater contaminants in groundwater affected by a residential septic system on Cape Cod, MA, Environ. Sci. Technol., 40, 4894–4902, https://doi.org/10.1021/es052595+, 2006. 10.1021/es052595+
[45]
Schwarzenbach, R. P., Gschwend, P. M., and Imboden, D. M.: Environmental Organic Chemistry, John Wiley & Sons, 681 pp., 1993.
[46]
Twarakavi, N. K. C., Šimůnek, J., and Seo, S.: Evaluating Interactions between Groundwater and Vadose Zone Using the HYDRUS-Based Flow Package for MODFLOW, Vadose Zone J., 7, 757, https://doi.org/10.2136/vzj2007.0082, 2008. 10.2136/vzj2007.0082
[47]
Yakirevich, A., Borisov, V., and Sorek, S.: A quasi three-dimensional model for flow and transport in unsaturated and saturated zones: 1. Implementation of the quasi two-dimensional case, Adv. Water Resour., 21, 679–689, https://doi.org/10.1016/S0309-1708(97)00031-6, 1998. 10.1016/s0309-1708(97)00031-6
[48]
Zhang, T., Wu, B., Sun, N., Ye, Y., and Chen, H.: Sorption and degradation of wastewater-associated pharmaceuticals and personal care products in agricultural soils and sediment, Water Sci. Technol., 68, 991–998, https://doi.org/10.2166/wst.2013.326, 2013. 10.2166/wst.2013.326
[49]
Zheng, C. and Wang, P. P.: MT3DMS: A Modular three-dimensional multispecies transport model, (December), 219, 1999.