Laboratory investigations of diclofenac migration in saturated porous media – a case study
PDF

Keywords

non-steroidal anti-inflammatory drug
column test
parameter estimation
optimisation method
MATLAB

How to Cite

Okońska, M., Marciniak, M., Zembrzuska, J., & Kaczmarek, M. (2019). Laboratory investigations of diclofenac migration in saturated porous media – a case study. Geologos, 25(3), 213–223. https://doi.org/10.2478/logos-2019-0023

Abstract

At present, concentrations of pharmaceuticals in surface and ground waters are low; however, even low concentrations of certain substances may prove very harmful. One of such pharmaceutical drugs is diclofenac, a popular non-steroidal anti-inflammatory drug (NSAID). For this reason, it is important to determine its mobility in groundwater and to estimate parameters of migration. Authors conducted column tests for two porous media: an artificial one, consisting of glass granules, and a natural one, i.e., sandur sand obtained from a site north of the city of Poznań (Poland). During the test, impulse breakthrough curves of chloride ions and diclofenac were recorded. The results were used to identify a specific sorption model and to determine values of migration parameters. Solutions of the inverse problem using optimisation methods and of equations of mathematical migration models were carried out in a MATLAB environment. Based on test results, the mobility of diclofenac is shown to be very high and comparable to that of chloride ions. The tests also revealed a slight and irreversible sorption of diclofenac on grains of both porous media.

https://doi.org/10.2478/logos-2019-0023
PDF

References

Acuna, V., Ginebreda, A., Mor, J.R., Petrovic, M., Sabater, S., Sumpter, J. & Barceló, D., 2015. Balancing the health benefits and environmental risks of pharmaceuticals: Diclofenac as an example. Environment International 85, 327–333.

Arfe, A., Scotti, L., Varas-Lorenzo, C., Nicotra, F., Zambon, A., Kollhorst, B., Schink, T., Garbe, E., Herings, R., Straatman, H., Schade, R., Villa, M., Lucchi, S., Valkhoff, V., Romio, S., Thiessard, F., Schuemie, M., Pariente, A., Sturkenboom, M. & Corrao, G., 2016. Non-steroidal anti-inflammatory drugs and risk of heart failure in four European countries: nested case-control study. British Medical Journal 354, i4857.

Bertelkamp, C., Reungoat, J., Cornelissen, E.R., Singhal, N., Reynisson, J., Cabo, A.J., van der Hoek, J.P. & Verliefde, A.R.D., 2014. Sorption and biodegradation of organic micropollutants during river bank filtration: A laboratory column study. Water Research 52, 231–241.

Bohdziewicz, J., Kudlek, E. & Dudziak, M., 2016. Influence of the catalyst type (TiO2 and ZnO) on the photocatalytic oxidation of pharmaceuticals in the aquatic environment. Desalination and Water Treatment 57, 1552–1563.

Caban, M., Lis, E., Kumirska, J. & Stepnowski, P., 2015. Determination of pharmaceutical residues in drinking water in Poland using a new SPE-GC-MS (SIM) method based on Speedisk extraction disks and DIMETRIS derivatization. Science of the Total Environment 538, 402–411.

Caracciolo, A.B., Topp, E. & Grenni, P., 2015. Pharmaceuticals in the environment: Biodegradation and effects on natural microbial communities. A review. Journal of Pharmaceutical and Biomedical Analysis 106, 25–36.

Czech, B., 2012. Usuwanie farmaceutyków z wód i ścieków z wykorzystaniem metod adsorpcyjnych i fotokatalitycznych [Removal of pharmaceuticals from water and sewage by applying adsorption and photocatalytic methods]. [In:] J. Ryczkowski (Ed.): Adsorbenty i katalizatory – Wybrane technologie a środowisko [Adsorbents and Catalysts – Selected Technologies and the Environment]. Uniwersytet Rzeszowski, Rzeszów, 443–452.

Drozdek, E., Żyłła, R., Gmurek, M., Milala, R. & Ledakowicz, S., 2018. Usuwanie trudno biodegradowalnych farmaceutyków zintegrowanymi metodami pogłębionego utleniania i filtracji membranowej [Removal of difficult biodegradable pharmaceuticals with integrated methods of advanced oxidation and membrane filtration]. Acta Scientiarum Polonorum Biotechnologia 17, 5–14.

Dux, S., Groslop, I., Garty, M. & Rosenfeld, J.B., 1983. Anaphylactic shock induced by diclofenac. British Medical Journal 286, 1861.

ECHA, 2018. Diclofenac (EC no. 239-348-5). European Chemicals Agency. [Online] Access: http://echa.europa.eu/, March 5, 2019.

EU, 2011. COM 875: Report from the Commission to the European Parliament and the Council on the outcome of the review of Annex X to Directive 2000/60/EC of the European Parliament and of the Council on priority substances in the field of water policy. [Online] Access: http://ec.europa.eu/environment/water/water-dangersub/, March 11, 2019.

EU, 2013. Directive 2013/39/EU of the European Parliament and of the Council of 12 August 2013 amending Directives 2000/60/EC and 2008/105/EC as regards priority substances in the field of water policy. Official Journal of the European Union L 226. [Online] Access: http://data.europa.eu/eli/dir/2013/39/oj, March 11, 2019.

Groning, J., Held, C., Garten, C., Claußnitzer, U., Kaschabek, S.R. & Schlomann, M., 2007. Transformation of diclofenac by the indigenous microflora of river sediments and identification of a major intermediate. Chemosphere 69, 509–516.

Guzik, U., Hupert-Kocurek, K., Mazur, A. & Wojcieszyńska, D., 2013. Biotransformacja wybranych niesteroidowych leków przeciwzapalnych w środowisku [Biotransformation of non-steroidal anti-inflammatory drugs in environment]. Bromatologia i Chemia Toksykologiczna 46, 105–112.

Li, W.C., 2014. Occurrence, sources, and fate of pharmaceuticals in aquatic environment and soil. Environmental Pollution 187, 193–201.

Lin, K. & Gan, J., 2011. Sorption and degradation of wastewater-associated non-steroidal anti-inflammatory drugs and antibiotics in soils. Chemosphere 83, 240–246.

Kasprzyk-Hordern, B., Dąbrowska, A., Vieno, N., Kronberg, L. & Nawrocki, J., 2008. Occurrence of acidic pharmaceuticals in the Warta River in Poland. Chemia Analityczna 53, 289–303.

Kleczkowski, A.S. (Ed.), 1984. Ochrona wód podziemnych [Protection of groundwater]. Wydawnictwa Geologiczne, Warszawa, 328 pp.

Knights, K.M., Winner, L.K., Elliot, D.J., Bowalgaha, K. & Miners, J.O., 2009. Aldosterone glucuronidation by human liver and kidney microsomes and recombinant UDP-glucuronosyltransferases: Inhibition by NSAIDs. British Journal of Clinical Pharmacology 68, 402–412.

Kreft, A. & Zuber, A., 1978. On the physical meaning of the dispersion equation and its solutions for different initial and boundary conditions. Chemical Engineering Science 33, 1471–1480.

Kret, E., Kiecak, A., Malina, G., Nijenhuis, I. & Postawa, A., 2015. Identification of TCE and PCE sorption and biodegradation parameters in a sandy aquifer for fate and transport modelling: batch and column studies. Environmental Science and Pollution Research 22, 9877–9888.

Kuczyńska, A., 2017. Wyniki pilotażowego badania zawartości substancji czynnych farmaceutyków w wodach podziemnych w próbkach wody pobranych z krajowej sieci monitoringu wód podziemnych [Results of a pilot study on the assessment of pharmaceuticals in groundwater in samples collected from the national groundwater monitoring network]. Przegląd Geologiczny 65, 1096–1103.

Kudlek, E., Dudziak, M. & Bohdziewicz, J., 2016. Influence of inorganic ions and organic substances on the degradation of pharmaceutical compound in water matrix. Water 8, 532.

Lahti, M. & Oikari, A., 2011. Microbial transformation of pharmaceuticals naproxen, bisoprolol, and diclofenac in aerobic and anaerobic environments. Archives of Environmental Contamination and Toxicology 61, 202–210.

Larsson, E., Rabayah, A. & Jönsson, J.A., 2013. Sludge removal of nonsteroidal anti-inflammatory drugs during wastewater treatment studied by direct hollow fiber liquid phase microextraction. Journal of Environmental Protection 4, 946–955.

Lonappan, L., Brar, S.K., Das, R.K., Verma, M. & Surampalli, R.Y., 2016. Diclofenac and its transformation products: Environmental occurrence and toxicity - A review. Environment International 96, 127–138.

Małecki, J.J., Nawalany, M., Witczak, S. & Gruszczyński, T., 2006. Wyznaczanie parametrów migracji zanieczyszczeń w ośrodku porowatym dla potrzeb badań hydrogeologicznych i ochrony środowiska. Poradnik metodyczny [Determination of pollutant migration parameters in a porous medium for hydrogeological and environmental protection research. Methodological guide]. Uniwersytet Warszawski, Warszawa, 249 pp.

Mersmann, P., Scheytt, T. & Heberer, T., 2002. Säulenversuche zum Transportverhalten von Arzneimittelwirkstoffen in der wassergesättigten Zone [Column experiments on the transport behavior of pharmaceutically active compounds in the saturated zone]. Acta Hydrochimica et Hydrobiologica 30, 1–10.

Myślińska, E., 1998. Laboratoryjne badania gruntów [Laboratory investigations of soils]. Wydawnictwo Naukowe PWN, Warszawa, 278 pp.

Okońska, M., 2006. Identyfikacja parametrów migracji zanieczyszczeń w porowatym ośrodku hydrogeologicznym metodą modelowania eksperymentu kolumnowego [The identification of pollutants migration parameters in a groundwater porous medium by the method of the column experiment modelling]. Geologos 9, Poznań, 97 pp.

Okońska, M. & Pietrewicz, K., 2018. Identification of a mathematical model and parameter estimation of erythromycin migration in two different porous media, based on column tests. Geologia Croatica 71, 47–53.

Okońska, M., Kaczmarek, M., Małoszewski, P. & Marciniak, M., 2017. The verification of the estimation of transport and sorption parameters in the MATLAB environment. A column test. Geology, Geophysics and Environment 43, 213–227.

Okońska, M., Marciniak, M. & Kaczmarek, M., 2019. The pulse descriptors in sensitivity studies of no sorption and single sorption column transport models. Journal of Porous Media 22, 563–582.

Parker, J.C. & van Genuchten, M.Th., 1984. Determining transport parameters from laboratory and field tracer experiments. Virginia Agricultural Experiment Station Bulletin 84, 1–97.

Rizzo, L., Fiorentino, A., Grassi, M., Attanasio, D. & Guida, M., 2015. Advanced treatment of urban wastewater by sand filtration and graphene adsorption for wastewater reuse: Effect on a mixture of pharmaceuticals and toxicity. Journal of Environmental Chemical Engineering 3, 122–128.

Santos, L.H.M.L.M., Araújoa, A.N., Fachini, A., Pena, A., Delerue-Matos, C. & Montenegro, M.C.B.S.M., 2010. Ecotoxicological aspects related to the presence of pharmaceuticals in the aquatic environment. Journal of Hazardous Materials 175, 45–95.

Soubrier, M., Rosenbaum, D., Tatar, Z., Lahayea, C., Dubost, J.-J. & Mathieu, S., 2013. Vascular effects of nonsteroidal antiinflammatory drugs. Joint Bone Spine 80, 358–362.

Scheytt, T., Mersmann, P., Leidig, M., Pekdeger, A. & Heberer, T., 2004. Transport of pharmaceutically active compounds in saturated laboratory columns. Ground Water 42, 767–773.

Serrano, D., Suarez, S., Lema, J.M. & Omil, F., 2001. Removal of persistent pharmaceutical micropollutants from sewage by addition of PAC in a sequential membrane bioreactor. Water Resources 45, 5323–5333.

Szymonik, A. & Lach, J., 2012. Zagrożenia środowiska wodnego obecnością środków farmaceutycznych [Pharmaceuticals – potential threats to water environment]. Inżynieria i Ochrona Środowiska 15, 249–263.

Siemens, J., Huschek, G., Walshe, G., Siebe, C., Kasteel, R., Wulf, S., Clemens, J. & Kaupenjohann, M., 2010. Transport of pharmaceuticals in columns of a waste-water-irrigated Mexican clay soil. Journal of Environmental Quality 39, 1201–1210.

Valcarcel, Y., Alonso, S.G., Rodriguez-Gil, J.L., Maroto, R.R., Gil, A. & Catala, M., 2011. Analysis of the presence of cardiovascular, analgesic, anti-inflammatory, antipyretic pharmaceuticals in river and drinking water of the Madrid Region of Spain. Chemosphere 82, 1062–1071.

WHO (World Health Organization), 2012. Pharmaceuticals in drinking-water. [Online] Access: http://www.who.int/water_sanitation_health/publications/2012/pharmaceuticals/en, March 2, 2018.

Wilga, J., 2008. Opracowanie metodyk oznaczania zawartości substancji farmaceutycznych w próbkach środowiskowych [Development of analytical methods for determining pharmaceutical substances in the environmental samples]. Politechnika Gdańska, Gdańsk, 121 pp. [Online] Access: http://pbc.gda.pl/Content/3850/phd_wilga.pdf, March 12, 2019.

Zając, A., 2017. Skuteczność usuwania wybranych niesteroidowych leków przeciwzapalnych ze ścieków metodą osadu czynnego [Efficiency of removing selected non-steroidal anti-inflammatory drugs from wastewater by activated sludge]. Politechnika Poznańska, Poznań, 189 pp.

Zając, A., Zembrzuska, J., Kruszelnicka, I. & Ginter-Kramarczyk, D., 2015. Sposoby usuwania produktów farmaceutycznych i ich metabolitów z wody i ścieków [Methods for removing pharmaceuticals and their metabolites from water and wastewater]. Przemysł Chemiczny 94, 76–80.

Zembrzuska, J., Ginter-Kramarczyk, D., Kruszelnicka, I. & Zając, A., 2016. Występowanie niesteroidowych leków przeciwbólowych w Wielkopolsce w ściekach komunalnych i przemysłowych i ich ekotoksykologiczna ocena ryzyka [Occurrence of non-steroidal antiinflammatory drugs in municipal wastewater and industrial wastewater of Wielkopolska and their ecotoxicological assessment]. [In:] Z. Dymaczewski, J. Jeż-Walkowiak & A. Urbaniak (Eds): Zaopatrzenie w wodę, jakość i ochrona wód [Water supply and water quality]. Polskie Zrzeszenie Inżynierów i Techników Sanitarnych, Poznań, 979–994.

Zwiener, C., 2007. Occurrence and analysis of pharmaceuticals and their transformation products in drinking water treatment. Analytical and Bioanalytical Chemistry 387, 1159–1162.