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Determination of Atrazine and Degradation Products in Luxembourgish Drinking Water: Origin and Fate of Potential Endocrine-Disrupting Pesticides T

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Determination of Atrazine and Degradation Products in Luxembourgish Drinking Water: Origin and Fate of Potential Endocrine-Disrupting Pesticides T This article was downloaded by: [CRP Gabriel Lippmann (Centre de Recherch] On: 05 January 2012, At: 04:44 Publisher: Taylor & Francis Informa Ltd Registered in England and Wales Registered Number: 1072954 Registered office: Mortimer House, 37-41 Mortimer Street, London W1T 3JH, UK Food Additives & Contaminants: Part A Publication details, including instructions for authors and subscription information: http://www.tandfonline.com/loi/tfac20 Determination of atrazine and degradation products in Luxembourgish drinking water: origin and fate of potential endocrine-disrupting pesticides T. Bohn a , E. Cocco a , L. Gourdol a , C. Guignard a & L. Hoffmann a a Centre de Recherche Public – Gabriel Lippmann, Department of Environment and Agro- Biotechnologies, 41, rue du Brill, L-4422 Belvaux, Luxembourg Available online: 27 Jun 2011 To cite this article: T. Bohn, E. Cocco, L. Gourdol, C. Guignard & L. Hoffmann (2011): Determination of atrazine and degradation products in Luxembourgish drinking water: origin and fate of potential endocrine-disrupting pesticides, Food Additives & Contaminants: Part A, 28:8, 1041-1054 To link to this article: http://dx.doi.org/10.1080/19440049.2011.580012 PLEASE SCROLL DOWN FOR ARTICLE Full terms and conditions of use: http://www.tandfonline.com/page/terms-and-conditions This article may be used for research, teaching, and private study purposes. Any substantial or systematic reproduction, redistribution, reselling, loan, sub-licensing, systematic supply, or distribution in any form to anyone is expressly forbidden. The publisher does not give any warranty express or implied or make any representation that the contents will be complete or accurate or up to date. The accuracy of any instructions, formulae, and drug doses should be independently verified with primary sources. The publisher shall not be liable for any loss, actions, claims, proceedings, demand, or costs or damages whatsoever or howsoever caused arising directly or indirectly in connection with or arising out of the use of this material. Food Additives and Contaminants Vol. 28, No. 8, August 2011, 1041–1054 Determination of atrazine and degradation products in Luxembourgish drinking water: origin and fate of potential endocrine-disrupting pesticides T. Bohn*, E. Cocco, L. Gourdol, C. Guignard and L. Hoffmann Centre de Recherche Public – Gabriel Lippmann, Department of Environment and Agro-Biotechnologies, 41, rue du Brill, L-4422 Belvaux, Luxembourg (Received 5 January 2011; final version received 5 April 2011) Several pesticides have been hypothesized to act as endocrine-disrupting compounds, exhibiting hormonal activity and perturbing normal physiological functions. Among these, especially s-triazine herbicides have received increased attention. Despite being banned in many countries, including the European Union, atrazine is still the world’s most widely used herbicide. Despite its discontinued use, considerable concentrations of atrazine and its degradation products, mainly desethylatrazine (DEA) and deisopropylatrazine (DIA), are still found in the environment, including drinking water sources. The aim of this investigation was to study concentrations of especially s-triazine herbicides and major degradation products in drinking water, including spring water, tap water and bottled water in Luxembourg. Spring water (2007/2008/2009, n ¼ 69/69/69), tap water (2008/2009, n ¼ 19/26), and bottled water (2007/2008/2009, n ¼ 5/13/7) were sampled at locations in Luxembourg and investigated for pesticides by LC-ESI-MS/MS. Atrazine was the predominant triazine, detectable in many spring water locations, tap and bottled water, ranging (mean) from 0–57 (9), 0–44 (4), and 0–4 (1) ng lÀ1, respectively. DEA and DIA in spring water ranged (mean) from 0–120 (19) and 0–27 (3) ng lÀ1, with higher concentrations from agricultural areas and low molar ratios of DEA:atrazine 50.5 and high ratios of atrazine:nitrate suggesting point-source contamination. Levels (mean) of DEA and DIA in tap water were 0–62 (14) and 0–6 (51) ng lÀ1 and in bottled water 0–11 (2) and 0–7 (2) ng lÀ1. Simazine and other triazines were detected in traces (55nglÀ1). Thus, the conducted monitoring suggested the presence of low concentrations of s-triazines in raw and finished water, presumably partly due to non-agricultural contamination, with concentrations being below thresholds advocated by the European Union Directive 98/83/EC. Keywords: s-triazine herbicides; atrazine degradation products; tap and spring water; DEA:atrazine ratio; nitrate; 2,6-dichlorobenzamide Introduction Among pesticides, especially the s-triazine herbicides Endocrine-disrupting compounds (EDC) are molecules such as terbutylazine, cyanazine, simazine and atra- exhibiting hormonal or antihormonal activities, thus zine, have achieved much attention in recent years, interacting and potentially perturbing normal physio- even though they have been used since the 1950 s logical functions. These include natural compounds, (Ribaudo and Bouzaher 2010). Although the strict such as mycotoxins, e.g. zearalenone (Mantovani et al. classification of atrazine (2-chloro-4-ethylamino-6-iso- 2009; Giraud et al. 2010) and soy isoflavonoids propylamine-s-triazine) as an EDC has been discussed (Cederroth et al. 2010), and man-made chemicals (Solomon 2009), it has been suggested to inflict such as pharmaceuticals (Pailler et al. 2009) and damage to the central nervous system (Rodriguez Downloaded by [CRP Gabriel Lippmann (Centre de Recherch] at 04:44 05 January 2012 polychlorinated biphenyls (Lasserre et al. 2009), and et al. 2005; Coban and Filipov 2007), the endocrine chemicals employed in agriculture. The latter group system (Rayner et al. 2004; Hayes et al. 2006) and the comprises a large number of pesticides, including, for immune system (Brodkin et al. 2007; Rowe et al. 2008), example, herbicides, fungicides and insecticides. affecting the reproductive health of rats (Kniewald As these compounds have been released on purpose et al. 2000), pigs (Betancourt et al. 2006) and amphib- and are often in direct contact with the future food ians (Hayes et al. 2006), fostering feminization in the product, great prudence in their choice, way of latter (Hayes et al. 2010). However, data on the impact application and concentration has to be maintained. on mammals and particularly humans are scant and Nevertheless, with the increased research on EDC, the effects remain unclear (Solomon 2009). including pesticides, several compounds have been Nevertheless, atrazine is still the most used herbi- hypothesized to impact the human hormonal system. cide in many countries and possibly worldwide *Corresponding author. Email: [email protected] ISSN 1944–0049 print/ISSN 1944–0057 online ß 2011 Taylor & Francis DOI: 10.1080/19440049.2011.580012 http://www.informaworld.com 1042 T. Bohn et al. (Thurman and Scribner 2008). It is used for weed including the s-triazine herbicides atrazine, simazine, removal, especially against broadleaf and grassy weeds, terbuthylazine, sebuthylazine, cyanazine and hexazi- employed in agricultural but also in urban areas such as non, and the atrazine degradation products desethyla- in private gardens, on railway tracks or other weed- trazine and deisopropylatrazine, the urea herbicides control programmes. Atrazine possesses a high ground- isoproturon, chlortoluron, monolinuron, metha- water ubiquity score (GUS) of approximately 3.6 benzthiazuron, metoxuron, diuron, linuron and meto- (Vogue et al. 1994) and thus a high potential for bromuron, the chloroacetanilide herbicides groundwater contamination. In fact, the major way of metazachlor and metolachlor, and 2,6-dichlorobenza- human intake for this pesticide is via water (Bray et al. mide (BAM; Figure 1), a breakdown product of the 2008). In the European Union usage of atrazine was herbicide dichlobenil, were obtained from LGC abandoned in 2004 following general precautionary Promochem (Molsheim, France). Methanol, acetone principles; however, significant concentrations can still and acetonitrile were procured from Biosolve be found in the environment such as in groundwater (Valkenswaard, the Netherlands). and surface water (Administration de la Gestion de l’Eau 2005; Planas et al. 2006; Kuster et al. 2010; Loos et al. 2010), often in concentrations above the 0.1 mglÀ1 Sampling campaigns limit set by the European Union Directive 98/83/EC Several campaigns were carried out in the framework (European Commission 1998). In addition to raw water, of this study: atrazine has been detected in finished (tap) water, up to 60 mglÀ1 in the United States (Wu et al. 2010), while . Spring water: 69 springs in the Luxembourg concentrations in bottled water are generally assumed City area from sandstone aquifer, the major to be much lower due to filtration steps through aquifer in Luxembourg (for a detailed descrip- activated carbon during production. tion, see Gourdol et al. 2010), were monitored Despite its persistence, atrazine has been shown to between summer 2007 and spring 2009, with a undergo degradation in the soil due to bacterial total of ten collection campaigns (July/ activities. These breakdown products include mainly August, November 2007; January, March, the comparatively stable desethylatrazine and deiso- May, June/July, September, October/ propylatrazine (Papiernik and Spalding 1998; Jason November 2008; January, March 2009; et al. 2010), which have likewise been detected in Figure 2). All these springs are involved in groundwater (Shomar et al. 2006; Loos et al. 2010),
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