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Transfer of Hexazinone and Glyphosate Through Undisturbed Soil Columns in Soils Under Christmas Tree Cultivation

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Transfer of Hexazinone and Glyphosate Through Undisturbed Soil Columns in Soils Under Christmas Tree Cultivation Chemosphere 57 (2004) 265–272 www.elsevier.com/locate/chemosphere Transfer of hexazinone and glyphosate through undisturbed soil columns in soils under Christmas tree cultivation S. Dousset a,*, C. Chauvin a, P. Durlet b,M.Thevenot a a UMR 1229 INRA/Universite de Bourgogne, Geosol, Centre des Sciences de la Terre, Universite de Bourgogne, 6 boulevard Gabriel, 21000 Dijon, France b Parc Naturel Regional du Morvan, Maison du Parc, 58230 Saint Brisson, France Received 24 February 2004 Abstract Field studies monitoring pesticide pollution in the Morvan region (France) have revealed surface water contami- nation by some herbicides. The purpose of this study was to investigate in greater detail the transport of two herbicides, used in Christmas tree production in the Morvan, under controlled laboratory conditions. Thus, the leaching of hexazinone (3-cyclohexyl-6-dimethyl-amino-1-methyl-1,3,5-triazine-2,4 (1H,3H) dione) and glyphosate (N-(phosphono-methyl-glycine)) through structured soil columns was studied using one loamy sand and two sandy loams from sites currently under Christmas tree cultivation in the Morvan. The three soils were cultivated sandy brunisol [Sound reference base for soils, D. Baize, M.C. Girard (Coord.), INRA, Versailles, 1998, 322 p] or, according to the FAO [FAO, World reference base for soil resources, ISSS-ISRIC-FAO, FAO, Rome, Italy, 1998], the La Garenne was an arenosol and the two other soils were cambisols. The clay contents of the soils ranged from 86 to 156 gkgÀ1 and the organic carbon ranged from 98 to 347 g kgÀ1. After 160 mm of simulated rainfall applied over 12 days, 2– 11% of the applied hexazinone was recovered in the leachate. The recovery was much higher than that of glyphosate, which was less than 0.01%. The greater mobility of hexazinone might be related to its much lower adsorption coeffi- À1 À1 cient, Koc, 19–300 l kg , compared with 8.5–10 231 l kg for glyphosate (literature values). Another factor that may explain the higher amounts of hexazinone recovered in the leachates of the three soil columns is its greater persistence (19.7–91 days) relative to that of glyphosate (7.9–14.4 days). The mobility of both herbicides was greater in the soils with higher gravel contents, coarser textures, and lower organic carbon contents. Moreover, glyphosate migration seems negatively correlated not only to soil organic carbon, but also to aluminium and iron contents of soils. This soil column study suggests that at the watershed scale, surface water contamination by hexazinone could occur via the horizontal subsurface flow in upper centimeters of soil. In contrast, the surface water contamination with glyphosate by this mechanism appears unlikely. Ó 2004 Elsevier Ltd. All rights reserved. Keywords: Leaching; Herbicide; Undisturbed soil column; Christmas tree 1. Introduction * Corresponding author. Tel.: +33-80-39-68-88; fax: +33-80- 39-63-87. Since the 1960s, the area under Christmas tree culti- E-mail address: [email protected] (S. Dous- vation increased in the Morvan region in an effort to set). diversify agricultural activities (about 1500 ha at present). 0045-6535/$ - see front matter Ó 2004 Elsevier Ltd. All rights reserved. doi:10.1016/j.chemosphere.2004.06.007 266 S. Dousset et al. / Chemosphere 57 (2004) 265–272 The Morvan is the principal region of Christmas tree nitrile (Chromanorm quality) were obtained from production in France with sales of approximately one Prolabo (Fontenay-sous-Bois, France). Hexazinone million trees per year, and areas of cultivation occupying and glyphosate were obtained from Cluzeau (Sainte- the majority of some watersheds (Durlet and Chauvin, Foy-La-Grande, France) with >99% and >98% certified 2003). Christmas tree production was not regulated in purity, respectively. Hexazinone (3-cyclohexyl-6-di- France until March 2003 (French Directive, 2003). methyl-amino-1-methyl-1,3,5-triazine-2,4 (1H,3H) di- The use of pesticides, particularly of herbicides, on one) is a colorless crystalline powder. Its vapor pressure the sandy soils where the Christmas trees are grown, is 3 · 10À5 Pa at 25 °C and its water solubility is 33 g lÀ1 and the high rainfall in the Morvan (1074 mm yearÀ1, at 25 °C (Tomlin, 1997). Its half-life is 19.7–91 days 10-year average from 1991 to 2000 at Saulieu meteoro- (Bottoni et al., 1996; Garcia-Valcarcel and Tadeo, 1999; logical station, 10 km from the sampling sites, Meteo- Fernandez et al., 2001; Calderon et al., 2004). Its À1 France data) increase the risks of surface water adsorption coefficient (Koc) varies from 19 to 300 l kg contamination in this area. In addition, in Morvan, (Bourchard and Lavy, 1985; Donati et al., 1994; Ko- drinking water is provided by numerous small shallow skinen et al., 1996; Oliveira et al., 2001). Glyphosate (N- aquifers. Little information on the environmental fate of (phosphono-methyl-glycine)) is a colorless crystalline herbicides used in France in forest management is powder. Its vapor pressure is negligible and its water available, and even less related to Christmas tree culti- solubility is 11.6 g lÀ1 at 25 °C (Tomlin, 1997). Its half- vation. However, a previous study on the area under life varies from 7.9 to 14.4 days (Eberbach, 1999; Acci- investigation showed herbicide contamination of the nelli et al., in press) and Koc varies from 8.5 to 10 231 drinking water (Chauvin et al., 2002). lkgÀ1 (Gerritse et al., 1996; Cheah et al., 1997; De Jonge Consequently, the present study aims to determine and De Jonge, 1999). the potential leaching of hexazinone and glyphosate, two heavily used herbicides in Christmas tree cultiva- 2.2. Soils and column sampling tion. Glyphosate use is not restricted by the EEC, whereas hexazinone has been prohibited (EEC, 1991, The three soils studied were sampled from the 0–20 2003). However, in France hexazinone may continue to cm depth in three watersheds located the north-east of be used on resinous trees until June 30, 2007, on the Morvan highlands (La Garenne WGS 84: 47°1005800 N, condition that it does not adversely affect the environ- 4°100600 E; Moulin Granvault: 47°1903900 N, 4°805900 E; ment (EEC, 2003). Several field studies have shown the and Courtil Gerard: 47°1803400 N, 4°120000 E; Fig. 1), presence of hexazinone in surface waters in USA (Ala- where Christmas tree production area is the most bama) (Michael and Neary, 1993), in drain water in developed. The three main species cultivated are Yellow Denmark (Felding, 1992) and groundwater in Canada spruce (Picea excelsa), Serbian spruce (Picea omorika), (Keizer et al., 2001). Few studies are available con- and Nordmann fir (Abies nordmanniana). Christmas tree cerning the presence of glyphosate in natural water. cultivation occupies 29% of the La Garenne, 20% of the Newton et al. (1994) found that residues in streams were Moulin Granvault, and 6% of the Courtil Gerard close to the detection limit or undetectable in 3–14 days, watersheds. At the time of the study, the trees on La and Skark et al. (1998) found glyphosate in the surface Garenne were 10 years old; at the Courtil Gerard site, water of rivers at a maximum concentration of 0.6 the Christmas trees were 2 years old and cultivated in lglÀ1. pots; and at the Moulin Granvault site, trees were also 2 This study was performed on three sandy brunisols years old. The soils were three sandy brunisols (SRBS, from three watersheds representative of the areas under 1998) (arenosol: La Garenne, cambisols: Courtil Gerard Christmas tree cultivation in the Morvan. The leaching and Moulin Granvault; FAO, 1998) developed on of hexazinone and glyphosate was evaluated through granite. Hexazinone and glyphosate were not applied on undisturbed soil columns under controlled laboratory these plantations in 2002. Analyses of the three soils conditions. The results will allow an assessment of the were performed by the INRA laboratory (Arras, risk of water contamination by the two herbicides when France) and the main characteristics are listed in Table used in Christmas tree production on soils with different 1. At the same time we sampled the soil columns, 10 kg physical and chemical characteristics. of each soil were collected and sieved to 2 mm. The coarse fraction was measured as the percentage of the fraction > to 2 mm based on the total weight of the air- 2. Materials and methods dried soil. Column extraction of the three soils occurred on July 2.1. Chemicals 17, 2002 and was facilitated by the use of a backhoe to carefully excavate the surrounding soil. Final carving All chemicals were of analytical reagent grade and of the soil was carefully performed by hand resulting in used without further purification. Methanol and aceto- 15 cm diameter cylinders of structured soil. A 25 cm S. Dousset et al. / Chemosphere 57 (2004) 265–272 267 Fig. 1. Map of soil columns sampling locations. Table 1 Surface soil characteristics (Ap horizons) a b;c b;c b;c b;d b b b Soil pHH2O CM Sand Silt Clay OC CEC Fe Al (g kgÀ1) (g kgÀ1) (g kgÀ1) (g kgÀ1) (g kgÀ1) (cmol kgÀ1) (g kgÀ1) (g kgÀ1) La Garenne 5.8 350 764 150 86 9.8 9.8 17.7 71.7 (loamy sand) Courtil Gerard 6.3 205 632 212 156 34.7 10.6 10.7 72.3 (sandy loam) Moulin 5.2 379 696 189 115 15.1 8.0 12.1 76.5 Granvault (sandy loam) a CM: coarse materials (>2 mm) in g kgÀ1 of the total weight of the air-dried soil. b Chemical analyses have been performed on the <2 mm fraction.
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