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Stakeholders need operational tools to assess crop protection strategies in regard to environmental impact. The need to assess and report on the impacts of pesticide use on the environment has led to the development of numerous indicators. However, only a few studies have addressed the predictive quality of these indicators. This is mainly due to the limited number of datasets adapted to the comparison of indicator outputs with pesticide measurement. To our knowledge, evaluation of the predictive quality of pesticide indicators in comparison to the quality of water as presented in this article is unprecedented in terms of the number of tested indicators (26 indicators and the MACRO model) and in terms of the size of datasets used (data collected for 4 transfer pathways, 20 active ingredients (a.i.) for a total of 1040 comparison points). Results obtained on a.i. measurements were compared to the indicator outputs, measured by: (i) correlation tests to identify linear relationship, (ii) probability tests comparing measurements with indicator outputs, both classified in 5 classes, and assessing the probability i.e. the percentage of correct estimation and overestimation (iii) by ROC tests estimating the predictive ability against a given threshold. Results showed that the correlation between indicator outputs and the observed transfers are low (r<0.58). Overall, more complex indicators taking into account the soil, the climatic and the environmental aspects yielded comparatively better results. The numerical simulation model MACRO showed much better results than those for indicators. These results will be used to help stakeholders to appropriately select their indicators, and will provide them with advice for possible use and limits in the interpretation of indicator outputs.

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This study evaluates the efficiency of two small constructed wetlands installed in the regulatory grass strips between a drained plot and a river. The observed nitrate removal efficiencies were independent of the season or type of constructed wetland and ranged from 5.4 to 10.9% of the inlet amounts. The pesticide mass budgets ranged from -618.5 to 100%, depending on the molecule. The negative efficiencies were attributed to runoff and remobilization. In contrast, the highest efficiencies were associated with pesticides with high Koc and low DT50 (half-life) values, suggesting sorption and degradation. However, the effectiveness of these wetlands is limited for pesticides with low Koc or high DT50 values; thus, the use of these molecules must be reduced. Increasing the number of these small, inexpensive and low-maintenance wetlands in the agricultural landscape would reduce the level of water pollution whilst preserving the extent of cultivated land, but their long-term effectiveness should be evaluated.

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Oxidative degradation of atrazine by hydroxyl radicals (()OH) was studied in aqueous medium. ()OH were formed in situ from electrochemically generating Fenton's reagent by an indirect electrochemical advanced oxidation process. Identification and evolution of seven main aromatic metabolites and four short-chain carboxylic acids were performed by using liquid chromatography analyses. Total organic carbon (TOC) and ionic chromatography were used in order to evaluate the mineralization efficiency of treated aqueous solutions. A high mineralization rate of 82% (never reported until now) was obtained. The oxidative degradation of cyanuric acid, the ultimate product of atrazine degradation, was highlighted for the first time. The absolute rate constant of the reaction between atrazine and hydroxyl radicals was evaluated by competition kinetics method as (2.54+/-0.22)x10(9)M(-1)s(-1). Considering all oxidation reaction intermediates and end products a general reaction sequence for atrazine degradation by hydroxyl radicals was proposed.

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Batch adsorption and desorption experiments were performed using thirteen agricultural soil samples and five pesticides. Experimental data indicated a gradient in pesticide adsorption on soil: trifluralin >> 2,4-D > isoproturon> atrazine >> bentazone. Atrazine, isoproturon and trifluralin adsorption were correlated to soil organic matter content (r2 = 0.7, 0.82, 0.79 respectively). Conversely, bentazone adsorption was governed by soil pH (r2 = 0.68) while insignificant effect has been shown in the case of 2,4-D. Multiple linear regressions were used to combine relationships between the various soil parameters and the Freundlich adsorption coefficient (K(f)) of each pesticide. Then desorption was assessed since it may reflect some of the interactions involved between the pesticides and the soil components. Adsorbed molecules were released into aqueous solution in the following order: bentazone >> atrazine> isoproturon> 2,4-D >> trifluralin. The occurrence of hysteresis did not allow an accurate interpretation of the pesticide desorption data because of the possible interplay of several processes.

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A soil column experiment under outdoor conditions was performed to monitor the fate of 14C-ring-labelled sulcotrione, 2-(2-chloro-4-mesylbenzoyl)cyclohexane-1,3-dione and atrazine, 6-chloro-N2-ethyl-N4-isopropyl-1,3,5-triazine-2,4-diamine, in water leachates and in the ploughed horizon of a sandy loam soil. Two months after treatment, the cumulative amounts of herbicide residues leached from the soil were 14.5% and 7% of the applied radioactivity for sulcotrione and atrazine, respectively. Maximum leachate concentrations for each herbicide were observed during the first month following application: 120 and 95 microg litre(-1) for sulcotrione and atrazine respectively. After 2 weeks, 78% of the sulcotrione and atrazine was extractable from the soil, whereas after two months only 10 and 4%, respectively, could be extracted. The maximum sulcotrione content in the first 10 cm of soil was identical with that of atrazine. For both molecules, the content of non-extractable residues was low, being around 15%. Sulcotrione seems to be more mobile than atrazine but the consequences for water contamination are similar since lower doses are used.

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Previous sorption/desorption batch experiments have indicated that bentazone is weakly sorbed by soils. In addition, field experiments have shown that 4% of the bentazone sprayed can be leached to drainage water. In order to complete bentazone characterisation, we have assessed the effect of time on its behaviour in contrasting soils. In laboratory studies, bentazone was added to three topsoils (sandy, loamy and clay soils). Bentazone degradation, sorption/desorption kinetics and isotherm measurements were carried out at different times. At 160 days after treatment, bentazone mineralisation amounts varied from 2.1% (sandy soil) to 14% (clay soil). The extractable amounts became lower (from 97% after treatment to 12% after 160 days for the clay soil) and a greater number of desorption series was needed to obtain these products. Nevertheless, at the end of the experiments, a small amount of bentazone was still extracted by water. At the same time, bound residues of bentazone reached 65% in clay soil. Statistical analysis indicated effects of both residence time and soil type on bentazone behaviour.

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