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Greenhouse and other covered cultivation systems have increased globally over the past several decades, leading to considerably improved product quality and productivity per land area unit. However, there is a paucity in information regarding the environmental impacts of covered production systems, especially regarding pesticides entering the surrounding environment. Aiming to address this knowledge gap, we collected grab samples downstream of greenhouses from seven Swedish streams every 14 days during a 12 month period. In three of the streams, samples were also taken upstream of the greenhouses and in four of the streams time-integrated samples were collected by TIMFIE samplers in the period between grab sampling occasions. The samples were analyzed for 28 substances (27 that were permitted for use in greenhouse production systems in Sweden and one degradation product to a permitted substance). Pesticide use journals were collected from the greenhouse producers for the 12 month period. The results were examined for indications of greenhouse contributions to detection frequencies, maximum and average concentrations, and potential ecotoxicicity in several ways: (1) comparing locations downstream of greenhouses with registered use of a substance with those without registered use, (2) comparing results from this study with those from the Swedish environmental monitoring program of pesticides in surface water from catchments with no greenhouses from the same period and region, (3) comparing concentration trends with registered pesticide application times in the greenhouses, and (4) comparing up- and downstream concentrations. The results strongly suggest that greenhouse applications do contribute to pesticide occurrences, maximum and median concentrations for most of the pesticides included in this study, and to potential toxicity to aquatic organisms for several of them, most notably imidacloprid, acetamiprid, carbendazim, and pirimicarb., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 The Authors. Published by Elsevier B.V. All rights reserved.)

Long-term pesticide water concentrations were investigated in four agricultural streams and their mixture toxicity on algae was assessed, based on realistic (i.e. observed) concentrations in laboratory tests using (i) natural weekly water samples and (ii) reconstituted pesticide-spiked water samples representing mixtures with predicted high mixture. This approach both covered the full complexity of natural water samples and the controlled approach of reconstituted water samples. Long-term monitoring data (time-integrated, weekly samples) revealed more than 11 pesticides (range 11.0 ± 0.25-24.0 ± 0.44) in 75% or more of the almost 1600 samples collected between 2002 and 2018. ∑TU algae exceeded 0.1 for 29 observations (or 1.8%). Despite the multitude of pesticides in a sample, ∑TU algae was frequently set by one or a few dominating pesticides that contribute to more than 90% of the mixture's toxicity. Algal growth inhibition tests with in situ stream water showed a high frequency of inhibition, despite the low ∑TU for most of these samples (range 0.000014-0.3858). These "false positive" results were attributed to confounding effects of turbidity, the complexation of nutrients, and toxic effects of metals and/or other unknown contaminants. Algal inhibition tests with spiked reconstituted water showed significant inhibitory effects in the range of 1-10x the ∑TU algae observed in worst-case field samples. Although these tests disregard the chemical complexity of natural water, they show that inhibitory effects of pesticides on algae may occur at the ∑TU algae observed in monitoring. Furthermore, considering that the ∑TU algae of stream water are based on weekly average concentrations and likely underestimate short-term peak concentrations of pesticides, these results strongly suggest that inhibitory effects on algae may occur in the agricultural streams of southern Sweden. We conjecture, however, that the rapid recovery of algae contributes to ameliorate these short-term effects and that pesticide contamination should be seen as one of many stressors in the streams that drain agricultural landscapes., (Copyright © 2021 The Authors. Published by Elsevier Inc. All rights reserved.)

Three passive sampler types including Chemcatcher® C 18 , polar organic chemical integrative sampler-hydrophilic-lipophilic balance (POCIS-HLB) and silicone rubber (SR) based on polydimethylsiloxane (PDMS) were evaluated for 124 legacy and current used pesticides at two sampling locations in southern Sweden over a period of 6 weeks and compared to time-proportional composite active sampling. In addition, an in situ calibration was performed resulting in median in situ sampling rates (R S , L day -1 ) of 0.01 for Chemcatcher® C 18 , 0.03 for POCIS-HLB, and 0.18 for SR, and median in situ passive sampler-water partition coefficients (log K PW , L kg -1 ) of 2.76 for Chemcatcher® C 18 , 3.87 for POCIS-HLB, and 2.64 for SR. Deisopropylatrazine D 5 showed to be suitable as a performance reference compound (PRC) for SR. There was a good agreement between the pesticide concentrations using passive and active sampling. However, the three passive samplers detected 38 pesticides (including 9 priority substances from the EU Water Framework Directive (WFD) and 2 pyrethriods) which were not detected by the active sampler. The most frequently detected pesticides with a detection frequency of >90% for both sites were atrazine, 2,6-dichlorobenzamide, bentazone, chloridazon, isoproturon, and propiconazole. The annual average environmental quality standard (AA-EQS) for inland surface waters of the EU WFD and the risk quotient (RQ) of 1 was exceeded on a number of occasions indicating potential risk for the aquatic environment., (Copyright © 2018 Elsevier B.V. All rights reserved.)

A better understanding of the dominant source areas and transport pathways of pesticide losses to surface water is needed for targeting mitigation efforts in a more cost-effective way. To this end, we monitored pesticides in surface water in an agricultural catchment typical of one of the main crop production regions in Sweden. Three small sub-catchments (88-242ha) were selected for water sampling based on a high-resolution digital soil map developed from proximal sensing methods and soil sampling; one sub-catchment had a high proportion of clay soils, another was dominated by coarse sandy soils while the third comprised a mix of soil types. Samples were collected from the stream, from field drains discharging into the stream and from within-field surface runoff during spring and early summer in three consecutive years. These samples were analyzed by LC-MS/MS for 99 compounds, including most of the polar and semi-polar pesticides frequently used in Swedish agriculture. Information on pesticide applications (products, doses and timing) was obtained from annual interviews with the farmers. There were clear and consistent differences in pesticide occurrence in the stream between the three sub-catchments, with both the numbers of detected compounds and concentrations being the largest in the area with a high proportion of clay soils and with very few detections in the sandy sub-catchment. Macropore flow to drains was most likely the dominant loss pathway in the studied area. Many of the compounds that were detected in drainage and stream water samples had not been applied for several years. This suggests that despite the predominant role of fast flow pathways in determining losses to the stream, long-term storage along the transport pathways also occurs, presumably in subsoil horizons where degradation is slow., (Copyright © 2017 Elsevier B.V. All rights reserved.)

We quantified pesticide contamination and its ecological impact up- and downstream of seven wastewater treatment plants (WWTPs) in rural and suburban areas of central Germany. During two sampling campaigns, time-weighted average pesticide concentrations (c TWA ) were obtained using Chemcatcher® passive samplers; pesticide peak concentrations were quantified with event-driven samplers. At downstream sites, receiving waters were additionally grab sampled for five selected pharmaceuticals. Ecological effects on macroinvertebrate structure and ecosystem function were assessed using the biological indicator system SPEAR pesticides (SPEcies At Risk) and leaf litter breakdown rates, respectively. WWTP effluents substantially increased insecticide and fungicide concentrations in receiving waters; in many cases, treated wastewater was the exclusive source for the neonicotinoid insecticides acetamiprid and imidacloprid in the investigated streams. During the ten weeks of the investigation, five out of the seven WWTPs increased in-stream pesticide toxicity by a factor of three. As a consequence, at downstream sites, SPEAR values and leaf litter degradation rates were reduced by 40% and 53%, respectively. The reduced leaf litter breakdown was related to changes in the macroinvertebrate communities described by SPEAR pesticides and not to altered microbial activity. Neonicotinoids showed the highest ecological relevance for the composition of invertebrate communities, occasionally exceeding the Regulatory Acceptable Concentrations (RACs). In general, considerable ecological effects of insecticides were observed above and below regulatory thresholds. Fungicides, herbicides and pharmaceuticals contributed only marginally to acute toxicity. We conclude that pesticide retention of WWTPs needs to be improved., (Copyright © 2017 Elsevier B.V. All rights reserved.)

This paper presents the ecotoxicological assessment and environmental risk evaluation of complex pesticide mixtures occurring in freshwater ecosystems in southern Sweden. The evaluation is based on exposure data collected between 2002 and 2013 by the Swedish pesticide monitoring program and includes 1308 individual samples, detecting mixtures of up to 53 pesticides (modal=8). Pesticide mixture risks were evaluated using three different scenarios for non-detects (best-case, worst-case and using the Kaplan-Meier method). The risk of each scenario was analyzed using Swedish Water Quality Objectives (WQO) and trophic-level specific environmental thresholds. Using the Kaplan-Meier method the environmental risk of 73% of the samples exceeded acceptable levels, based on an assessment using Concentration-Addition and WQOs for the individual pesticides. Algae were the most sensitive organism group. However, analytical detection limits, especially for insecticides, were insufficient to analyze concentrations at or near their WQO's. Thus, the risk of the analyzed pesticide mixtures to crustaceans and fish is systematically underestimated. Treating non-detects as being present at their individual limit of detection increased the estimated risk by a factor 100 or more, compared to the best-case or the Kaplan-Meier scenario. Pesticide mixture risks are often driven by only 1-3 compounds. However, the risk-drivers (i.e., individual pesticides explaining the largest share of potential effects) differ substantially between sites and samples, and 83 of the 141 monitored pesticides need to be included in the assessment to account for 95% of the risk at all sites and years. Single-substance oriented risk mitigation measures that would ensure that each individual pesticide is present at a maximum of 95% of its individual WQO, would also reduce the mixture risk, but only from a median risk quotient of 2.1 to a median risk quotient of 1.8. Also, acceptable total risk levels would still be exceeded in more than 70% of the samples., (Copyright © 2017 Elsevier B.V. All rights reserved.)

The use of pesticides in Mozambique is increasing along with the development of agriculture in the country. Mangroves along the coastlines are ecologically important areas and vital nursing grounds for many aquatic species, several of which are of high economic value in Mozambique. Barred mudskipper (Periophthalmus argentilineatus), Jarbua fish (Terapon jarbua), Indian white prawn (Penaeus indicus) and the clam Meretrix meretrix were collected at three mangrove sites in the Maputo Bay area. This was complemented with samplings of the freshwater fish Mozambique tilapia (Oreochromis mossambicus), which was collected from three sampling sites along rivers in the surroundings of Maputo and from three sites along the Olifants and Limpopo River. Acetylcholinesterase (AChE) activity, which is an established biomarker for organophosphates and carbamate pesticides, was measured in brain and liver tissue in fish, and hepatopancreas tissue in prawn and clam. Butyrylcholinesterase (BChE) activity was also analyzed. Freshwater samples for pesticide analyses were collected in order to get an initial understanding of the classes and levels of pesticides present in aquatic systems in Mozambique. In addition to field samplings two 48-h exposure experiments were also conducted where the Indian white prawn and Barred mudskipper were exposed to malathion, and Mozambique tilapia exposed to malathion and diazinon. Field results show a significant decrease in AChE activity in fish from four of the sampling sites suggesting that pesticides present in water could be one stressor potentially affecting aquatic organisms negatively. The 48 h exposure experiment results showed a clear dose-response relationship of AChE activity in mudskipper and tilapia suggesting these species as suitable as sentinel species in environmental studies., (Copyright © 2016. Published by Elsevier Ltd.)

Five different passive sampler devices were characterized under laboratory conditions for measurement of 124 legacy and current used pesticides in water. In addition, passive sampler derived time-weighted average (TWA) concentrations were compared to time-integrated active sampling in the field. Sampling rates (RS) and passive sampler-water partition coefficients (KPW) were calculated for individual pesticides using silicone rubber (SR), polar organic chemical integrative sampler (POCIS)-A, POCIS-B, Chemcatcher(®) SDB-RPS and Chemcatcher(®) C18. The median RS (Lday(-1)) decreased as follows: SR (0.86)>POCIS-B (0.22)>POCIS-A (0.18)>Chemcatcher(®) SDB-RPS (0.05)>Chemcatcher(®) C18 (0.02), while the median logKPW (Lkg(-1)) decreased as follows: POCIS-B (4.78)>POCIS-A (4.56)>Chemcatcher(®) SDB-RPS (3.17)>SR (3.14)>Chemcatcher(®)C18 (2.71). The uptake of the selected compounds depended on their physicochemical properties, i.e. SR showed a better uptake for more hydrophobic compounds (log octanol-water partition coefficient (KOW)>5.3), whereas POCIS-A, POCIS-B and Chemcatcher(®) SDB-RPS were more suitable for hydrophilic compounds (logKOW<0.70). Overall, the comparison between passive sampler and time-integrated active sampler concentrations showed a good agreement and the tested passive samplers were suitable for capturing compounds with a wide range of KOW's in water., (Copyright © 2015 Elsevier B.V. All rights reserved.)

Climate change is not only likely to improve conditions for crop production in Sweden, but also to increase weed pressure and the need for herbicides. This study aimed at assessing and contrasting the direct and indirect effects of climate change on herbicide leaching to groundwater in a major crop production region in south-west Sweden with the help of the regional pesticide fate and transport model MACRO-SE. We simulated 37 out of the 41 herbicides that are currently approved for use in Sweden on eight major crop types for the 24 most common soil types in the region. The results were aggregated accounting for the fractional coverage of the crop and the area sprayed with a particular herbicide. For simulations of the future, we used projections of five different climate models as model driving data and assessed three different future scenarios: (A) only changes in climate, (B) changes in climate and land-use (altered crop distribution), and (C) changes in climate, land-use, and an increase in herbicide use. The model successfully distinguished between leachable and non-leachable compounds (88% correctly classified) in a qualitative comparison against regional-scale monitoring data. Leaching was dominated by only a few herbicides and crops under current climate and agronomic conditions. The model simulations suggest that the direct effects of an increase in temperature, which enhances degradation, and precipitation which promotes leaching, cancel each other at a regional scale, resulting in a slight decrease in leachate concentrations in a future climate. However, the area at risk of groundwater contamination doubled when indirect effects of changes in land-use and herbicide use, were considered. We therefore concluded that it is important to consider the indirect effects of climate change alongside the direct effects and that effective mitigation strategies and strict regulation are required to secure future (drinking) water resources., (Copyright © 2014 Elsevier B.V. All rights reserved.)

The European Water Framework Directive requires surface water bodies to have a good chemical and ecological status. Although relatively few pesticides are included in the list of priority pollutants, they pose, due to their intrinsic biological activity, a significant risk for the integrity of aquatic ecosystems. In this context, the pesticide (up to 128 pesticides including some transformation products) exposure pattern in four agricultural streams and two rivers was determined from 2002 to 2011 under the umbrella of the Swedish national monitoring program employing time-proportional and grab sampling strategies, respectively. After transforming the measured pesticide concentrations into toxic units, the European Uniform Principles for algae (chronic), invertebrates and fish (both acute), which are partly employed as benchmark for pesticide regulation, were only occasionally (<2%) exceeded. Moreover, this evaluation showed no long-term trends over the years. However, recent publications suggested that those thresholds are not protective for ecosystem structure and function, indicating a risk of up to 20% and 35% of the samples from the agricultural streams and the rivers, respectively. Moreover, the monitoring data show a continuous but rather low toxic potential of pesticides for all three trophic levels throughout the year, which suggests pesticides as an evolutionary force in agriculturally impacted aquatic ecosystems. However, the flow-triggered sampling, which was implemented as an additional sampling strategy in one of the agricultural streams starting in 2006, displayed an up to 7-fold underestimation of the maximum concentration in terms of toxic units for daphnids and fish during run-off events. The present study thus underpins that the optimal sampling design for pesticide monitoring strongly depends on its overall purpose. If the long-term exposure pattern is of concern a time-proportional composite sampling strategy is recommended, while for an assessment of peak exposures a flow-event-triggered high-resolution sampling strategy is superior., (Copyright © 2014 Elsevier B.V. All rights reserved.)