Rain events may impact the chemical pollution burden in rivers. Forty-four small streams in Germany were profiled during several rain events for the presence of 395 chemicals and five types of mixture effects in in vitro bioassays (cytotoxicity, activation of the estrogen, aryl hydrocarbon and peroxisome proliferator-activated receptors and oxidative stress response). While these streams were selected to cover a wide range of agricultural impacts, in addition to the expected pesticides, wastewater-derived chemicals and chemicals typical for street run-off were detected. The unexpectedly high estrogenic effects in many samples indicated impact by wastewater or overflow of combined sewer systems. The 128 water samples exhibited a high diversity of chemical and effect patterns, even for different rain events at the same site. The detected 290 chemicals explained only a small fraction (<8 %) of the measured effects. The experimental effects of designed mixtures of detected chemicals that were expected to dominate the mixture effects of detected chemicals were consistent with predictions for concentration addition by a factor of two for 94 % of the mixtures.Overall, the burden of chemicals and effects were much higher than previously detected in surface water during dry weather with the effects often exceeding effect-based trigger values. In-vitro bioassay test batteryEndocrine effects • ER Metabolism • AhR • PPARy Adaptive stress response: • Oxidative stress Chemical analysis Sampling triggered by rain events Mixture models

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a b s t r a c tLand use related habitat degradation in freshwater ecosystems has considerably increased over the past decades, resulting in effects on the aquatic and the riparian communities. Previous studies, mainly in undisturbed systems, have shown that aquatic emergent insects contribute substantially to the diet of riparian predators. To evaluate the effect of land use on aquatic prey subsidies of riparian spiders, we performed a longitudinal study from June to August 2012 along a first order stream (Rhineland-Palatinate, Germany) covering three land use types: forest, meadow and vineyard. We determined the contribution of aquatic and terrestrial resources to the diet of web-weaving (Tetragnathidae spp.) and ground-dwelling (Pardosa sp.) riparian spiders using stable isotope analyses of aquatic emergent insects and terrestrial arthropods. The contribution of aquatic and terrestrial sources differed between Tetragnathidae spp. and Pardosa sp. as well as among land use types. Tetragnathidae spp. consumed 80-100% of aquatic insects in the meadows and 45-65% in the forest and vineyards. Pardosa sp. consumed 5-15% of aquatic insects in the forest, whereas the proportions of aquatic and terrestrial sources were approximately 50% in the meadow and vineyard. Thus, aquatic emergent insects are an important subsidy to riparian spiders and land use is likely to affect the proportion of aquatic sources in the spider diet.

Neonicotinoids are increasingly applied on trees as protection measure against insect pests. Consequently, neonicotinoids are inevitably transferred into aquatic environments either via spray drift or surface runoff or (due to neonicotinoids' systemic nature) via senescent leaves. There particularly leaf-shredding invertebrates may be exposed to neonicotinoids through both the water phase and the consumption of contaminated leaves. In 7 day bioassays (n = 30), we examined ecotoxicological differences between these two exposure scenarios for an amphipod and an insect nymph with their feeding rate as the response variable. Organisms either experienced waterborne neonicotinoid (i.e., imidacloprid, thiacloprid, and acetamiprid) exposure only or a combined exposure (waterborne and dietary) through both the consumption of contaminated leaves and neonicotinoids leaching from leaves into water. The amphipod (7 day ECs from 0.3 to 8.4 μg/L) was more sensitive than the insect nymph (7 day ECs from 7.0 to 19.4 μg/L). Moreover, for both species, concentration-response models derived from water concentrations indicated higher effects under the combined exposure. Together with the observed inability of shredders to avoid neonicotinoid-contaminated leaves, our results emphasize the relevance of dietary exposure (e.g., via leaves) for systemic insecticides. Thus, it would be prudent to consider dietary exposure during the registration of systemic insecticides to safeguard ecosystem integrity.

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