Pyrethroids are the active ingredients in most insecticides available to consumers for residential use in the United States. Yet despite their dominance in the marketplace, there has been no attempt to analyze for most of these compounds in watercourses draining residential areas. Roseville, California was selected as a typical suburban development, and several creeks that drain subdivisions of single-family homes were examined. Nearly all creek sediments collected caused toxicity in laboratory exposures to an aquatic species, the amphipod Hyalella azteca, and about half the samples caused nearly complete mortality. This same species was also found as a resident in the system, but its presence was limited to areas where residential influence was least. The pyrethroid bifenthrin is implicated as the primary cause of the toxicity, with additional contributions to toxicity from the pyrethroids cyfluthrin and cypermethrin. The dominant sources of these pyrethroids are structural pest control by professional applicators and/ or homeowner use of insecticides, particularly lawn care products. The suburbs of Roseville are unlikely to be unique, and similar sediment quality degradation is likely in other suburban areas, particularly in dry regions where landscape irrigation can dominate seasonal flow in some water bodies.

The agricultural industry and urban pesticide users are increasingly relying upon pyrethroid insecticides and shifting to more potent members of the class, yet little information is available on residues of these substances in aquatic systems under conditions of actual use. Seventy sediment samples were collected over a 10-county area in the agriculture-dominated Central Valley of California, with most sites located in irrigation canals and small creeks dominated by agricultural effluent. The sediments were analyzed for 26 pesticides including five pyrethroids, 20 organochlorines, and one organophosphate. Ten-day sediment toxicity tests were conducted using the amphipod Hyalella azteca and, for some samples, the midge Chironomus tentans. Forty-two percent of the locations sampled caused significant mortality to one test species on at least one occasion. Fourteen percent of the sites (two creeks and four irrigation canals) showed extreme toxicity (>80% mortality) on at least one occasion. Pyrethroid pesticides were detected in 75% of the sediment samples, with permethrin detected most frequently, followed by esfenvalerate > bifenthrin >lambda-cyhalothrin. Based on a toxicity unit analysis, measured pyrethroid concentrations were sufficiently high to have contributed to the toxicity in 40% of samples toxic to C. tentans and nearly 70% of samples toxic to H. azteca. Organochlorine compounds (endrin, endosulfan) may have contributed to the toxicity at a few other sites. This study provides one of the first geographically broad assessments of pyrethroids in areas highly affected by agriculture, and it suggests there is a greater need to examine sediment-associated pesticide residues and their potential for uptake by and toxicity to benthic organisms.

Pyrethroid pesticides have replaced organophosphates for many urban applications, including structural pest control, landscape maintenance, and residential home and garden use. This study was intended to determine if pyrethroids are detectable and widespread in diverse urban systems and if concentrations are high enough to cause associated aquatic toxicity. Urban creeks in California and Tennessee were tested on up to four occasions for pesticide residues in sediments, and aquatic toxicity was determined by acute toxicity tests using the amphipod, Hyalella azteca. In California, 12 of the 15 creeks tested were toxic on at least one sampling occasion, and sediment pyrethroid concentrations were sufficient to explain the observed toxicity in most cases. The pyrethroid bifenthrin, due to its high concentrations and relative toxicity as compared to other pyrethroids, was likely responsible for the majority of the toxicity at most sites. Cypermethrin, cyfluthrin, deltamethrin, and lambda-cyhalothrin also contributed to toxicity at some locations. The source of cypermethrin and deltamethrin was probably almost entirely structural pest control by professional applicators. Bifenthrin, cyfluthrin, and lambda-cyhalothrin may have originated either from professional structural pest control or from lawn and garden care by homeowners. None of the sediments collected from the 12 Tennessee creeks were toxic, and pyrethroids were rarely detectable. Regional differences between Tennessee and California are possibly attributable to climate, differences in types of residential development, and pesticide use practices.

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Two chemical approaches, Tenax extraction and matrix solid-phase microextraction (matrix-SPME), were compared to assess the bioavailability of hydrophobic contaminants from sediment. Hexachlorobiphenyl, DDE, permethrin, chlorpyrifos, and phenanthrene were individually spiked into two sediments differing in physical characteristics. Bioaccumulation was determined by exposing the oligochaete, Lumbriculus variegatus, to the spiked sediments. The rapidly desorbing fraction from Tenax extraction at 6 h and fiber concentration at 14 d from the matrix-SPME were compared for predicting bioaccumulation. Further, a comparison between laboratory-spiked and field-contaminated sediments was conducted. A regression between the rapidly desorbed sediment concentration at 6 h and the amount bioaccumulated across compounds and sediments described 94% of the variation in the data when phenanthrene was excluded. Phenanthrene was excluded because of complications due to a combination of biotransformation and rapid elimination during the sampling process. Contaminant accumulation by L. variegatus also correlated well with matrix-SPME fiber concentrations, accounting for 92% of the variation in the data, again excluding phenanthrene. Both chemical methods provided matrix- and chemical-independent estimations of bio-accumulation for hydrophobic contaminants without extensive biotransformation.

Passive sampling methods (PSMs) allow the quantification of the freely dissolved concentration (Cfree) of an organic contaminant even in complex matrices such as sediments. Cfree is directly related to a contaminant's chemical activity, which drives spontaneous processes including diffusive uptake into benthic organisms and exchange with the overlying water column. Consequently, Cfree provides a more relevant dose metric than total sediment concentration. Recent developments in PSMs have significantly improved our ability to reliably measure even very low levels of Cfree. Application of PSMs in sediments is preferably conducted in the equilibrium regime, where freely dissolved concentrations in the sediment are well-linked to the measured concentration in the sampler via analyte-specific partition ratios. The equilibrium condition can then be assured by measuring a time series or a single time point using passive samplers with different surface to volume ratios. Sampling in the kinetic regime is also possible and generally involves the application of performance reference compounds for the calibration. Based on previous research on hydrophobic organic contaminants, it is concluded that Cfree allows a direct assessment of 1) contaminant exchange and equilibrium status between sediment and overlying water, 2) benthic bioaccumulation, and 3) potential toxicity to benthic organisms. Thus, the use of PSMs to measure Cfree provides an improved basis for the mechanistic understanding of fate and transport processes in sediments and has the potential to significantly improve risk assessment and management of contaminated sediments. Integr Environ Assess Manag 2014;10:197–209. © 2014 The Authors. Integrated Environmental Assessment and Management published by Wiley Periodicals, Inc. on behalf of SETAC.

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