Abstract

Pesticide concentration trends in streams dominated by urban land use were assessed using data from 27 urban streams sampled as part of the U.S. Geological Survey National Water-Quality Assessment Program. The sites were divided into four regions, Northeast, South, Midwest, and West, to examine possible regional patterns. Three partially overlapping 9-year periods (1992–2000, 1996–2004, and 2000–2008) were examined for eight herbicides and one degradation product (simazine, prometon, atrazine, deethylatrazine, metolachlor, trifluralin, pendimethalin, tebuthiuron, and Dacthal), and five insecticides and two degradation products (chlorpyrifos, malathion, diazinon, fipronil, fipronil sulfide, desulfinylfipronil, and carbaryl). The data were analyzed for trends in concentration using a parametric regression model with seasonality, flow-related variability, and trend, called SEAWAVE-Q. The SEAWAVE-Q model also was used to generate estimated daily concentration percentiles for each analysis period to provide a summary of concentration magnitudes.

For herbicides, the largest 90th percentiles of estimated concentrations for simazine were in the South, prometon at some sites in all of the regions, atrazine and deethylatrazine in the South and Midwest, metolachlor in the Midwest and a few sites in the South, pendimethalin at scattered sites in all of the regions, and tebuthiuron in the South and a few sites in the Midwest and West. For insecticides, the largest 90th percentiles of estimated concentrations for diazinon and carbaryl were distributed among various sites in all regions (especially during 1996–2004), and fipronil at isolated sites in all of the regions during 2000–2008.

Trend analysis results for the herbicides indicated many significant trends, both upward and downward, with varying patterns depending on period, region, and herbicide. Overall, deethylatrazine showed the most consistent pattern of upward trends, especially in the Northeast (2000–2008), South (1996–2004 and 2000–2008), and Midwest (1996–2004 and 2000–2008). Other herbicides showed less consistent upward trends, including simazine in the South (1996–2004), prometon in the Midwest (2000–2008), and atrazine in the South (1996–2004). The most consistent downward trends were for simazine in the Northeast and Midwest (1996–2004), prometon in the Northeast and Midwest (1996–2004) and West (1996–2004 and 2000–2008), and tebuthiuron in the South (1996–2004 and 2000–2008) and West (2000–2008).

Strong similarity existed between the trends for atrazine and deethylatrazine during 1996–2004. During 2000–2008, however, there were mixed upward and downward trends in atrazine and predominantly upward trends in deethylatrazine. Ten sites with a downward trend in atrazine were paired with an upward trend in deethylatrazine and for three of these sites (1 in the South and 2 in the Midwest) both opposing trends were significant. Opposing trends showing a decrease in atrazine and an increase in deethylatrazine may indicate that decreases in atrazine from surface runoff are being offset in some cases by increases in deethylatrazine from groundwater for the latter analysis period.

Trend results for insecticides indicated widespread significant downward trends for chlorpyrifos (especially 1996–2004), diazinon (1996–2004 and 2000–2008), and malathion (especially 1996–2004); widespread significant upward trends for fipronil and its degradation products (2000–2008); and mostly nonsignificant trends for carbaryl (1996–2004 and 2000–2008). The downward trends for chlorpyrifos and diazinon were consistent with the regulatory phaseout of residential uses of these insecticides and the upward trends for fipronil and its degradation products were consistent with its introduction in 1996 and subsequent increasing use as a possible substitute for chlorpyrifos and diazinon. The downward trends in malathion may be caused by voluntary substitution of pyrethroids or fipronil for malathion. Although carbaryl trends were mostly nonsignificant, most of the trends for 1996–2004 were upward and four of the upward trends were significant. The upward tendency in carbaryl concentrations during that time may indicate some substitution of carbaryl for chlorpyrifos and diazinon. For 2000–2008, carbaryl trends were mixed upward and downward and the trends were mostly nonsignificant. Despite voluntary cancellation of some residential uses of carbaryl beginning in about 2000, there were only four significant downward trends during 2000–2008 and two significant upward trends during that time. Voluntary cancellations of some carbaryl uses may not have decreased overall carbaryl usage in some areas, or decreases in some uses may have been offset by substitution of carbaryl for chlorpyrifos and diazinon.

First posted February 3, 2011