Occurrence, Spatial, and Seasonal Variations, and Gas–Particle Partitioning of Atmospheric Current-Use Pesticides (CUPs) in the Great Lakes Basin

There is very little information on the gas-particle partition and spatial and seasonal variations of current-use pesticides (CUPs) in the Great Lakes basin. The atmospheric concentrations of 36 CUPs were measured in 24 h gas and particle samples collected in 2017 at six sites in the Great Lakes basin. Thirteen individual CUPs were detected at least once in both gas- and particle-phase samples, with chlorothalonil, trifluralin, metolachlor, λ-cyhalothrin, cypermethrin, and chlorpyrifos detected in >50% samples. The gas-particle partitioning analysis suggests that gas-phase chemicals like trifluralin and chlorpyrifos were not influenced by either temperature or relative humidity while particle-phase chemicals like metolachlor were marginally and negatively correlated with relative humidity. Median total CUP concentrations were 339, 238, 84, 33, 60, and 6.0 pg/m³ at Chicago, Cleveland, Sturgeon Point, Point Petre, Sleeping Bear Dunes, and Eagle Harbor, respectively. The concentrations of total CUPs and most individual CUPs were generally higher at the urban sites of Chicago and Cleveland than at the rural/remote sites of Sturgeon Point, Point Petre, Sleeping Bear Dunes, and Eagle Harbor. Chlorothalonil, trifluralin, bifenthrin, and chlorpyrifos were the most abundant individual CUPs among fungicides, herbicides, pyrethroid insecticides, and other insecticides, respectively. The spatio-seasonal variation suggests that fungicides at Sturgeon Point and Sleeping Bear Dunes, with the highest fraction of agricultural land use, were associated with agricultural activities, while pyrethroid insecticides were generally driven by human activities.