Spatial and temporal trends of gas and particle phase atmospheric DDT and metabolites in Michigan: Evidence of long-term persistence and atmospheric emission in a high-DDT-use fruit orchard

Abstract

Michigan was among the top three apple producing states in the United States from the 1940s to 1969 when DDT was heavily used on its fruit orchards. More than 2 decades after Michigan banned DDT use in 1969, we collected air samples from four sites around the state to measure concentrations of six DDT-related compounds in the atmosphere. At South Haven, an apple producing area, average gas phase concentrations of DDT and DDE compounds were at least 10 times greater than the other sites including Pellston in the north, Deckerville in the east, and Dexter in south-central. Concentrations at South Haven showed a very strong seasonal cycle, an effect of higher air temperatures on moving these residues into the gas phase from a local source. We calculated ΔH values for all six compounds from the South Haven data which showed that p,p′-DDE was the highest at 108 kJ mol -1. The ΔH values for all compounds at South Haven had a high correlation with Henry's Law Constant (HLC) (r = 0.7), verifying that HLC is a good indicator of tendency for compound conversion to the gas phase. South Haven was the only site with significant atmospheric particle-associated DDT. Particle/gas ratios there for p,p′-DDT and p,p′-DDE also had a predictable seasonal variation. Overall, these results show that agricultural sites with similar DDT use history will be continuous sources of atmospheric DDT for decades after application. Copyright 2007 by the American Geophysical Union.