Atmospheric distribution and long-range transport behavior of organochlorine pesticides in north America

Annually averaged concentrations and enantiomeric compositions of organochlorine pesticides (OCPs) in air were determined in 2000/2001 at 40 stations across North America using XAD-based passive samplers. Absolute concentration differences across the continent, the skewness and kurtosis of the concentration distribution, the relative abundance of parent compound and metabolites, and the chiral signatures can identify regional sources of OCP to the atmosphere. Specifically, air samples collected in the southeastern United States had elevated concentrations of chlordane-related compounds, higher ratios of transto cis-chlordane and heptachlor to heptachlor epoxide, as well as higher enantiomeric fractions of trans-chlordane as compared to other regions, suggesting continued release of microbially unprocessed chlordane to the regional atmosphere. Similarly, greatly elevated concentrations of p,p'-DDT, low relative abundance of the metabolite DDE, and a racemic composition of o,p'-DDT in samples from southern Mexico and Belize indicate recent use of DDT in these regions. Belize is also a potential source region for dieldrin. Reflecting its continued use in North America, endosulfan is now one of the most abundant and ubiquitous UPS in the continental atmosphere. In contrast to these OCPs, air concentrations of penta- and hexachlorobenzene vary only by factors of 2-4 across the continent, reflecting a long atmospheric residence time and few primary sources. Atmospheric levels of the chlorobenzenes, (x-endosulfan, and p,p'-DDE increase with elevation in the Canadian Rocky Mountains. Empirical travel distances for the OCPs derived from latitudinal concentration profiles are in good agreement with model-derived indicators of long-range transport potential and, in particular, lead to a similar categorization of the OCPs. Large-scale passive air sampling networks are suitable for monitoring compliance with, and effectiveness of, regulatory control measures and for establishing experimentally the atmospheric long-range transport behavior of organic air pollutants.