Chlorine-36 as a tracer of perchlorate origin

Abstract

Perchlorate (ClO 4 − ) is ubiquitous in the environment. It is produced naturally by atmospheric photochemical reactions, and also is synthesized in large quantities for military, aerospace, and industrial applications. Nitrate-enriched salt deposits of the Atacama Desert (Chile) contain high concentrations of natural ClO 4 − , and have been exported worldwide since the mid-1800s for use in agriculture. The widespread introduction of synthetic and agricultural ClO 4 − into the environment has contaminated numerous municipal water supplies. Stable isotope ratio measurements of Cl and O have been applied for discrimination of different ClO 4 − sources in the environment. This study explores the potential of 36 Cl measurements for further improving the discrimination of ClO 4 − sources. Groundwater and desert soil samples from the southwestern United States (U.S.) contain ClO 4 − having high 36 Cl abundances ( 36 Cl/Cl = 3100 × 10 −15 to 28,800 × 10 −15 ), compared with those from the Atacama Desert ( 36 Cl/Cl = 0.9 × 10 −15 to 590 × 10 −15 ) and synthetic ClO 4 − reagents and products ( 36 Cl/Cl = 0.0 × 10 −15 to 40 × 10 −15 ). In conjunction with stable Cl and O isotope ratios, 36 Cl data provide a clear distinction among three principal ClO 4 − source types in the environment of the southwestern U.S.