Isotopic discrimination of natural and anthropogenic perchlorate sources in groundwater in a semi-arid region of northeastern Oregon (USA)

Hatzinger, Paul B.; Böhlke, J. K.; Jackson, W. Andrew; Gu, Baohua; Mroczkowski, Stanley J.; Sturchio, Neil C.

doi:10.1016/j.apgeochem.2022.105232

Title: Isotopic discrimination of natural and anthropogenic perchlorate sources in groundwater in a semi-arid region of northeastern Oregon (USA)

Journal Article · Mon Feb 21 00:00:00 EST 2022 · Applied Geochemistry

DOI:https://doi.org/10.1016/j.apgeochem.2022.105232· OSTI ID:1879959

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Aptim Federal Services, Lawrenceville, NJ (United States)
US Geological Survey, Reston, VA (United States)
Texas Tech Univ., Lubbock, TX (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Delaware, Newark, DE (United States)

Perchlorate (ClO₄^-) has synthetic and natural sources. Synthetic ClO₄^- is released to the environment from its use as an oxidant in military and aerospace applications, and from its presence in a variety of common commercial products, such as safety flares, chlorate herbicides, and fireworks. Natural sources of ClO₄^- in the environment include imported nitrate fertilizers derived from salt deposits in the Atacama Desert of Chile and indigenous natural ClO₄^- that accumulates in unsaturated soils and groundwaters in other arid and semi-arid environments, largely from atmospheric deposition. The stable isotope ratios of chlorine (³⁷Cl/³⁵Cl) and oxygen (¹⁸O/¹⁶O, ¹⁷O/¹⁶O) and the isotopic abundance of radioactive ³⁶Cl in ClO₄^- can be used to discriminate these different sources. Perchlorate was previously detected at relatively high concentrations (3.8–34.7 μg/L) in groundwater from many wells in the Boardman-Umatilla area near the Columbia River in northeastern Oregon, which is a semi-arid, highly agricultural, heavily irrigated area that includes several past and current military installations. Eight representative groundwater wells were sampled throughout this region and isotopic characteristics of ClO₄^- collected from each well were measured along with other chemical and isotopic parameters including tritium and other groundwater age indicators. We report isotopic data indicate that indigenous natural ClO₄^- was present in groundwater from all sampled wells and was the predominant source in five of the wells. Synthetic ClO₄^- was present in the three remaining wells with natural ClO₄^-, and a minor fraction of Atacama-fertilizer-derived ClO4- was indicated in one of the wells. Data from this study expand the geographic area of the USA in which indigenous natural ClO₄^- has been detected to include the semi-arid northwest. This study also illustrates the role of irrigation recharge as a mechanism for producing relatively high concentrations of indigenous natural ClO₄^- in groundwater by flushing accumulated salts from the unsaturated zone.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOD; USGS

Grant/Contract Number:: AC05-00OR22725; W912HQ-05-C-0022; W912HQ-08-0061

OSTI ID:: 1879959

Journal Information:: Applied Geochemistry, Vol. 139, Issue 1; ISSN 0883-2927

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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58 GEOSCIENCES
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Perchlorate
Nitrate
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Umatilla
Groundwater
Fertilizer
Irrigation
Atacama
Chile

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