4.7 Article

Large seasonal fluctuations of groundwater radioiodine speciation and concentrations in a riparian wetland in South Carolina

Journal

SCIENCE OF THE TOTAL ENVIRONMENT
Volume 816, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.scitotenv.2021.151548

Keywords

Iodine-129; Organo-iodine; Wetlands; Seasons; Temperature; Speciation

Funding

  1. Department of Energy's Subsurface Biogeochemical Research Program within the Office of Science [DE-FG02-08ER64567, DE-SC0021024]
  2. SRNL's Laboratory Directed Re-search and Development program [LDRD-2018-00005]
  3. Savannah River National Laboratory under the U.S. De-partment of Energy [DE-AC09-96SR18500]
  4. U.S. Department of Energy (DOE) [DE-SC0021024] Funding Source: U.S. Department of Energy (DOE)

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Recent studies in a riparian wetland in South Carolina, USA, showed strong seasonal fluctuations in groundwater radioiodine (I-129) concentrations, with higher concentrations in summer than in winter. These fluctuations were observed only in the wetlands and only with I-129, not with other contaminants. The study proposed a hypothesis that the fluctuations were a result of coupled processes involving hydrology, water temperature, microbiology, and chemistry. The findings underscore the importance of understanding the seasonal variations of contaminants for effective long-term monitoring programs in wetlands.
Recent studies evaluating multiple years of groundwater radioiodine (I-129) concentration in a riparian wetland located in South Carolina, USA identified strong seasonal concentration fluctuations, such that summer concentrations were much greater than winter concentrations. These fluctuations were observed only in the wetlands but not in the upland portion of the plume and only with I-129, and not with other contaminants of anthropogenic origin: nitrate/nitrite, strontium-90, technecium-99, tritium, or uranium. This unexplained observation was hypothesized to be the result of strongly coupled processes involving hydrology, water temperature, microbiology, and chemistry. To test this hypothesis, an extensive historical groundwater database was evaluated, and additional measurements of total iodine and iodine speciation were made from recently collected samples. During the summer, the water table decreased by as much as 0.7 m, surface water temperature increased by as much as 15 degrees C, and total iodine concentrations were consistently greater (up to 680%) than the following winter months. Most of the additional iodine observed in the summer could be attributed to proportional gains in organo-iodine, and not iodide or iodate. Furthermore, I-129 concentrations were observed to be two-orders-of magnitude greater at the bottom of the upland aquifer than at the top. A coupled hydrological and biogeochemical conceptual model is proposed to tie these observations together. First, as the surface water temperature increased during the summer, microbial activity was enhanced, which in turn stimulated the formation of mobile organo-I. Hydrological processes were also likely involved in the observed iodine seasonal changes: (1) as the water table decreased in summer, the remaining upland water entering the wetland was comprised of a greater proportion of water containing elevated iodine concentrations from the low depths, and (2) water flow paths in summer changed such that the wells intercepted more of the contaminant plume and less of the diluting rainwater (due to evapotranspiration) and streamwater (as the lower levels promote a predominantly recharging system). These results underscore the importance of coupled processes influencing contaminant concentrations, and the need to assess seasonal contaminant variations to optimize long-term monitoring programs of wetlands. (C) 2021 Elsevier B.V. All rights reserved.

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