Evaluation of dissolution flux of iodine from brackish lake sediments under different temperature and oxygenic conditions

Abstract

Dissolution flux of iodine from aquatic sediments in a brackish lake (Lake Obuchi), facing the Pacific Ocean and adjacent to a nuclear fuel reprocessing plant in northeast Japan, was evaluated using incubation experiments on sediment core samples. The experiments were performed under three different temperatures (29, 17, and 6 °C) and oxygenic (air flow, N₂ gas flow, and untreated) conditions for 48 h. The total dissolved iodine (TDI) concentration (i.e., the sum of iodide, iodate, and dissolved organic iodine, DOI) increased under all temperatures and oxygenic conditions in the first 6 h of incubation. From 6 to 27 h, noticeable increases in TDI concentration only occurred at high temperatures. Dissolution fluxes of iodine estimated by linear regression analysis of the measured TDI concentration in the first 6 h were always higher than those estimated in the first 27 h. This result indicates that dissolution flux of iodine should be evaluated through short-term (within several hours) incubation experiments because absorption reactions which transport iodine from the overlying water back to the sediment become active in the long-term. No substantial difference in dissolution flux, estimated by TDI concentration, was observed under different oxygenic conditions in the first 6 h. However, dissolution flux increased significantly with an increase in temperature. Increases in flux and temperature were significantly and positively correlated (R² = 0.90), suggesting that temperature was the dominant factor that regulated iodine flux during the incubation. Changes in TDI concentration at all temperatures and oxygenic conditions corresponded to those in iodide concentration, indicating that iodide was the main form of iodine dissolved from the sediments. In later stages of the experiments, from 27 to 48 h, the TDI concentration in overlying water increased only at high temperature, while concentrations at medium and low temperatures remained constant or decreased. In particular, oxic experiments showed substantial decreases in iodide concentration at medium and low temperatures. This suggests that oxic conditions promote the absorption of iodine from the overlying water to the sediments. Finally, the dissolution flux of radioiodine (iodine-129) from the sediments of Lake Obuchi to the overlying water was estimated by combining these results with data from earlier studies. The results suggest that only 0.006% of the iodine-129 accumulated in the sediments is released through dissolution to the overlying water per year, suggesting that this radioactive isotope is essentially stable in the sediments.

Keywords: Coastal area; Incubation experiments; Iodine; Lake Obuchi; Nuclear fuel reprocessing; Sediment cores.