Tracing the Transport, Geochemical Cycling and Fate of Iodine-129 in Earth Surface Reservoirs

Iodine-129 is a naturally and anthropogenically produced radioisotope (half-life: 15.7 million years) the majority of which is produced by nuclear fuel reprocessing. These releases have dispersed 129I throughout the environment making it possible to use 129I as a tracer. It is also of concern for the disposal of radioactive waste. This research develops a new laboratory method for 129I extraction and analysis, and explores the geochemical cycling and environmental fate of 129I in remote catchments following the Fukushima-Daiichi Nuclear Accident (FDNA). A new technique was developed to investigate 129I partitioning and quantitatively extract it from solid samples. Samples are combusted and volatilized iodine is trapped in solution. The efficiency is traced using the iodine isotope, 125I. This technique was proven using standard reference materials and is used in other chapters of this thesis. A baseline study of 129I in Yukon watersheds was undertaken to determine the impact of anthropogenic 129I emissions and identify possible sources. Using atmospheric back-trajectory modeling, sources of 129I from Fukushima, nuclear fuel reprocessing and marine volatilization were identified in remote watersheds. Peat moss samples showed significant retention of 129I in modern samples. Following the reconnaissance study, a catchment scale investigation of anthropogenic 129I cycling was undertaken through precipitation and runoff monitoring. 129I was found to be an excellent indicator of initial snowmelt contributions to discharge due to enrichment by dry deposition. Furthermore, water source transitions in discharge were recorded by 129I, 127I and the 129I/127I ratio showing iodine can be used as a tracer of hydrologic processes. A mass balance found that 77% of the 129I mass input accumulates annually, primarily in organic soils. Sampling of Vancouver, B.C. precipitation and groundwater was done following the FDNA to determine the fate of 129I and evaluate it as a tracer of groundwater recharge. Immediately following the FDNA the 129I concentration in precipitation increased 6 times above background. Groundwater samples also showed 129I increases consistent with expected recharge times indicating FDNA derived 129I was transported into groundwater with minimal retardation, likely via preferential flowpaths