Influence of tritium exposure route on vegetation types at the Savannah River Site.

Plant, soil, water, and other media from various locations at the Savannah River Site were measured for total tritium (T) content and T speciation to characterize T in these areas, as well as investigate its uptake behavior and the transport of T species in these media. This characterization included the isolation and measurement of T in tritiated water (HTO), and (when possible) exchangeable organic bound T (E-OBT) and non-exchangeable organic bound T (NE-OBT). Two areas of interest were investigated: (1) a holding pond with T-contaminated water and (2) open basins or streams with low to background levels of T. Water in the holding pond is used to irrigate forest plots in the local area as a T remediation approach. This study compares the analytical data for water, soil/sediment, plants, and lichens from these locations. The results indicate that the behavior of T in plants from these areas can be a function of one or more of the following: seasonal precipitation, the plant's primary route of access to the T-contamination (such as water uptake through the root vs. shoot), plant physical location (relative to T-contaminated water sources), plant rooting depth, pond water level, and plant height above the ground. Total T concentrations were lowest in the un-irrigated forest plants, followed by irrigated forest plants, shallow rooting plants near the pond, deep rooting plants further from the pond, and then water-saturated plants. The OBT:HTO and NE-OBT:E-OBT ratios were always greater for plants from irrigated forest plots compared to those from the holding pond.

Influence of irrigation approaches and spatial geolocation on tritium speciation, uptake and depuration.

Pine needles and tree cores from a tritium (T) contaminated phytoremediation forest at the Savannah River Site (SRS in Aiken, SC) Mixed Waste Management Facility (MWMF) were measured for total T and T speciation and compared to other locations at the SRS and the surrounding area. Tree core ages ranged from 9 to 14 years old, covering over half of the ∼20-year on-going remediation efforts, while pine needles represent more recent time periods of 1-to-2-year increments. Remedial irrigation efforts at the MWMF are found to directly influence the pine needle T concentrations. The T content in the MWMF samples is higher than non-irrigated needle samples from other locations around the SRS. Further, the different forms of organic bound T are preferentially stored in tree core tissue, compared to pine needles where tritiated water dominates.

Historical record of tritium from tree cores at the Savannah River Site.

Tree cores from various locations at the Savannah River Site (SRS) and local area were measured for total tritium (T) content and T speciation to include tritiated water (HTO), exchangeable organic bound T (E-OBT) and non-exchangeable organic bound T (NE-OBT) species. The tree cores dated back to the 1960's or prior which provided an opportunity to measure T over the last 60-70 years. The total T levels from pine and oak tree cores were consistent with the record of known T atmospheric releases from nuclear activities at the SRS between the mid-1950's and 1990's with a notable peak in T tree core levels during the late 1960's. The T speciation data for some tree core samples from SRS demonstrated elevated levels of OBT : HTO and NE-OBT : E-OBT identified primarily in the last ∼20 years due to T inputs from remedial irrigation with OBT-rich pond water. Elevated but lower levels of OBT : HTO and NE-OBT : E-OBT were observed due to inputs from SRS operations during the last 70 years and prior to irrigation with the T-rich pond water.

Comparing and contrasting In-Vial and full-scale systems for sparging volatile analytes.

In-vial sparging was demonstrated as an effective, practical alternative to a full-scale sparging system for supporting the analysis of volatile constituents. Using elemental mercury (Hg0) and toluene as representative purgeable analytes, the mass removal for various sparge configurations was measured and a reduced order model was developed and validated. In the primary experiments, Hg0 in the sparge gas was trapped on activated carbon or gold, thermally desorbed, and quantified using atomic absorption or atomic fluorescence spectroscopy. Toluene experiments using the same in-vial sparge apparatus and sparge parameters were performed to demonstrate the applicability of the reduced order model to a broad range of compounds. Toluene removal was tracked by measuring the remaining toluene in sparged aliquots using Ultraviolet-visible (UV-Vis) spectroscopy. For the sparging, flow rates varied from 25 to 75 mL/min for periods from 0 to 30 min. Sparge performance, mass removal as a function of time, and sparge gas volume were measured for both in-vial and full-scale systems. A model based on dimensionless Henry's Law coefficient, normalized sparge gas volume, and fractional extent of equilibrium matched the experimental data for both compounds and provides a practical tool for future applications. For the conditions tested in this study, the calibrated model indicated that the sparge gas in the in-vial system reached approximately 33% of its equilibrium value before exiting the water surface, while a full-scale system reached approximately 100%. The tests validated the quality, reproducibility, and predictability of sparging performance for both full scale and in-vial sparge systems. Related factors such as waste generation, worker risk, and labor were also assessed. Full scale sparge systems provide the advantage of lower detection levels due to larger sample volume, while the in-vial sparge systems provide advantages for most other factors; including automatability, reducing secondary wastes, lessening the need to clean and check the sparge apparatus, and lowering labor and costs. The data and associated reduced order model support continued development and deployment of in-vial sparge platforms as a practical option for analysis of purgeable analytes such as volatile organic compounds and volatile metals/organometallics.