Measured and modelled tritium concentrations in freshwater Barnes mussels (Elliptio complanata) exposed to an abrupt increase in ambient tritium levels

To improve understanding of environmental tritium behaviour, the International Atomic Energy Agency (IAEA) included a Tritium and C-14 Working Group (WG) in its EMRAS (Environmental Modelling for Radiation Safety) program. One scenario considered by the WG involved the prediction of time-dependent tritium concentrations in freshwater mussels that were subjected to an abrupt increase in ambient tritium levels. The experimental data used in the scenario were obtained from a study in which freshwater Barnes mussels (Elliptio complanata) were transplanted from an area with background tritium concentrations to a small Canadian Shield lake that contains elevated tritium. The mussels were then sampled over 88 days, and concentrations of free-water tritium (HTO) and organically-bound tritium (OBT) were measured in the soft tissues to follow the build-up of tritium in the mussels over time.The HTO concentration in the mussels reached steady state with the concentration in lake water within one or two hours. Most models predicted a longer time (up to a few days) to equilibrium. All models under-predicted the OBT concentration in the mussels one hour after transplantation, but over-predicted the rate of OBT formation over the next 24 h. Subsequent dynamics were not well modelled, although all participants predicted OBT concentrations that were within a factor of three of the observation at the end of the study period. The concentration at the final time point was over-predicted by all but one of the models. The relatively low observed concentration at this time was likely due to the loss of OBT by mussels during reproduction.     

HTO and OBT activity concentrations in soil at the historical atmospheric HT release site (Chalk River Laboratories)

Tritium is routinely released by the Chalk River Laboratories (CRL) nuclear facilities. Three International HT release experiments have been conducted at the CRL site in the past. The site has not been disturbed since the last historical atmospheric testing in 1994 and presents an opportunity to assess the retention of tritium in soil. This study is devoted to the measurement of HTO and OBT activity concentration profiles in the subsurface 25 cm of soil.In terms of soil HTO, there is no evidence from the past HT release experiments that HTO was retained. The HTO activity concentration in the soil pore water appears similar to concentrations found in background areas in Ontario. In contrast, OBT activity concentrations in soil at the same site were significantly higher than HTO activity concentrations in soil. Elevated OBT appears to reside in the top layer of the soil (0-5 cm). In addition, OBT activity concentrations in the top soil layer did not fluctuate much with season, again, quite in contrast with soil HTO. This result suggests that OBT activity concentrations retained the signature of the historical tritium releases.     

He mass spectrometry for very low-level measurement of organic tritium in environmental samples

The design, setup and performance of a mass spectrometric system for the analysis of low to very low-level tritium in environmental samples are described. The tritium concentration is measured indirectly by the ³He ingrowth from radioactive decay after complete initial degassing of the sample. The analytical system is fully computer-controlled and consists in a commercial helium isotope mass spectrometer coupled with a high vacuum inlet system. A detection limit of 0.15 Bq/kg is routinely obtainable for sample sizes of 20 g of water equivalent and an accumulation time of three months. Larger samples (and/or longer accumulation time) can be used to obtain lower detection limits. In addition to the benefit of a lower detection limit, another advantage of this non-destructive method lies in the simplicity of the analytical procedure which strongly limits the risk of contamination. An inter-comparison was successfully performed with the conventional beta counting technique on lyophilized grass samples, in a range of tritium concentrations of environmental interest. It shows that the ³He mass spectrometry method yields results that are fully consistent with the conventional liquid scintillation technique over a wide range of tritium concentrations.     

Development and validation of a dynamical atmosphere-vegetation-soil HTO transport and OBT formation model

A numerical model simulating transport of tritiated water (HTO) in atmosphere-soil-vegetation system, and, accumulation of organically bound tritium (OBT) in vegetative leaves was developed. Characteristic of the model is, for calculating tritium transport, it incorporates a dynamical atmosphere-soil-vegetation model (SOLVEG-II) that calculates transport of heat and water, and, exchange of CO₂. The processes included for calculating tissue free water tritium (TFWT) in leaves are HTO exchange between canopy air and leaf cellular water, root uptake of aqueous HTO in soil, photosynthetic assimilation of TFWT into OBT, and, TFWT formation from OBT through respiration. Tritium fluxes at the last two processes are input to a carbohydrate compartment model in leaves that calculates OBT translocation from leaves and allocation in them, by using photosynthesis and respiration rate in leaves. The developed model was then validated through a simulation of an existing experiment of acute exposure of grape plants to atmospheric HTO. Calculated TFWT concentration in leaves increased soon after the start of HTO exposure, reaching to equilibrium with the atmospheric HTO within a few hours, and then rapidly decreased after the end of the exposure. Calculated non-exchangeable OBT amount in leaves linearly increased during the exposure, and after the exposure, rapidly decreased in daytime, and, moderately nighttime. These variations in the calculated TFWT concentrations and OBT amounts, each mainly controlled by HTO exchange between canopy air and leaf cellular water and by carbohydrates translocation from leaves, fairly agreed with the observations within average errors of a factor of two.     

A follow up of the decrease of non exchangeable organically bound tritium levels in the surroundings of a nuclear research center

In the past decades limited amounts of tritium were handled on the CEA site of Bruyères le Châtel with authorised atmospheric releases. A small fraction of the tritium released entered into environmental samples under three forms: (i) as part of free water (TFWT - Tissue Free Water Tritium), or associated with organic matter in two ways; either (ii) bound to the oxygen and nitrogen atoms of the material as exchangeable organically bound tritium (E-OBT), or (iii) bound to carbon atoms as non exchangeable organically bound tritium (NE-OBT). The first two components provide only a picture of atmospheric tritium concentrations at the sampling time as they are in equilibrium with atmospheric moisture and soil humidity. Unlike these exchangeable forms, however, NE-OBT is tightly bound to the organic matter and provides an integrated record of atmospheric tritium during the growing phase of the vegetation. We mapped NE-OBT in tree leaf samples in an area of about 25 × 30 km² around the centre of the CEA site and compared the results with those obtained during a previous sampling exercise in 1989. At this time, the activity levels were almost ten times higher than those observed presently in a similar area almost 20 years later which is consistent with the decrease of atmospheric releases issued from the centre. As the activity levels are now close to environmental background specific attention was also paid to the analytical procedure to ensure reliable low level NE-OBT detection.