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.     

Tissue free water tritium and organically bound tritium in the rice plant acutely exposed to atmospheric HTO vapor under semi-outdoor conditions.

Potted rice plants were exposed to atmospheric HTO in a box outdoors for 1 h at 9 different times from booting to yellow-ripe stages. It is indicated that the leaf TFWT concentration may reach equilibrium within 1 h in clear weather. The plant TFWT concentration decreased at a rapid rate for the first several hours and at a much slower rate thereafter. The decrease till harvest was by factors of 600-95,000 depending on the plant parts and exposure times. The time course of the ear OBT concentration was characterized by the exposure time. After exposure at the booting to heading stages, the leaf OBT concentration decreased rapidly for the first several hours and then very slowly. The plant OBT concentration was initially about 2 orders of magnitude lower, but at harvest an order of magnitude higher, than the TFWT concentration. The OBT concentration in hulled seeds at harvest varied with exposure times by a factor of 70, being highest in the exposure performed at the earlier stage of rapid grain growth. Also in this exposure, the plant total OBT was greatest due to the seed OBT.     

Fate of HTO following its acute soil deposition at different growth stages of Chinese cabbage

Lysimeter experiments were carried out in a greenhouse to study the fate of HTO following its soil deposition at different growth stages of Chinese cabbage. An HTO solution was applied to the surface of an acidic sandy soil at a time before, and four different times after, sowing. The transfer of HTO to the plants was quantified with the areal transfer factor (TFa, m2 kg(-1)-fresh) defined as the ratio of the plant concentration at harvest to the areal activity deposition. In the four post-sowing applications, the TFa values were in the ranges of 1.6 x 10(-5)-4.9 x 10(-3) for TFWT and 4.5 x 10(-6) -4.3 x 10(-5) for OBT, increasing with a decrease in the time interval between application and harvest. In the pre-sowing application, which was followed by a soil mixing, the TFa values for TFWT and OBT were 1.3 x 10(-4) and 8.6 x 10(-6), respectively. One week after harvest, soil samplings were made for the applications at 26 (A(26)) and 63d (A(63)) after sowing. Peaks of the depth profiles of the soil HTO appeared in the 10-15 cm layer for A(26) and the 5-10 cm layer for A(63). The top 30 cm of soil contained 0.5% and 20% of the applied activity for A(26) and A(63), respectively. Negligible fractions seemed to be in the deeper zone. It was estimated that almost all or most of the applied HTO had escaped to the air before plants' harvest.     

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.     

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.     

Intercomparison of model predictions of tritium concentrations in soil and foods following acute airborne HTO exposure

This paper describes the results of a model intercomparision exercise for predicting tritium transport through foodchains. Modellers were asked to assume that farmland was exposed for one hour to an average concentration in air of 10⁴ MBq tritium m^-3. They were given the initial soil moisture content and 30 days of hourly averaged historical weather and asked to predict HTO and OBT concentrations in foods at selected times up to 30 days later when crops were assumed to be harvested. Two fumigations were postulated, one at 10.00 h (i.e., in day-light), and the other at 24.00 h (i.e., in darkness).Predicted environmental media concentrations after the daytime exposure agreed within an order of magnitude in most cases. Important sources of differences were variations in choices of numerical values for transport parameters. The different depths of soil layers used in the models appeared to make important contributions to differences in predictions for the given scenario. Following the night-time exposure, however, greater differences in predicted concentrations appeared. These arose largely because of different ways key processes were assumed to be affected by darkness. Uptake of HTO by vegetation and the rate it is converted to OBT were prominent amongst these processes. Further research, experimental data and modelling intercomparisons are required to resolve some of these issues.     

Organically bound tritium (OBT) for various plants in the vicinity of a continuous atmospheric tritium release

In order to quantify tritium impact on the environmental, we studied vegetation continuously exposed to a tritiated atmosphere. We chose lichens as bio-indicators, trees for determination of past tritium releases of the Valduc Centre, and lettuce as edible vegetables for dose calculation regarding neighbourhood. The Pasquill and Doury models from the literature were tested to estimate tritium concentration in the air around vegetable for distance from the release point less than 500m. The results in tree rings show that organically bound tritium (OBT) concentration was strongly correlated with tritium releases. Using the GASCON model, the modelled variation of OBT concentration with distance was correlated with the measurements. Although lichens are recognized as bio-indicators, our experiments show that they were not convenient for environmental surveys because their age is not definitive. Thus, tritium integration time cannot be precisely determined. Furthermore, their biological metabolism is not well known and tritium concentration appears to be largely dependent on species. An average conversion rate of HTO to OBT was determined for lettuce of about 0.20-0.24%h(-1). Nevertheless, even if it is equivalent to values already published in the literature for other vegetation, we have shown that this conversion rate, established by weekly samples, varies by a factor of 10 during the different stages of lettuce development, and that its variation is linked to the biomass derivative.     

Uptake of deuterium by dead leaves exposed to deuterated water vapor in a greenhouse at daytime and nighttime

Dead leaves were exposed to deuterated water vapor (D(2)O) as a substitute of tritiated water (HTO) in a greenhouse at daytime and nighttime to examine uptake and release of tritium by dead leaves because they cover a wide area of the forest floor and are therefore a major target material to be exposed when HTO is atmospherically derived to the forest. The dead cedar needles showed faster uptake and faster release rates during and after the exposure than the fresh ones, and the equilibrium concentration of the dead cedar needles was about two times higher than the fresh ones, indicating a quick response and a high buffering potential of dead leaves. The relation between uptake of D(2)O and number of stoma was examined for dead deciduous leaves; the species with larger number of stoma accumulated more D(2)O at the daytime and nighttime exposures. However, drying of the dead leaves suppressed D(2)O uptake greatly at daytime, suggesting stomata's opening and closing controls the D(2)O uptake of dead leaves.     

Determination of organically bound tritium background level in biological samples from a wide area in the south-west of France

In this paper, the authors describe a sensitive method for low-level non-exchangeable OBT determination. This methodology combines suitable sample treatment, a combustion apparatus for large-sized samples and low-background liquid scintillation spectrometry, along with precautions that substantially reduce the risks of sample contamination. Great care must be taken in the measurement of non-exchangeable OBT at environmental levels. Many authors have discussed the opportunities for cross-contamination between samples and contamination by exchange with the laboratory atmosphere. The authors also describe an application of the methodology to a large-scale sampling and measurement campaign, aimed at the determination of the environmental non-exchangeable OBT background level in tree leaves and ferns collected on the site and in the vicinity of a research centre located in the south-west of France, not far from Bordeaux. This study constitutes a "zero level" for the non-exchangeable OBT activity, as, to our knowledge, there is no tritium source within or in the surroundings of the sampled area capable of producing non-exchangeable OBT activities above the natural levels. Our analyses showed that non-exchangeable OBT activities in the collected samples were very low, ranging from below the detection limit (ca 0.7 Bq kg(-1) of dry material) to ca 2 Bq kg(-1) of dry material. These values are similar to the natural tritium background measured in water samples. No discrepancies can be shown between fern samples and oak tree leaf samples or between samples collected inside and outside the research site.     

A dynamic model for assessing radiological consequences of tritium routinely released in rivers. Application to the Loire River

A dynamic model for assessing the transfer of tritium in a food chain was applied to the Loire River, where 14 nuclear power plants situated on five different sites operate. The model considers several potential exposure pathways in the aquatic and terrestrial ecosystems: transfer of tritium through the aquatic food chain (especially fish); use of river water for agricultural purposes (irrigation) and transfer of radionuclides through the terrestrial food chain (vegetables, meat, milk); subsequent internal exposure of humans due to ingestion of contaminated foodstuffs. For biological environmental compartments, the transfer of tritium to organic matter (i.e. OBT) was simulated. For each of the parameters introduced in this model, a probability density function, allowing further uncertainty and sensitivity analyses, was proposed. Uncertainty/sensitivity analyses were performed to determine a confidence interval for the mean annual dose to critical groups and to identify the parameters responsible for the uncertainty and subsequent research priorities.     

Tritium concentrations in the atmospheric environment at Rokkasho, Japan before the final testing of the spent nuclear fuel reprocessing plant

This study aimed at obtaining background tritium concentrations in precipitation and air at Rokkasho where the first commercial spent nuclear fuel reprocessing plant in Japan has been under construction. Tritium concentration in monthly precipitation during fiscal years 2001-2005 had a seasonal variation pattern which was high in spring and low in summer. The tritium concentration was higher than that observed at Chiba City as a whole. The seasonal peak concentration at Rokkasho was generally higher than that at Chiba City, while the baseline concentrations of both were similar. The reason for the difference may be the effect of air mass from the Asian continent which is considered to have high tritium concentration. Atmospheric tritium was operationally separated into HTO, HT and hydrocarbon (CH₃T) fractions, and the samples collected every 3 d-14 d during fiscal year 2005 were analyzed for these fractions. The HTO concentration as radioactivity in water correlated well with that in the precipitation samples. The HT concentration was the highest among the chemical forms analyzed, followed by the HTO and CH₃T concentrations. The HT and CH₃T concentrations did not have clear seasonal variation patterns. The HT concentration followed the decline previously reported by Mason and Östlund with an apparent half-life of 4.8 y. The apparent and environmental half-lives of CH₃T were estimated as 9.2 y and 36.5 y, respectively, by combining the present data with literature data. The Intergovernmental Panel on Climate Change used the atmospheric lifetime of 12 y for CH₄ to estimate global warming in its 2007 report. The longer environmental half-life of CH₃T suggested its supply from other sources than past nuclear weapon testing in the atmosphere.     

Deposition of gaseous radionuclides to fruit

14C, 35S and 3H are released to the environment during the operation of gas-cooled reactors and were identified as radionuclides of interest by the BIOMASS Fruits Working Group. This paper provides a review of the deposition, uptake, allocation and loss of these radionuclides with respect to fruit and conceptual models for gaseous radionuclides. It is concluded that the mechanisms for the uptake of CO35S, HTO and 14CO2 are well understood and that their deposition velocities have been quantified. There is also a reasonable body of work on the translocation of 14C once in the crop, but much less for 35S and 3H, which are considered to follow source-sink relationships. The loss rates of the three radionuclides show large differences, with tritium lost rapidly in the form of HTO but retained longer when converted to OBT. The losses of 14C are less and those of sulphur are minimal post fixation. When fruit crops alone are considered, the quantity of information is further reduced but predictions on possible behaviour of these radionuclide species can be made from the current knowledge.     

Re-emission of heavy water vapour from soil to the atmosphere

The re-emission process of tritiated water (HTO) deposited on a soil surface is an important process to assess tritium doses to the general public around nuclear fusion facilities in future. A field experiment using heavy water (HDO) as a substitute for HTO was carried out in the summertime to investigate the re-emission process of HTO from soil to the atmosphere. In the experiment, the time variations of depth profiles of HDO concentrations in soil exposed to HDO vapour and soil mixed with HDO were measured during the re-emission process on the field. The HDO concentrations in soil water in top soil layers of both the exposed and mixed soil rapidly decreased with time during the re-emission. However, the decrease of exposed soil was much greater than that of mixed soil. The re-emission process was analysed using a model including the evaporation of HDO from soil, the exchange between soil HDO and air H2O, and the diffusion of HDO in soil. It was found that the model is applicable to calculating the time variations of detailed depth profiles of HDO concentration in soil water in surface soil layers, using an estimated exchange velocity.     

Foliar contamination of Phaseolus vulgaris with aerosols of 137Cs, 85Sr, 133Ba and 123mTe: influence of plant development stage upon contamination and rain

As part of a requirement to improve the assessment of the impact of radioactive fallout on consumed agricultural products, bean plants at four development stages (seedlings, preflowering, late flowering and mature plants) were contaminated by dry deposition of (137)Cs, (85)Sr, (133)Ba and (123m)Te aerosols. The influence of two rain scenarios and of the development stage upon contamination on interception, retention, and translocation to pods was studied. Interception of the four radionuclides was almost identical and varied from 30 to 60% with increasing development stage. The most important rain parameter was the time which elapsed between contamination and the first rain. Whatever the development stage, rain washed off more cesium from the leaves when it occurred 2 days after the deposit (37% at the seedling stage, for example) rather than later on (6 days, 27%), due to rapid migration of Cs in the plant. The first rain washed off nearly 40% of Ba whatever the scenario. For later stages, Sr and Ba were more washed off by heavy weekly rains than by weak twice-a-week rains, perhaps because of the Sr/Ba-contaminated material loss associated with wash off (desquamation of cuticles). Te showed little wash off (less than 5%). Wash off decreased with an older development stage for a weak rain intensity, due to the superimposition of leaves. Heavy rains removed this shelter effect. At harvest, rain effect was no longer detectable as foliar activity was similar for both rain scenarios. Translocation factors (TF) for strontium and barium increased from 6 x 10(-3) to 1 x 10(-1) with the plant development stage upon contamination, whereas those for cesium remained almost unchanged between 2 x 10(-1) and 4 x 10(-1). Flowering is the most critical stage towards residual contamination in pods at harvest, with the exception of direct deposit on pods at the mature stage (TF values are one order of magnitude higher). TF value for Te was 6.5 x 10(-2) and was due to direct deposit. Modelling reflected the trends, through the differential values of the wash off and absorption coefficients, of what was reported for experimental results.     

Soil-to-plant halogens transfer studies 1. Root uptake of radioiodine by plants

Long-term controlled experiments under natural conditions in the field have been carried out in the Chernobyl Exclusion zone in order to determine the parameters governing radioiodine transfer to plants from four types of soils (podzoluvisol, greyzem and typical and meadow chernozem) homogeneously contaminated in the 20-cm upper layer with an addition of (125)I. An absence of (125)I depletion in arable soil layers due to volatilization was noted up to one year after contamination. During one year, depletion due to the vertical migration of radioiodine from the arable layer of each of the soils did not exceed 4% of the total (125)I content. Radioiodine concentration ratios (CR) were obtained in radish roots, lettuce leaves, bean pods, and wheat grain and straw. The highest CR values were observed in podzoluvisol: 0.01-0.03 for radish roots and lettuce leaves, 0.003-0.004 for bean pods and 0.001 for wheat grains. In the other three soils, these values were one order of magnitude lower. The parameters relating to changes in radioiodine bioavailability were determined, based on the contamination dynamics of plants in field conditions.     

Selenium bioavailability and uptake as affected by four different plants in a loamy clay soil with particular attention to mycorrhizae inoculated ryegrass

The aim of this study was to investigate the influence of plant species, especially of their rhizosphere soil, and of inoculation with an arbuscular mycorrhizal (AM) fungus on the bioavailability of selenium and its transfer in soil-plant systems. A pot experiment was performed with a loamy clay soil and four plant species: maize, lettuce, radish and ryegrass, the last one being inoculated or not with an arbuscular mycorrhizal fungus (Glomus mosseae). Plant biomass and Se concentration in shoots and roots were estimated at harvest. Se bioavailability in rhizosphere and unplanted soil was evaluated using sequential extractions. Plant biomass and selenium uptake varied with plant species. The quantity of rhizosphere soil also differed between plants and was not proportional to plant biomass. The highest plant biomass, Se concentration in plants, and soil to plant transfer factor were obtained with radish. The lowest Se transfer factors were obtained with ryegrass. For the latter, mycorrhizal inoculation did not significantly affect plant growth, but reduced selenium transfer from soil to plant by 30%. In unplanted soil after 65 days aging, more than 90% of added Se was water-extractable. On the contrary, Se concentration in water extracts of rhizosphere soil represented less than 1% and 20% of added Se for ryegrass and maize, respectively. No correlation was found between the water-extractable fraction and Se concentration in plants. The speciation of selenium in the water extracts indicated that selenate was reduced, may be under organic forms, in the rhizosphere soil.     

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.     

Soil-to-plant halogens transfer studies 2. Root uptake of radiochlorine by plants

Long-term field experiments have been carried out in the Chernobyl exclusion zone in order to determine the parameters governing radiochlorine (36Cl) transfer to plants from four types of soil, namely, podzoluvisol, greyzem, and typical and meadow chernozem. Radiochlorine concentration ratios (CR) in radish roots (15+/-10), lettuce leaves (30+/-15), bean pods (15+/-11) and wheat seed (23+/-11) and straw (210+/-110) for fresh weight of plants were obtained. These values correlate well with stable chlorine values for the same plants. One year after injection, 36Cl reached a quasi-equilibrium with stable chlorine in the agricultural soils and its behavior in the soil-plant system mimicked the behavior of stable chlorine (this behavior was determined by soil moisture transport in the investigated soils). In the absence of intensive vertical migration, more than half of 36Cl activity in arable layer of soil passes into the radish, lettuce and the aboveground parts of wheat during a single vegetation period.     

Background exposure rates of terrestrial wildlife in England and Wales

It has been suggested that, when assessing radiation impacts on non-human biota, estimated dose rates due to anthropogenically released radionuclides should be put in context by comparison to dose rates from natural background radiation. In order to make these comparisons, we need data on the activity concentrations of naturally occurring radionuclides in environmental media and organisms of interest. This paper presents the results of a study to determine the exposure of terrestrial organisms in England and Wales to naturally occurring radionuclides, specifically (40)K, (238)U series and (232)Th series radionuclides. Whole-body activity concentrations for the reference animals and plants (RAPs) as proposed by the ICRP have been collated from literature review, data archives and a targeted sampling campaign. Data specifically for the proposed RAP are sparse. Soil activity concentrations have been derived from an extensive geochemical survey of the UK. Unweighted and weighted absorbed dose rates were estimated using the ERICA Tool. Mean total weighted whole-body absorbed dose rates estimated for the selected terrestrial organisms was in the range 6.9 x 10(-2) to 6.1 x 10(-1) microGy h(-1).     

Assessing potential risks from exposure to natural uranium in well water

Over 50% of the wells in the Nambe region of northern New Mexico exceed the US Environmental Protection Agency's recommended drinking water standard of 20 microg l(-1) for 238U; the highest in the area was measured at 1,200 microg U l(-1). Uranium uptake was estimated in tomato (Lycopersicon esculentum), squash (Cucurbita pepo), lettuce (Lactuca scarriola), and radish (Raphanus sativus) irrigated with Nambe well water containing <1, 150, 500, and 1,200 microg U l(-1). Plant uptake and human dose and toxicity associated with ingestion of water and produce and inhalation of irrigated soil related to gardening activities were evaluated. Uranium concentration in plants increased linearly with increasing U concentration in irrigation water, particularly in lettuce and radish. The estimated total committed effective dose for 70 years of maximum continuous exposure, via the three pathways to well water containing 1,200 microg U l(-1), was 0.17 mSv with a corresponding kidney concentration of 0.8 microg U g(-1) kidney.