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.     

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.     

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.     

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.     

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.     

Tritium levels in Chinese cabbage and radish plants acutely exposed to HTO vapor at different growth stages

To simulate an acute exposure of Chinese cabbage and radish plants to airborne HTO, the potted plants were exposed to HTO vapor under semi-outdoor conditions for 1h at different times from the early to late growth stages. The plants were grown outdoors and the plant tritium was measured at the end of an exposure (h(0)) and at harvest. The leaf tissue free water tritium (TFWT) concentrations at h(0) were considerably lower than estimated equilibrium concentrations. In the leaves of Chinese cabbage, the exposure at the earlier growth stage generally ended with a higher TFWT concentration. Such a tendency was not apparent either in the leaves or roots of radish. On the other hand, the earlier stage exposure gave rise to lower TFWT concentrations at the harvest of both crops. For the OBT (organically bound tritium), however, the same occurred only in the Chinese cabbage leaves. During the period between the exposure and harvest, the TFWT concentrations reduced by factors of up to 1.1 x 10(6) for the Chinese cabbage leaves and 1.3 x 10(4) for the radish roots. Based on the activity ratios of OBT to TFWT at harvest, it is estimated that OBT mostly contributes much more to the ingestion dose than TFWT does.     

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.     

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.     

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.     

Tritium profiles in snowpacks

The release of tritiated water (HTO) to the atmosphere during the winter can contribute significantly to snow contamination and to water-soil-plant contamination after the spring thaw. The dose significance of such a release depends on the persistence of tritiated water in the snowpack, which is primarily controlled by the HTO diffusion process in snow and the rate of re-emission into the atmosphere from the snowpack surface. Monitoring data collected after an acute winter release at Chalk River Laboratories and data obtained in winter over a chronically contaminated area were analyzed to estimate the diffusion coefficient of HTO in the snowpack. Under conditions of cold and dry snow, the diffusion coefficient lay in the range 1-2 × 10⁻¹⁰ m² s⁻¹, an order of magnitude lower than diffusion in water but an order of magnitude higher than self-diffusion in ice. These results confirm the theoretical predictions (Bales, 1991). Values up to six times higher were found for warmer periods and just before spring melt, when other processes contribute to profile evolution. The low diffusion rate of tritium in cold, dry snow means that tritium remains in the snowpack throughout the winter, to be released during spring thaw to potentially contaminate surface water, soil and crops.     

Recent Cs deposition in sediments of Admiralty Bay, Antarctica

Cesium-137, radium-226 and lead-210 profiles of a 25 cm sediment core give an indication of recent changes in land-ocean interactions at a polar coastal environment (Admiralty Bay, King George Island, Antarctica). The linear sedimentation accumulation rate at the study site calculated from the unsupported ²¹⁰Pb profile was 6.7 mm/year from 1965 to 2005. A 3.5-fold increase in ¹³⁷Cs concentrations was observed in the top layer of this sediment core. This sharp increase seems to indicate a recent redistribution of fallout radionuclides previously deposited on soil, vegetation and snow. These results imply enhanced land-ocean interactions at this site likely as a result of climate change. Because our results are based on a single core, additional investigations are needed to confirm our observations.     

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.     

Radiocaesium fallout behaviour in volcanic soils in Iceland

The retention of 137Cs in various types of Andosols in Iceland was investigated. Soils were sampled at 29 sites with varying precipitation and environmental conditions. Samples were obtained from 0 to 5, 5 to 10, and 10 to 15 cm depths. The amount of radiocaesium present was quite variable, ranging between 300 and 4800 Bq m(-2) and correlated closely to total annual precipitation (r2=0.71). The majority of 137Cs, 82.7% on average, was retained in the uppermost 5 cm of the soil. The greatest penetration of 137Cs was observed for organic Histosols (76.3% in top 5 cm). The Icelandic Vitrisols (barren, poorly developed Andosols) are coarse grained with only 2-5% clay content and contain little organic matter (<1%). Yet these soils retained 74% of 137Cs in the top 5 cm. The results indicate that radiocaesium fallout is strongly retained by colloidal materials characteristic of Andosols, such as allophane and ferrihydrite. Most soils in Iceland are subject to severe and prolonged freezing and waterlogging; despite this, 137Cs is retained in the upper soil horizons and vertical migration is negligible in Icelandic Andosols. However, erosion and aeolian activity can markedly influence the amount and vertical distribution of radiocaesium in Icelandic soils.     

Rodents as receptor species at a tritium disposal site

New methods are being employed on the Department of Energy's Savannah River Site to deal with the disposal of tritium, including the irrigation of a hardwood/pine forest with tritiated water from an intercepted contaminant plume to reduce concentrations of tritium outcropping into Fourmile Branch, a tributary of the Savannah River. The use of this system has proven to be an effective means of tritium disposal. To evaluate the impact of this activity on terrestrial biota, rodent species were captured on the tritium disposal site and a control site during two trapping seasons in order to assess tritium exposure resulting from the forest irrigation. Control site mice had background levels of tritium, 0.02 Bq/mL, with disposal site mice having significantly higher tritium concentrations, mean=34.86 Bq/mL. Whole body tritium concentrations of the mice captured at the disposal site were positively correlated with tritium application and negatively correlated with precipitation at the site.     

Biotic, temporal and spatial variability of tritium concentrations in transpirate samples collected in the vicinity of a near-surface low-level nuclear waste disposal site and nearby research reactor

The results of a 21 month sampling program measuring tritium in tree transpirate with respect to local sources are reported. The aim was to assess the potential of tree transpirate to indicate the presence of sub-surface seepage plumes.Transpirate gathered from trees near low-level nuclear waste disposal trenches contained activity concentrations of ³H that were significantly higher (up to ∼700 Bq L⁻¹) than local background levels (0-10 Bq L⁻¹). The effects of the waste source declined rapidly with distance to be at background levels within 10s of metres. A research reactor 1.6 km south of the site contributed significant (p < 0.01) local fallout ³H but its influence did not reach as far as the disposal trenches.The elevated ³H levels in transpirate were, however, substantially lower than groundwater concentrations measured across the site (ranging from 0 to 91% with a median of 2%). Temporal patterns of tree transpirate ³H, together with local meteorological observations, indicate that soil water within the active root zones comprised a mixture of seepage and rainfall infiltration. The degree of mixing was variable given that the soil water activity concentrations were heterogeneous at a scale equivalent to the effective rooting volume of the trees. In addition, water taken up by roots was not well mixed within the trees. Based on correlation modelling, net rainfall less evaporation (a surrogate for infiltration) over a period of from 2 to 3 weeks prior to sampling seems to be the optimum predictor of transpirate ³H variability for any sampled tree at this site.The results demonstrate successful use of ³H in transpirate from trees to indicate the presence and general extent of sub-surface contamination at a low-level nuclear waste site.     

Analysis of radiocaesium in the Lebanese soil one decade after the Chernobyl accident

Fallout from the Chernobyl reactor accident due to the transport of a radioactive cloud over Lebanon in the beginning of May 1986 was studied 12 years after the accident for determining the level of (137)Cs concentration in soil. Gamma spectroscopy measurements were performed by using coaxial high sensitivity HPGe detectors. More than 90 soil samples were collected from points uniformly distributed throughout the land of Lebanon in order to evaluate their radioactivity. The data obtained showed a relatively high (137)Cs activity per surface area contamination, up to 6545Bqm(-2) in the top soil layer 0-3cm. The average activity of (137)Cs in the top soil layer 0-3cm in depth was 59.7Bqkg(-1) dry soil ranging from 15 to 119Bqkg(-1) dry soil. The horizontal variability was found to be about 45% between the sampling sites. The depth distribution of total (137)Cs activity in soil showed an exponential decrease. Estimation of the annual effective dose due to external radiation from (137)Cs contaminated soil for selected sites gave values ranging from 19.3 to 91.6 micro Svy(-1).     

Fate of Co at a sludge land application site

Vertical distributions of ⁶⁰Co are determined in soil cores obtained from a 10-ha grassland, where anaerobically digested sludge was applied by surface spraying from 1986 to 1995 on the U.S. Department of Energy's Oak Ridge Reservation. These results, along with historical application records, are used to estimate vertical-migration rates and perform a mass balance. The presence of ⁶⁰Co results solely from the sludge-application process. Soil, vegetation, and surface-water samples were collected. Eleven soil cores were sectioned into 3-cm increments and analyzed by gamma-ray spectrometry. No ⁶⁰Co was detected in the vegetation or water samples. The downward migration rate of ⁶⁰Co in the upper 15 cm of soil ranged from 0.50 to 0.73 cm/yr. About 98%, 0.020 ± 0.011 Bq/cm², of ⁶⁰Co remained in the upper 15 cm of soil, which compared favorably with the expected ⁶⁰Co activity based on historical records of 0.019 ± 0.010 Bq/cm².     

Extraction of fallout 210Pb from soils and its distribution in soil profiles

Natural fallout ²¹⁰Pb may be extracted from soils with hot, dilute nitric acid without extracting significant quantities of ²¹⁰Pb produced by decay of radon in the soil. This method was used to determine the distribution of fallout ²¹⁰Pb in the profiles of nine New Zealand soils. The measured levels were similar to equilibrium cumulative depositions calculated from deposition records. The results indicate that these soils have quantitatively retained fallout ²¹⁰Pb, with 75–100% of it being concentrated in the top 10 cm of soil. This permanent retention of fallout lead by soils suggests that accumulation of lead in the upper soil layer is likely in areas of aerosol lead pollution.     

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.