Development of a dynamic transfer model of (14)C from the atmosphere to rice plants

A dynamic compartment model was investigated to describe ¹⁴C accumulation in rice plants exposed to atmospheric ¹⁴C with temporally changing concentrations. In the model, rice plants were regarded to consist of three compartments: the ear and the mobile and immobile carbon pools of the shoot. Photosynthetically fixed carbon moves into the ear and the mobile carbon pool, and these two compartments release a part of this carbon into the atmosphere by respiration. Carbon accumulated in the mobile carbon pool is redistributed to the ear, while carbon transferred into the immobile carbon pool from the mobile one is accumulated there until harvest. The model was examined by cultivation experiments using the stable isotope, ¹³C, in which the ratios of carbon photosynthetically fixed at nine times during plant growth to the total carbon at the time of harvest were determined. The model estimates of the ratios were in relatively good agreement with the experimental observations, which implies that the newly developed compartment model is applicable to estimate properly the radiation dose to the neighboring population due to an accidental release of ¹⁴C from nuclear facilities.     

Estimation of 14CO2 flux at soil-atmosphere interface and distribution of 14C in forest ecosystem

To realize the dynamical behavior of 14C among exchangeable carbon reservoirs in terrestrial environment, a method for in situ determination of 14CO2 flux at soil-atmosphere interface and a high flow rate CO2 sampler were developed. This method allowed us to collect integrated quantity of CO2 for determining 14C activity over an extended time period under environmental conditions with minimal site disturbance. The 14CO2 flux from ground surface was estimated to be 1.59 x 10(-5) Bq m (-2) S (-1) in a forest floor with the method. The specific activities of 14C in environmental materials such as some biological and air samples were also determined in the vicinity of the place, where the flux measurement was made, to discuss the behavior of 14C in the forest ecosystem. The results indicated that fresh pine needles had a similar 14C specific activity to the atmospheric CO2 at the same height due to its fairly rapid equilibrium, 14C specific activity in the atmospheric CO2 has a concentration gradient near the ground surface and, at least in this site, CO2 with high 14C specific activity was generated by decomposition of soil organic matter which may be accumulated in soil as a result of former nuclear weapons tests.     

Carbon-14 transfer into rice plants from a continuous atmospheric source: observations and model predictions

Carbon-14 ((14)C) is one of the most important radionuclides from the perspective of dose estimation due to the nuclear fuel cycle. Ten years of monitoring data on (14)C in airborne emissions, in atmospheric CO(2) and in rice grain collected around the Tokai reprocessing plant (TRP) showed an insignificant radiological effect of the TRP-derived (14)C on the public, but suggested a minor contribution of the TRP-derived (14)C to atmospheric (14)C concentrations, and an influence on (14)C concentrations in rice grain at harvest. This paper also summarizes a modelling exercise (the so-called rice scenario of the IAEA's EMRAS program) in which (14)C concentrations in air and rice predicted with various models using information on (14)C discharge rates, meteorological conditions and so on were compared with observed concentrations. The modelling results showed that simple Gaussian plume models with different assumptions predict monthly averaged (14)C concentrations in air well, even for near-field receptors, and also that specific activity and dynamic models were equally good for the prediction of inter-annual changes in (14)C concentrations in rice grain. The scenario, however, offered little opportunity for comparing the predictive capabilities of these two types of models because the scenario involved a near-chronic release to the atmosphere. A scenario based on an episodic release and short-term, time-dependent observations is needed to establish the overall confidence in the predictions of environmental (14)C models.     

Conceptual approaches for the development of dynamic specific activity models of 14C transfer from surface water to humans

Carbon-14 is a particularly interesting radionuclide from the perspective of dose estimation. Many nuclear facilities, including power reactors, release 14C into the environment, and much of this is as 14CO2. This mixes readily with stable CO2, and hence enters the food chain as fundamental biomolecules. This isotopic mixing is often used as the basis for dose assessment models. The present model was developed for the situation of 14C releases to surface waters, where there are distinct changes in the water 14C activity concentrations throughout the year. Complete isotopic mixing (equilibrium) cannot be assumed. The model computes the specific activity (activity of 14C per mass of total C) in water, phytoplankton, fish, crops, meat, milk and air, following a typical irrigation-based food-chain scenario. For most of the biotic compartments, the specific activity is a function of the specific activity in the previous time step, the specific activity of the substrate media, and the C turnover rate in the tissue. The turnover rate is taken to include biochemical turnover, growth dilution and mortality, recognizing that it is turnover of C in the population, not a tissue or an individual, that is relevant. Attention is paid to the incorporation of 14C into the surface water biota and the loss of any remaining 14CO2 from the surface water-air interface under its own activity concentration gradient. For certain pathways, variants in the conceptual model are presented, in order to fully discuss the possibilities. As an example, a new model of the soil-to-plant specific activity relationship is proposed, where the degassing of both 14C and stable C from the soil is considered. Selection of parameter values to represent the turnover rates as modeled is important, and is dealt with in a companion paper.     

The amount and identity of [14C] residues in bluegills (Lepomis macrochirus) exposed to [14C] triclopyr

The level and identity of [¹⁴C] residues in bluegills (Lepomis macrochirus)_exposed to 2.5 mg/L [¹⁴C] triclopyr (3,5,6-trichloro-2-pyridinyloxyacetic acid) have been determined. The highest level of radioactivity observed in the flesh of a fish at any time point (0.13 mg/kg, calculated as equivalent mg triclopyr/kg fish) was less than 5% of the fish exposure level of 2.5 mg/L, while the maximum level in the remainder (head, skin, and viscera) was about 95% (2.33 mg/kg) of the fish exposure level, indicating no concentrating effect. The principal components observed in the fish tissues were triclopyr, 3,5,6-trichloro-2-pyridinol, 2-methoxy-3,5,6-trichloropyridine and a conjugate. These components accounted for greater than 75% of all the residues observed.     

Urinary methyl tert-butyl ether and benzene as biomarkers of exposure to urban traffic

Methyl tert-butyl ether (MTBE) and benzene are added to gasoline to improve the combustion process and are found in the urban environment as a consequence of vehicular traffic. Herein we evaluate urinary MTBE (MTBE-U) and benzene (BEN-U) as biomarkers of exposure to urban traffic. Milan urban policemen (130 total) were investigated in May, July, October, and December for a total of 171 work shifts. Personal exposure to airborne benzene and carbon monoxide (CO), and atmospheric data, were measured during the work shift, while personal characteristics were collected by a questionnaire. A time/activity diary was completed by each subject during the work shift. Spot urine samples were obtained for the determination of MTBE-U and BEN-U. Median personal exposure to CO and airborne benzene were 3.3 mg/m(3) and 9.6 μg/m(3), respectively; median urinary levels in end-of-shift (ES) samples were 147 ng/L (MTBE-U) and 207 ng/L (BEN-U). The time spent on traffic duty at crossing was about 40% of work time. Multiple linear regression models, taking into account within-subject correlations, were applied to investigate the role of urban pollution, atmospheric conditions, job variables and personal characteristics on the level of biomarkers. MTBE-U was influenced by the month of sampling and positively correlated to the time spent in traffic guarding, CO exposure and atmospheric pressure, while negatively correlated to wind speed (R(2) for total model 0.63, P<0.001). BEN-U was influenced by the month and smoking habit, and positively correlated to urinary creatinine; moreover, an interaction between CO and smoking was found (R(2)=0.62, P<0.001). These results suggest that MTBE-U is a reliable marker for assessing urban traffic exposure, while BEN-U is determined mainly by personal characteristics.     

Evaluation of 14C abundance in soil respiration using acclerator mass spectrometry

To clarify the behavior of 14C in terrestrial ecosystems, 14C abundance in soil respiration was evaluated in an urban forest with a new method involving a closed chamber technique and 14C measurement by accelerator mass spectrometry (AMS). Soil respiration had a higher Delta14C than the contemporary atmosphere. This indicates that a significant portion of soil respiration is derived from the decomposition of soil organic matter enriched in 14C by atmospheric nuclear weapons tests, with a notable time lag between atmospheric 14C addition and re-emission from soil. On the other hand, delta14C in soil respiration demonstrated that 14C abundance ratio itself in soil-respired CO2 is not always high compared with that in atmospheric CO2 because of the isotope fractionation during plant photosynthesis and microbial decomposition of soil organic matter. The Delta14C in soil respiration was slightly lower in August than in March, suggesting a relatively high contribution of plant root respiration and decomposition of newly accumulated and/or 14C-depleted soil organic matter to the total soil respiration in August.     

Model simulations of the fate of 14C added to a Canadian shield lake

Carbon-14 was added to the epilimnion of a small Canadian Shield lake to investigate primary production and carbon dynamics. The nature of the spike and subsequent monitoring allowed the investigation of both short-term and longer-term processes relevant to evaluating impacts of accidental and routine releases and of solid waste disposal. Data from this experiment were used in the BIOMOVS II program as a validation test for modelling the fate of the ¹⁴C added to the lake. Four models were used: (1) a simple probabilistic mass balance model of a lake; (2) a relatively complex deterministic model; (3) a complex deterministic model; and (4) a more complex probabilistic model. Endpoints were ¹⁴C concentrations in water, sediment and lake whitefish over a thirteen year period. Each model produced reasonable predictions when compared to the range of the observed data and when uncertainty in model predictions is taken into consideration. The simple lake model did not account for internal recycling of ¹⁴C and, in this respect, its predictions were not as realistic as those of the more complex models for concentrations in water. However, the simple model predictions for the ¹⁴C inventory remaining in lake sediment were closest to the observed values. Overall, the more complex probabilistic model was the most accurate in simulating ¹⁴C concentrations in water and in whitefish but it overestimated ¹⁴C retention in the lake sediments, as did the other complex models. Choice of parameter values for transfer rate to sediment and gaseous evasion are important in influencing model predictions. Although predicted concentrations of ¹⁴C in fish of dynamic models were more accurate than those using equilibrium bioconcentration factors typically used in assessments, large variability in observed ¹⁴C concentrations in whitefish emphasizes the need for a better understanding of the important processes that influence these contaminant concentrations.     

Radiocarbon dating of archaeological samples (sambaqui) using CO(2) absorption and liquid scintillation spectrometry of low background radiation

Sambaqui means, in the Tupi language, a hill of shells. The sambaquis are archaeological sites with remains of pre-historical Brazilian occupation. Since the sambaqui sites in the Rio de Janeiro state region are older than 10,000 years, the applicability of CO(2) absorption on Carbo-sorb and (14)C determination by counting on a low background liquid scintillation counter was tested. In the present work, sambaqui shells were treated with H(3)PO(4) in a closed vessel in order to generate CO(2). The produced CO(2) was absorbed on Carbo-sorb. On saturation about 0.6g of carbon, as CO(2), was mixed with commercial liquid scintillation cocktail (Permafluor), and the (14)C activity determined by counting on a low background counter, Packard Tricarb 3170 TR/SL, for a period of 1000 mins to enable detection of a radiocarbon age of 22,400 BP. But only samples with ages up to 3500 BP were submitted to the method because the samples had been collected in the municipality of Guapimirim, in archaeological sambaqui-type sites belonging to this age range. The same samples were sent to the (14)C Laboratory of the Centro de Energia Nuclear na Agricultura (CENA/USP) where similar results were obtained.     

Carbon-14, tree rings,and urban air pollution

Differences in natural ¹⁴C content of rings from trees from urban and rural locations have been compared on a year by year basis. The differences as a fraction of the urban tree's radioactivity reflect the local excess ¹⁴C-free carbon dioxide from fossil fuel combustion in the urban environment. New York City, Boston, and Washington, D.C., show different degrees of excess carbon dioxide. New York City averages about 6% excess carbon dioxide between 1950 and 1970. From this is infered an average carbon monoxide concentration during this period of 5 ppm.     

C, δC and total C content in soils around a Brazilian PWR nuclear power plant

Nuclear power plants release ¹⁴C during routine operation mainly as airborne gaseous effluents. Because of the long half-life (5730 years) and biological importance of this radionuclide (it is incorporated in plant tissue by photosynthesis), several countries have monitoring programs in order to quantify and control these emissions. This paper compares the activity of ¹⁴C in soils taken within 1 km from a Brazilian nuclear power plant with soils taken within a reference area located 50 km away from the reactor site. Analyses of total carbon, δ¹³C and ¹³⁷Cs were also performed in order to understand the local soil dynamics. Except for one of the profiles, the isotopic composition of soil organic carbon reflected the actual forest vegetation present in both areas. The ¹³⁷Cs data show that the soils from the base of hills are probably allocthonous.     

Transfer of radiocarbon liquid releases from the AREVA La Hague spent fuel reprocessing plant in the English Channel

The recent risk assessment by the North-Cotentin Radioecology Group (, 1999) outlined that (14)C has become one of the major sources of the low dose to man through seafood consumption. It was recommended that more data should be collected about (14)C in the local marine environment. The present study aims to respond to this recommendation. The estimation of (14)C activity in marine species is based on concentration factor values. The values reported here ranged from 1x10(3) to 5x10(3)Bqkg(-1)ww/BqL(-1). A comparison was made between the observed and predicted values. The accuracy of (14)C activity calculations was estimated between underestimation by a factor of 2 and over-estimation by 50% (95% confidence interval). However, the use of the concentration factor parameter is based on the biological and seawater compartments being in steady state. This assumption may not be met at short distances from the point of release of discharges, where rapid changes in seawater concentration may be smoothed out in living organisms due to transfer kinetics. The data processing technique, previously published by Fiévet and Plet (2003. Estimating biological half-lives of radionuclides in marine compartments from environmental time-series measurements. Journal of Environmental Radioactivity 65, 91-107), was used to deal with (14)C transfer kinetics, and carbon half-lives between seawater and a few biological compartments were thus estimated.     

Parameterization of a dynamic specific activity model of 14C transfer from surface water-to-humans

Carbon-14 is a particularly interesting radionuclide from the perspective of dose estimation because it mixes readily with stable CO2, and hence enters the food-chain as fundamental biomolecules. A model was developed for the situation of 14C releases to surface waters, where there are distinct changes in the water 14C activity concentrations throughout the year. The model computes the specific activity in water, phytoplankton, fish, crops, meat, milk and air, following a typical irrigation-based food-chain scenario. This paper describes the derivation of the required 14C-specific parameter values. Many of the key parameters are not commonly measured, at least not in the context of dose assessment. Thus, inference from other sources of data was required, and this is the scientific contribution described in this paper. The best estimates and appropriate measures of statistical dispersion are provided. This required consideration of both the temporal and spatial averaging domains to ensure they were correct for parameters as defined in the model. The model coupled with these parameter values represents several new developments for modelling 14C transfers.     

Radiocarbon behaviour in seawater and the brown algae Fucus serratus in the vicinity of the COGEMA La Hague spent fuel reprocessing plant (Goury)--France

Extensive studies of the radiocarbon (14C) distribution and transfer in the marine environment of the North-Cotentin peninsula and along the English Channel have been carried out. The main aims of these studies have been to estimate the spatial and temporal variation of the 14C concentration in seawater and to calculate 14C concentration factors for some biological species. Such information will be helpful in order to calculate precisely radiation doses to humans. First results obtained in the vicinity of the COGEMA La Hague nuclear plant (Goury) indicate a 14C labelling of the dissolved inorganic carbon (DIC) in seawater (8.0-26.2 Bq.m(-3)) and a tight relationship between the 14C in the liquid releases from the plant and the 14C concentrations in DIC. The particulate organic carbon (POC) is also labelled. The concentration factor calculations for the brown algae (Fucus serratus) sampled from Goury, and also along the English Channel, give 14C values around 3000 Bq.kg(-1) fresh weight / Bq.L(-1).     

Distribution of carbon 14 in the terrestrial environment close to French nuclear power plants

For 10 years, (14)C measurements have been performed around French nuclear power plant sites, both in zones influenced and zones not influenced by gaseous releases. Examining the results from these measurements in the terrestrial environment shows that the discharges have a very slight impact on the radiocarbon level (with a relative increase in the specific activity of the order of 3 Bqkg(-1)C in the influenced areas). In correlation, there is a near-negligible increase in dose, on average less than 0.1 microSvyr(-1), with reference to a dose from background radiation, which is of the order of 10 microSvyr(-1). The deltaC13 values are very similar between the influenced zone and the non-influenced zone, with a mean of -27 per thousand. The mean DeltaC14 varies from 101 per thousand in the non-influenced zone to 123 per thousand in the influenced zone. Moreover, a general reduction in (14)C concentration was found, with a time constant of the order of 95 years. The current level of (14)C specific activity in terrestrial environment is estimated to be 242+/-6 Bqkg(-1)C.     

Carbon-14 in tree rings and other terrestrial samples in the vicinity of Ignalina Nuclear Power Plant, Lithuania

The results of (14)C measurements in the annual tree rings from the Ignalina Nuclear Power Plant (INPP) surroundings, Lithuania, for the period of its operation from 1984 to 2002 are presented. The terrestrial samples, mainly moss and related soil, are studied in places as well. The tree rings have shown slightly enhanced (14)C activity due to operation of the nuclear power plant. The maximal calculated normalized (14)C release of 11TBqGW(e)(-1)year(-1) and the maximal effective dose of 2.0x10(-3)mSvyear(-1) resulting from the (14)C were estimated for 1999. For other years of INPP operation these values are lower. The excess of (14)C specific activity measured in the moss and soil samples from moss-covered sites near the nuclear power plant (up to 0.5km) showed highly elevated (14)C contents (up to 813pMC), probably indicating releases of particulate material.     

Depth profiles of radiocarbon and carbon isotopic compositions of organic matter and CO2 in a forest soil

Depth profiles of the specific activities of (14)C and carbon isotopic compositions (Delta(14)C, delta(13)C) in soil organic matter and soil CO(2) in a Japanese larch forest were determined. For investigating the transport of CO(2) in soil, specific activities of (14)C, Delta(14)C and delta(13)C in the organic layer, and atmospheric CO(2) in the same forest area were also determined. The specific activity of (14)C and Delta(14)C in the soil organic matter decreased with the increase in depth of 0-60cm, while that of soil CO(2) did not vary greatly at a soil depth of 13-73cm and was more prevalent than that of atmospheric CO(2). Peaks of specific activities of (14)C appeared at the depth of 0-4cm and Delta(14)C values were positive in the depth range from 0 to 15cm. These results suggest that the present soil at a depth of 0-4cm had been produced from the mid-1950s up until 1963, and the bomb C had reached the depth of 15cm in the objective soil area. The delta(13)C in the soil organic matter increased at the depth of 0-55cm, while that of soil CO(2) collected on 8 November 2004 decreased rapidly at the depth of 0-13cm and only slightly at the depth of 53-73cm. By combining the Delta(14)C and delta(13)C of the respective components and using the Keeling plot approach it was made clear that the entering of atmospheric CO(2) showed a large contribution to soil CO(2) at the depth of 0-13cm and a negligible contribution at the depth of 53-73cm for soil air collected on 8 November 2004. Respiration of live roots was presumed to be the main source of soil CO(2) at the depth of 53-73cm on 8 November 2004.     

Reconstructing the history of 14C discharges from Sellafield: part 1--atmospheric discharges

14C specific activities, above ambient background levels, were determined in individual treerings (corresponding to the years 1950-1999) sectioned from an oak tree that was felled in autumn 1999, from a location 1.5 km east of the Sellafield nuclear fuel reprocessing plant in Cumbria. north-west England. The data were used to produce a new, improved, reconstruction of Sellafield's annual atmospheric 14C discharges between 1951 and 1999, using the most reliable discharge data set (1994-1999) as the primary basis for the determination of a new calibration factor that relates excess 14C activity in individual tree rings to the annual discharge during the corresponding year. The results indicate that the current British Nuclear Fuels plc (BNFL) estimate of total 14C discharges to the atmosphere prior to 1978 is significantly overestimated, while the current estimate of total 14C discharges after 1978 is very similar to that determined in this study. In this study, the total activity of 14C discharged to the atmosphere from Sellafield between 1951 and 1999 is estimated to be 259+/-63 TBq (at 2 std. dev.). The BNFL current estimate is 360TBq.     

Disposition and metabolic profiling of [14C]-decabromodiphenyl ether in pregnant Wistar rats

Fully brominated diphenyl ether, decabromodiphenyl ether (DBDE), is one of the most widely used brominated flame retardants worldwide. Little data is available about the metabolic fate of DBDE in animal models and nothing at all about the extent of foetal exposure. In this work, pregnant Wistar rats were force-fed with 99.8% pure [14C]-DBDE over 96 h at a late stage of gestation (days 16 to 19). More than 19% of the administered dose was recovered in tissues and carcasses, demonstrating efficient absorption of DBDE despite its high molecular weight and low solubility. The highest concentrations of DBDE residues were found in endocrine glands (adrenals, ovaries) and in the liver, with lower values recorded for fat. In all tissue extracts, most of the radioactivity was associated with unchanged DBDE. The use of high-grade purity [14C]-DBDE allowed quantification of several metabolites present both in maternal tissues and in foetuses. These biotransformation products accounted for 9-27% of the extractable radioactivity in tissues and 14% of that in foetuses. Three nona-BDEs and one octa-BDE were identified by LC-APPI/MS. The unequivocal characterisation of a hydroxylated octa-BDE isolated from liver was confirmed by NMR. In rat, the main metabolic pathways of DBDE are debromination and oxidation. DBDE, and very likely most of its metabolites, are able to cross the placental barrier in rat. Metabolic profiles, obtained in vivo for the first time, demonstrated the presence of DBDE and major biotransformation products in endocrine glands as well as in foetuses. The biological activity of these metabolites still needs to be assessed in order to better understand the potential toxicity of DBDE.