Determination of 99Tc, 63Ni and 121m+126Sn in the marine environment

Four artificially produced radionuclides (${}^{99}\text{Tc, t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 2·15 × 10}{}^5\text{y;}{}^{63}\text{Ni, t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 93 y}$ and ${}^{\mathrm{121m+126}}\text{Sn, t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 55·5 y}$) have been analyzed in sediments and organisms from the marine environment. The samples were obtained from the vicinities of nuclear energy facilities, at sites of nuclear weapon tests and at sites remote from both of these locales. The activities of these nuclides per unit dry weight are remarkably similar at the first two of the above areas but are usually detectable only with difficulty, if at all, in the third area. Techniques for sample treatment and measurement are given.     

Experimental studies on the bioaccumulation of plutonium from sea water and a deep-sea sediment by clams and polychaetes

The bioavailability of ²³⁷Pu in the (III + IV) and (V + VI) oxidation states from sea water and a NE Atlantic deep-sea sediment has been studied for clams (Venerupis decussata) and polychaete worms (Hermione hystrix). After 22 days' exposure in sea water transfer factors (TF) had not reached equilibrium, and were 74 ± 5 and 61 ± 1 for clams and 370 ± 10 and 275 ± 11 for polychaetes, for Pu (III + IV) and Pu (V + VI) respectively. Depuration rates after sea water exposure followed a single exponential form ($\text{T}{}_{\mathrm{<mtext>b</mtext><mtext>1</mtext><mtext>2</mtext>}}\text{= 50}\text{days}$) for clams, and for polychaetes at least a two component from with $\text{T}{}_{\mathrm{<mtext>b</mtext><mtext>1</mtext><mtext>2</mtext>}}\text{= 1·3}\text{days}$ and 54 days. TF values for ²³⁷Pu bioaccumulation from sediments were very low, 6 × 10^?3 and 5 × 10^?2 for clams and polychaetes, respectively, after 20 days' exposure.Plotonium appears to be about 50% more bioavailable to the same species than americium as measured by laboratory experiments using a similar deep-sea sediment. Depuration experiments with clams after 40 days' exposure to labelled sediment indicated loss followed a single exponential form with a $\text{T}{}_{\mathrm{<mtext>b</mtext><mtext>1</mtext><mtext>2</mtext>}}\text{= 24}\text{days}$. Significant differences in the behaviour of Pu introduced into the uptake and loss experiments in different oxidation states were not observed in general.     

Nonidentifiability of competing risks

Frequently one is interested in examining the survival experience of a set of individuals exposed to k risks. If W is the time of failure for the individual and J is the indicator variable for cause of death, then the competing risk framework assumes that W = min X_i and J = j if X_j is the minimum, where the X_i's are the survival lifetimes when only risk R_i is operating on the population. To examine the underlying structure of the survival experience one has to know the joint distribution of the $\text{X}{}_{\mathrm{i}}\text{(F}{}_{\mathrm{<mtext>x</mtext>}}\text{)}$. It is shown here that if only W and J are observed, the joint distribution of the $\text{X}{}_{\mathrm{i}}\text{(F}{}_{\mathrm{<mtext>x</mtext>}}\text{)}$ is nonidentifiable.     

Air-to-vegetation transfer rates of natural submicron aerosols

Submicron aerosol deposition to outdoor vegetation was evaluated by measuring vegetation and air concentrations of ²¹²Pb, ²¹⁴Pb, and ⁷Be attached to atmospheric aerosols. A biomass-normalized deposition velocity (V_D), with units of m³ kg^?1 s^?1, was used to compare species and isotopes with respect to air-to-vegetation transfer rates. For ²¹²Pb ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 10·64 h}$), higher night-time air concebtrations dominate deposition, while for ²¹⁴Pb ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 26·8}\text{min}$), deposition measurements over shorter time periods relative to changing atmospheric conditions were possible. Calculated V_D values were usually higher for ²¹⁴Pb, possibly reflecting wind-enhanced deposition during the afternoon period of sampling. Evergreen species, including pines, were not appreciably different from deciduous species. Most striking was the narrow range of results (factor of 6 for 34 ²¹²Pb measurements of 20 species). Beryllium-7 ($\text{t}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{= 53·3 d}$) was used to evaluate time-integrated deposition by sampling vegetation in California near the end of dry summers. Similar deposition rates were found for this isotope. The results of the study indicated that naturally radioactive atmospheric aerosols can be used to understand the dynamics of submicron aerosol deposition to ecosystems.     

Threshold and dose response estimation using the “filter model”

The “filter model” has been developed to explain the biologic effects of radiation and chemicals. We have examined nearly 300 sets of dose response data, of which 50 are presented here. Responses (induced by radiation and chemicals) which have been examined include in vitro survival studies on animal and plant tissues, induction of cellular aberrations and time to tumor or death. Similar data from in vivo studies has also been examined. All of the data appear to fit the model R = a lnD + b(lnD)² + c, where R is the response, a and b are parameters fitted by regression to a particular set of data, and c is the response at zero (or lowest) dose. By writing this model in exponential form, it can be seen that the response R results from multistage filtering (by net amounts a and b) of the initial dose, D. The threshold is obtained from this model as the point, $\text{D}\text{?}{}_{\mathrm{T}}$, at which the second derivative becomes zero. This is given by $\text{D}\text{?}{}_{\mathrm{T}}\text{=}\text{exp}\text{(1 ?}\text{a}\text{2b}\text{)}$ when a and b are oppositelt signed.     

Comparing computing formulas for estimating concentration ratios

The purpose of this paper is to provide guidance on the choice of computing formulas (estimators) for estimating average concentration ratios and other ratio-type measures of radionuclides and other environmental contaminant transfers between ecosystem components. Mathematical expressions for the expected value of three commonly used estimators (arithmetic mean of ratios, geometric mean of ratios, and the ratio of means) are obtained when the multivariate lognormal distribution is assumed. These expressions are used to explain why these estimators will not in general give the same estimate of the average concentration ratio. They illustrate that the magnitude of the discrepancies depends on the magnitude of measurement biases, and on the variance and correlations associated with spatial heterogeneity and measurement errors. This paper also reports on a computer simulation study that compares the accuracy of eight computing formulas for estimating a ratio relationship that is constant over time and/or space. Statistical models appropriate for both controlled spiking experiments and observational field studies for either normal or lognormal distributions are considered. Our results indicate that for either type of study the geometric mean is generally preferred if the lognormal distribution applies. However, the geometric mean has the disadvantage that its expected value depends on n, the number of measurements taken. Ricker's estimator, $\text{R}\text{?}{}_{\mathrm{rt}}$, appears to perform worse than the other estimators studied when the observations are lognormal. All eight estimators appear to be equally accurate for the controlled spiking study when data are normally distributed. For observational field studies when data are normally distributed the ratio of means or slight modifications thereof are preferred to other estimators investigated. Before one chooses a computing formula for estimating a concentration ratio, thought should be given to what target value needs to be estimated to satisfy study objectives, and to whether the normal or lognormal distribution is a more realistic model. The geometric mean performs well for lognormal distributions, but comparison of geometric means or of a geometric mean with environmental limits can be misleading if n is small. The arithmetic mean of ratios is a conservative choice in that it will always give a larger estimate than will the geometric mean. It may also be severely biased when data are lognormal and the variances of measurement errors are large. The ratio of the means is a reasonable choice if the distribution is normal. The median of the observed ratios, $\text{R}\text{?}{}_{\mathrm{<mtext>md</mtext>}}$, is useful estimate since it is easily obtained and has an easily understood interpretation as the point above which and below which 50% of the observed ratios lie. Also, it is appropriate no matter what the distribution of the observed ratios may be. Confidence limits on the median are also easily obtained. Finally, while this paper emphasizes applications in radionuclide research, our results should be applicable to a wide range of environmental contaminants since many contaminants have approximately lognormal distributions.     

Statistical assessment of subsampling procedures

As shown by the examples in this paper, the concentrations in subsamples are not necessarily independently and normally distributed despite vigorous grinding and mixing of the original sample. Studies of the statistical properties of subsample concentrations should test for deviations from independence and normality and, if deviations are found, should model the observed distribution. The tests include an analysis of variance to check for less variation among nearby subsamples than among widely spaced subsamples, as well as the computation of the probability plot correlation coefficient to check for nonnormality. These tests are illustrated with ${}^{239}\text{Pu}\text{+}{}^{240}\text{Pu}$ measurements on subsamples prepared for use as standard reference materials. These materials are used in quality assurance for environmental radioactivity measurements. The material consisting of Human Liver (SRM 4352) exhibits dependence, which may be due to inadequate mixing or to later handling that caused segregation. The material consisting of Human Lung (SRM 4351) and the material consisting of soil from Rocky Flats (SRM 4353) exhibit nonnormality due to the particulate nature of some plutonium-bearing fractions of the material. The lung measurements are modeled with the gamma distribution. The soil measurements are modeled with a combination of the normal distribution and a distribution that models the occurrence of outliers. The use of these models to describe the subsamples involves assessment of the contribution of the measurement error.     

Variability of the sorption of Cs, Zn, Sr, Co, Cd, Ce, Ru, Tc and I at trace concentrations by a forest soil along a transect

The variability of the sorption properties (characterized by the distribution coefficient K_d) of a forest soil for Cs, Zn, Sr, Co, Cd, Ce, Ru, Tc, and I were determined along a transect of 150 m in regular intervals of 3 m. Radioactive tracers were used to ensure trace concentrations of these elements. For comparison, for each soil sample the loss on ignition, as a measure of the soil organic matter content, and the pH were also determined. On average, the K_d values increase in the sequence Tc < I < Ru ≈ Co ≈ Zn ≈ Sr < Cd < Ce < Cs; the spatial variability in the sequence I < Zn ≈ Sr ≈ Co ≈ Cd ≈ Ru ≈ Tc < Cs, and I ≈ Ce < Tc. Correlation analysis revealed that, when moving along the transect, the K_d values for some elements changed in a similar, and for others in a dissimilar pattern. In a few cases a correlation between the pH or the loss on ignition and the K_d values was also present. The spatial structure of the data was examined by semivariograms. For the elements Co, Cd, Zn, and Sr, the K_d values showed an almost periodic behaviour along the transect, which is probably due to periodic changes of some soil properties in a forest with regularly spaced trees.     

Bioavailability of sediment-associated and low-molecular-mass species of radionuclides/trace metals to the mussel Mytilus edulis

Sediments can act as a sink for contaminants in effluents from industrial and nuclear installations or when released from dumped waste. However, contaminated sediments may also act as a potential source of radionuclides and trace metals to the water phase due to remobilisation of metals as dissolved species and resuspension of particles. The marine mussel Mytilus edulis is a filter-feeding organism that via the gills is subjected to contaminants in dissolved form and from contaminants associated to suspended particles via the digestive system. In this paper the bioavailability of sediment-associated and seawater diluted Cs, Co, Cd and Zn radioactive tracers to the filtering bivalve M. edulis has been examined. The mussels were exposed to tracers diluted in ultrafiltered (<10 kDa) seawater (Low Molecular Mass form) or to tracers associated with sediment particles from the Stepovogo Fjord at Novaya Zemlya in short-term uptake experiments, followed by 1-month depuration experiments in flow-through tanks. A toxicokinetic model was fitted to the uptake and depuration data, and the obtained parameters were used to simulate the significance of the two uptake pathways at different suspended sediment loads and sediment-seawater distribution coefficients. The results of the model simulations, assuming steady state conditions, suggest that resuspended particles from contaminated sediments can be a highly significant pathway for mussels in the order ¹⁰⁹Cd ≌ ⁶⁵Zn < ¹³⁴Cs < ⁶⁰Co. The significance increases with higher suspended sediment load and with higher K_d. Furthermore, the experimental depuration data suggest that Cs is retained longer and Co, Cd and Zn shorter by the mussels when associated with ingested sediments, than if the metals are taken up from the low molecular mass (LMM) phase.     

Cesium accumulation by fish following acute input to lakes: a comparison of experimental and Chernobyl-impacted systems

An uptake parameter u (L kg⁻¹ d⁻¹) and a loss rate parameter k (d⁻¹) were estimated for the patterns of accumulation and loss of ¹³³Cs by three fish species following an experimental ¹³³Cs addition into a pond in South Carolina, USA. These u and k parameters were compared to similar estimates for fish from other experimental ponds and from lakes that received ¹³⁷Cs deposition from Chernobyl. Estimates of u from ponds and lakes declined with increasing potassium concentrations in the water column. Although loss rates were greater in the experimental ponds, the times required to reach maximum Cs concentrations in fish were similar between ponds and lakes, because ponds and lakes had similar retentions of Cs in the water column. The maximum Cs concentrations in fish were largely determined by initial Cs concentrations in the water column. These maximum concentrations in fish and the times required to reach these maxima are potentially useful indicators for assessments of risks to humans from fish consumption.     

Vertical distributions of (99)Tc and the (99)Tc/(137)Cs activity ratio in the coastal water off Aomori, Japan

Using a sector-field ICP-MS the vertical distributions of the ⁹⁹Tc concentration and ⁹⁹Tc/¹³⁷Cs activity ratio were measured in the coastal waters off Aomori Prefecture, Japan, where a spent-nuclear-fuel reprocessing plant has begun test operation. The ⁹⁹Tc concentrations in surface water ranged from 1.8 to 2.4 mBq/m³, no greater than the estimated background level. Relatively high ⁹⁹Tc/¹³⁷Cs activity ratios (10-12 × 10⁻⁴) would be caused by the inflow of the high-⁹⁹Tc/¹³⁷Cs water mass from the Japan Sea. There is no observable contamination from the reprocessing plant in the investigated area. The ⁹⁹Tc concentration and the ⁹⁹Tc/¹³⁷Cs activity ratio in water column showed gradual decreases with depth. Our results implied that ⁹⁹Tc behaves in a more conservative manner than ¹³⁷Cs in marine environments.     

Comparative accumulation of (109)Cd and (75)Se from water and food by an estuarine fish (Tetractenos glaber)

Few data are available on the comparative accumulation of metal(loid)s from water and food in estuarine/marine fish. Smooth toadfish (Tetractenos glaber), commonly found in estuaries in south-eastern Australia, were separately exposed to radio-labelled seawater (14kBqL(-1) of (109)Cd and 24kBqL(-1) of (75)Se) and food (ghost shrimps; Trypaea australiensis: 875Bqg(-1)(109)Cd and 1130Bqg(-1)(75)Se) for 25 days (uptake phase), followed by exposure to radionuclide-free water or food for 30 days (loss phase). Toadfish accumulated (109)Cd predominantly from water (85%) and (75)Se predominantly from food (62%), although the latter was lower than expected. For both the water and food exposures, (109)Cd was predominantly located in the gut lining (60-75%) at the end of the uptake phase, suggesting that the gut may be the primary pathway of (109)Cd uptake. This may be attributed to toadfish drinking large volumes of water to maintain osmoregulation. By the end of the loss phase, (109)Cd had predominantly shifted to the excretory organs - the liver (81%) in toadfish exposed to radio-labelled food, and in the liver, gills and kidney (82%) of toadfish exposed to radio-labelled water. In contrast, (75)Se was predominantly located in the excretory organs (gills, kidneys and liver; 66-76%) at the end of the uptake phase, irrespective of the exposure pathway, with minimal change in percentage distribution (76-83%) after the loss phase. This study emphasises the importance of differentiating accumulation pathways to better understand metal(loid) transfer dynamics and subsequent toxicity, in aquatic biota.     

Characterization of ²⁴¹ Am and ¹³⁴Cs bioaccumulation in the king scallop Pecten maximus: investigation via three exposure pathways

In order to understand the bioaccumulation of ²⁴¹Am and ¹³⁴Cs in scallops living in sediments, the uptake and depuration kinetics of these two elements were investigated in the king scallop Pecten maximus exposed via seawater, food, or sediment under laboratory conditions. Generally, ²⁴¹Am accumulation was higher and its retention was stronger than ¹³⁴Cs. This was especially obvious when considering whole animals exposed through seawater with whole-body concentration factors (CF_7d) of 62 vs. 1, absorption efficiencies (A_0l) of 78 vs. 45 for seawater and biological half-lives (T_b½l) of 892 d vs. 22 d for ²⁴¹Am and ¹³⁴Cs, respectively. In contrast, following a single feeding with radiolabelled phytoplankton, the assimilation efficiency (AE) and T_b½l of ¹³⁴Cs were higher than those of ²⁴¹Am (AE: 28% vs. 20%; T_b½l: 14 d vs. 9 d). Among scallop tissues, the shells always contained the higher proportion of the total body burden of ²⁴¹Am whatever the exposure pathway. In contrast, the whole soft parts presented the major fraction of whole-body burden of ¹³⁴Cs, which was generally associated with muscular tissues. Our results showed that the two radionuclides have contrasting behaviors in scallops, in relation to their physico-chemical properties.     

Krypton-85 in the atmosphere 1950–1977: a data review

For over 20 years the radioactive noble gas ⁸⁵Kr, the product of nuclear industry, has been released to the environment mainly from nuclear fuel reprocessing plants. Owing to its relatively long half-life $\text{T(}\text{1}\text{2}\text{= 10.76}\text{y}\text{)}$ and the absence of other appreciable sinks, a cumulative buildup of ⁸⁵Kr in the atmosphere is observed. The mean ⁸⁵Kr surface air activity in the northern hemisphere has increased from about 20 dpm/mmol Kr in 1950 to about 750 dpm/mmol Kr in 1977. In recent years, a substantial slow-down of the ⁸⁵Kr emission rate to the atmosphere has been observed. The published data indicate rather good mixing of ⁸⁵Kr in the northern hemisphere, but a gradient is observed in the southern hemisphere due to the fact that all nuclear fuel reprocessing plants are situated in the northern hemisphere and due to poor mixing of the atmosphere in the meridional direction.This paper summarizes nearly all of the data on ⁸⁵Kr activity in the atmosphere published up to the middle of 1978. The spatio-temporal distribution of ⁸⁵Kr atmospheric activity is discussed. Some forecasts of future ⁸⁵Kr concentration in the atmosphere and its possible ecological consequences are also presented.     

Sea-to-land transfer of technetium-99 through the use of contaminated seaweed as an agricultural soil conditioner

The use of seaweed as an agricultural soil conditioner gives rise to a potential pathway for the transfer of Technetium-99 ((99)Tc) from marine to terrestrial ecosystems and thence to man. However, to date there is little information on the extent of the release of (99)Tc from seaweed into soil and the mechanisms involved. This pot experiment has shown that (99)Tc is released fairly rapidly from Fucus vesiculosus into a sandy coastal soil. Despite low temperature conditions, 60% of the (99)Tc added with the seaweed had accumulated in the soil 15 weeks after addition. Concurrent CO(2) monitoring (used as a measure of microbial decomposition or catabolism) suggested that the initial (99)Tc release (up to 40% in the first 8 weeks) was due to leaching from the seaweed and that microbial decomposition was responsible for the release of the remaining (99)Tc in the latter phase (12-15 weeks).