Results of the European Commission Marina II study: part II--effects of discharges of naturally occurring radioactive material

Enhanced levels of naturally occurring radioactive materials (NORM) are produced through various industrial operations and may lead to discharges to the marine environment. A recent study, called MARINA II, carried out for the European Commission considered discharges of radionuclides from the NORM industries to north European marine waters and their consequences. There are two main sources that were considered in the study. The use of phosphogypsum during the production of phosphoric acid by the fertiliser industry and the pumping of oil and gas from the continental shelf in the North Sea which produces large quantities of water contaminated with enhanced levels of naturally occurring radionuclides. Discharges of alpha emitting radionuclides from these two industries have contributed significantly to the total input of alpha emitters to north European waters over the period 1981-2000 (data were not available prior to 1981). Discharges due to the use of phosphogypsum have declined since the early 1990s and are now very low. Discharges from the oil and gas industries stabilised in the second half of the 1990s and are now the major contributor to alpha discharges to the region. As most European countries do not report discharges of radioactivity with the water produced during extraction, there is considerable uncertainty in the discharges used in the study. The impact of the discharges has been estimated both in terms of the effect on non-human biota and the radiological impact for people. In the 1980s the radiation dose rates to marine biota in the region around a phosphate plant on the north-west coast of England were as high due to the discharges from the phosphate plant as those near to the Sellafield reprocessing plant due to its discharges. In recent years the additional dose to marine biota in this region due to the past NORM discharges is of the same order of magnitude as the natural background. The collective dose rate was estimated to determine the radiological impact on people. The peak collective dose rate from the NORM industries occurred in 1984 and was just over 600 manSv y(-1). The collective dose rate fell with time as discharges from the phosphate industry reduced and was estimated as under 200 manSv y(-1) in 2000.     

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.     

The influence of the cigarette smoke pollution and ventilation rate on alpha-activities per unit volume due to radon and its progeny

Alpha and beta activities per unit volume air due to radon, thoron and their decay products were evaluated in the air of various cafe rooms polluted by cigarette smoke. Both CR-39 and LR-115 type II solid state nuclear track detectors (SSNTD) were used. Equilibrium factors between radon and its progeny and thoron and its daughters have been evaluated in the air of the studied cafe rooms. The committed equivalent doses due to short-lived radon decay products were determined in different regions of the respiratory tract of non-smoker members of the public. The influence of cigarette smoke pollution, ventilation rate and exposure time on committed equivalent dose in the respiratory systems of non-smokers was investigated. Committed equivalent doses ranged from 1.15 x 10(-11)-2.7 x 10(-7) Sv.y(-1)/h of exposure in the extrathoracic region and from 0.8 x 10(-12)-1.7 x 10(-8) Sv.y(-1)/h of exposure in the thoracic region of the respiratory tract of non-smokers.     

Detection of tritium sorption on four soil materials

In order to measure groundwater age and design nuclear waste disposal sites, it is important to understand the sorption behavior of tritium on soils. In this study, batch tests were carried out using four soils from China: silty clays from An County and Jiangyou County in Sichuan Province, both of which could be considered candidate sites for Very Low Level Waste disposal; silty sand from Beijing; and loess from Yuci County in Shanxi Province, a typical Chinese loess region. The experimental results indicated that in these soil media, the distribution coefficient of tritium is slightly influenced by adsorption time, water/solid ratio, initial tritium specific activity, pH, and the content of humic and fulvic acids. The average distribution coefficient from all of these influencing factors was about 0.1-0.2 mL/g for the four types of soil samples. This relatively modest sorption of tritium in soils needs to be considered in fate and transport studies of tritium in the environment.     

Concentration of radionuclides in hydrosphere affected by Temelín Nuclear Power Plant in Czech Republic

The paper presents results of a long-term field study of the possible impact of Temelín NPP on the Vltava and Elbe Rivers. The study was divided into 2 stages: before and after the operation of the NPP. The main goal of the investigation before the operation (1989–2000) was to determine the background levels of radionuclides resulting from the tests of nuclear weapons and the Chernobyl accident for different components of the environment. The paper discusses also the risk of a river radioactive contamination due to the tritium discharges in wastewater from Temelín NPP. During the operation period of 2001–2006, the results of the monitoring did not detect any impact of Temelín NPP on the concentrations of activation and fission products in the hydrosphere, apart from tritium. The annual average tritium concentrations in the Vltava River correspond with the previously calculated predictions for the conditions of the average and minimum guaranteed flows. The maximum concentration of tritium of 26.6 Bq/l in Vltava River at Prague was observed after dry period in 2003.     

Tritium concentrations of groundwater in Naka Terrace,Ibaraki Prefecture,Japan

Levels of tritium in groundwater of the inland area of Naka Terrace were measured during 1981–1983 to establish a baseline for evaluation of any changes which may result from release of tritium from nuclear facilities in the coastal region of the terrace. Most of the samples yielded concentrations in the range 40–90 pCi litre⁻¹, which were similar to those of two rivers bordering the area of concern, whereas tritium levels in monthly precipitation samples were in the range 30–50 pCi litre⁻¹. These results imply that the rivers are fed from groundwater reservoirs, which are releasing the higher tritium levels recharged during the previous 20 years when bomb-produced tritium caused higher levels in precipitation. Only two groundwater samples yielded concentrations below detection limit, both from the deep Pleistocene gravel layer in a buried river channel underlying the terrace. Some ground-waters in the coastal area yielding more than 100 pCi litre⁻¹ are considered to be already influenced by tritium released from nuclear facilities.     

Radionuclide contamination of sediment deposits in the Ob and Yenisey estuaries and areas of the Kara Sea

The Ob and Yenisey rivers are major contributors to total riverine discharge to the Arctic Ocean. Several large nuclear facilities discharge into these rivers, which could affect actual and potential discharges of radionuclides to the Arctic region. This article presents new radionuclide concentration and grain-size data resulting from analyses of several sediment samples collected during research cruises in the Ob and Yenisey estuaries and adjacent areas during 2000 and 2001. Results indicate that discharges from the main nuclear facilities do not constitute a major contribution to the level of radioactive contamination in the marine areas studied, though Co-60 was detected at low concentrations in some sediment horizons. However, the aggregate contamination from different sources is not radioecologically significant in sediments within the study area, maximum Cs-137 levels being approximately 80 Bq kg(-1) dry weight.     

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.     

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.     

The distribution of tritium in the terrestrial and aquatic environments of the Creys-Malville nuclear power plant (2002-2005)

The Creys-Malville nuclear plant, located on the left bank of the Rh?ne, was shut down in 1998. The facilities are currently in their initial stage of dismantling. In order to establish a baseline for tritium in the vicinity of the site prior to the main dismantling phase, we carried out a monitoring program between 2002 and 2005 in the main terrestrial and aquatic compartments of the local environment. Tritium levels in the groundwaters and in the Rh?ne waters correspond to the regional tritium concentration in precipitation. The data obtained for the terrestrial environment are also in good agreement with the regional background and do not show any specific signature linked to the nuclear plant. The various aquatic compartments of the Rh?ne (fish, plant, sediment) are significantly enriched in tritium both upstream and downstream of the power plant: although Tissue-Free Water Tritium concentrations are in equilibrium with the river water, the non-exchangeable fraction of organic bound tritium in plants and fishes shows values which outpace the river water background by one to two orders of magnitude, and up to four to five orders of magnitude in the sediments. This tritium anomaly is not related to the nuclear plant, as it is already present at the Swiss border 100km upstream of the site. Although fine particles of tritiated polystyrene entering the composition of the luminous paints used by the clock industry have been suspected on several occasions, the exact nature and the origin of this tritium source remain unknown and require further investigations.     

RS与GIS支持下的南京市景观格局动态变化研究

利用1986、1994、2000年的TM图像和2000年的土地利用现状图,运用GIS和核心景观指数研究南京市自1986年以来景观格局的动态演变规律。结果表明：南京市在快速城市化的过程中,城市景观结构的变化主要表现为耕地、绿地、水体和未利用地等自然或半自然景观向城市、农村居民地、工矿用地以及交通用地等人文景观转变;景观的多样性增加,斑块的平均面积增大,分离度、破碎度和孔隙度减小,城市的开发趋向有序化、规模化;但由于人类活动作用方式或作用程度的不同,不同的景观类型在同一时间段,或者同一景观类型在不同的时间内空间格局的转变模式不同,1986~1994年城市扩展的速度很快,开发比较混乱,城市、农村居民地和交通用地等人文景观的面积大幅增加,耕地、绿地和未利用地的面积大量减少,斑块分布不均匀,空隙度增加,1994~2000年城市扩展的速度减慢,开发趋向有序化,除耕地外,其他景观类型的分离度、破碎度和孔隙度减小,空间分布趋向均匀。     

Experimental investigation and modelling of tritium washout by precipitation in the area of the nuclear power plant of Paks, Hungary

Tritium occurs in nature in trace amounts, but its concentration is changing due to natural and artificial sources. Studies focusing on natural tritium have to take into account the effect of artificial sources. Also, the impact of tritium is an important issue in environmental protection, e.g. in connection with the emissions from nuclear power plants. The present work focuses on the rain washout of tritium emitted from the Paks nuclear power plant in Hungary. Rainwater collectors were placed around the plant and after a period of precipitation, rainwater was collected and analysed for tritium content. Samples were analysed using low-level liquid scintillation counting, with some also subject to the more accurate ³He ingrowth method. The results clearly show the trace of the tritium plume emitted from the plant; however, values are only about one order of magnitude higher than environmental background levels. A washout model was devised to estimate the distribution of tritium around the plant. The model gives slightly higher concentrations than those measured in the field, but in general the agreement is satisfactory. The modelled values demonstrate that the effect of the plant on rainwater tritium levels is negligible over a distance of some kilometres.     

Modelling the spatio-temporal evolution of 3H in the waters of the River Tagus

Measurements of tritium specific activity levels and of temperatures in waters of the Torrejón-Tagus reservoir (Spain) showed that their radioactive characteristics were basically influenced by the radioactive liquid effluent from the Almaraz Nuclear Power Plant. This enters the Torrejón-Tagus reservoir via the Arrocampo cooling reservoir, which exchanges water with the first. We studied the temporal and spatial (in two dimensions) evolution of the mentioned parameters for years 1997 and 1998. The tritium levels were found to be significantly correlated with temperature. Two numerical models were constructed for a quantitative study of the tritium levels along Torrejón reservoir: a 1D model was used for the dispersion of tritium along the whole length of the reservoir, and a 2D depth-averaged model was used for a detailed study of the area where tritium is released into the reservoir. Both models solve the hydrodynamic equations, to obtain the currents induced by the exchanges of water between the reservoirs in the River Tagus and Arrocampo, and the advection/diffusion equation to calculate the dispersion of tritium. In general, the model results were in agreement with the experimental observations.     

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.     

A box model for calculation of collective dose commitment from radioactive waterborne releases to the baltic sea

To meet the new regulations of maximum yearly releases from Swedish nuclear power plants issued by the Swedish National Radiation Protection Institute, and to make realistic calculations of collective dose commitment derived from radionuclides discharged to the Baltic Sea, a box model AQUAPATH-BALTIC has been developed. The model calculates radionuclide concentrations in 25 boxes for discharges into given compartments and takes into consideration the dispersion rates of the water masses, the sediment-water interaction and radioactive decay. The calculated concentrations in water and sediment at steady state are then used to evaluate individual and collective intakes of activity and external exposures. The radiation doses to the global population following discharges to the Baltic Sea are also calculated.     

Observed half-lives of 3H, 90Sr and 137Cs in hydrosphere in the Vltava River basin (Bohemia)

A near field study was set up to follow the effects of the Temelin nuclear power plant construction. Reference levels of artificial radionuclides were monitored in the Vltava River upper course and its tributaries in the period 1990-2001. Monitoring continued even after the waste water release startup during the pilot operation in 2002. The assessment of the (90)Sr and (137)Cs concentrations histories in ground water, river bottom sediments and fish showed a decreasing trend. This trend was not influenced by the nuclear power plant pilot operation. In the case of tritium, trend of increasing concentration had been already observed since the pilot operation startup. The monitoring of changes in concentrations of artificial and natural radionuclides in influenced and uninfluenced profiles will be maintained to assess the possible influence of the operation of the Temelin nuclear power plant.     

Deposition of 134,137Cs from Chernobyl fallout on Norway spruce and forest soil and its incorporation into spruce twigs

The aims of the present research are to describe the amounts, and the variation with time, of ¹³⁴Cs and ¹³⁷Cs in spruce-twigs (P. abies karst.) and in the soil of a spruce forest in Switzerland following deposition of the Chernobyl fallout. The activity of the twigs was subdivided into 3 compartments: the activity on their surfaces (i.e. the activity which can be removed from the twigs along with their natural wax coating), the activity incorporated into the needles and, finally, the activity incorporated into the wood. These compartments were separately sampled 6 times over a period from 54 to 233 days after the Chernobyl incident. Twigs which sprouted in two successive years (1985, 1986) were sampled and were found to show different behaviours. The activities associated with the 1986 twigs were roughly constant with time, while those of the 1985 twigs decreased exponentially, with half-lives around 150 days. The mean activity associated with 1 g (dry) of 1985 twigs is 724 mBq ¹³⁷Cs g⁻¹, of which 58% is incorporated into the twig wood, 17% into the needles and 25% associated with the adhering aerosol. ¹³⁷Cs on the surface of the needles was found to be water-insoluble. It is believed to be strongly adsorbed on to the soil-derived fraction of the aerosol residing on the needle surface and thus provides a tracer for studying the behaviour of natural aerosols on such surfaces.The same soil profile was measured before and after the Chernobyl incident, allowing direct comparison between nuclear weapons and Chernobyl fallout. The latter is mainly (56%) stored in the litter layer, with only 4% below a depth of 13 cm; it has penetrated into the soil to a much lesser extent than weapons fallout. The forest soil inventory of ¹³⁷Cs showed 2600 Bq m⁻² from nuclear weapons fallout and 6200 Bq m⁻² from Chernobyl.The ¹³⁴Cs/¹³⁷Cs activity ratio of the Chernobyl fallout was found to be 0·58 ± 0·01; the activity ratios in the different compartments investigated prove that incorporation of Cs into spruce occurred exclusively by uptake through the needles. A rough estimate indicates that in a spruce forest the activity stored in the twigs is half that stored in the soil.     

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.     

Long-term investigations of radiocaesium activity concentrations in carp in North Croatia after the Chernobyl accident

Long-term investigations of radiocaesium activity concentrations in carp in the Republic of Croatia are presented. The radiocaesium levels in carp decreased exponentially and the effective ecological half-life of (137)Cs was estimated to be about 1 year during 1987-2002 and 5 years during 1993-2005. The observed (134)Cs:(137)Cs activity ratio in carp was found to be similar to the ratio observed in other environmental samples. The concentration factor for carp (wet weight) was estimated to be 128+/-74 Lkg(-1), which is in reasonable agreement with model prediction based on K(+) concentrations in water. Estimated annual effective dose received by adult members of the Croatian population due to consumption of carp contaminated with (134)Cs and (137)Cs are small: per capita dose from this source during 1987-2005 was estimated to be 0.5+/-0.2 microSv. Due to minor freshwater fish consumption in Croatia and low radiocaesium activity concentrations in carp, it can be concluded that carp consumption was not a critical pathway for the transfer of radiocaesium from fallout to humans after the Chernobyl accident.     

An assessment of two decades of trace metals monitoring in wild mussels from the Northwest Atlantic and Cantabrian coastal areas of Spain, 1991–2011

Since 1991, the Instituto Español de Oceanografía has monitored the concentrations of trace metals in wild mussels from the north (Cantabrian Sea) and northwest (Atlantic) coasts of Spain to define geographical distributions and temporal trends. While Cu, Zn and As concentrations presented fairly uniform geographical distributions, Hg and Pb concentrations were higher in mussels from the Cantabrian sea region as a result of historical anthropogenic activities. Cd, on the other hand, appeared to be more affected by natural processes on the northwest Atlantic coast (i.e., upwelling) than by human activity. Approximately 70% of the paired observations showed downward trends, 50% of these significant, with time. An improvement in environmental conditions along the northern coasts of Spain is evident despite that some metal levels resulted above the Background Assessment Concentrations given by OSPAR to assess potentially harmful occurrences.