On the sensitivity of a marine dispersion model to parameters describing the transfers of radionuclides between the liquid and solid phases

The sensitivity of a marine dispersion model for non-conservative radionuclides, previously developed and validated for the English Channel, to parameters describing the exchanges between the liquid and solid phases (suspended matter and bottom sediments) has been studied using a Monte Carlo method. A probability distribution is assigned to each parameter. They are sampled to obtain a set of model parameters and a model run is carried out. This process is repeated to obtain a distribution of model outputs. Partial correlation coefficients are calculated to assess the relative influence of each parameter on model output. Errors are also assigned to model results. Three situations are studied: an instantaneous release of radionuclides, a continuous release and the case of a contaminated sediment behaving as a long-term source of radionuclides. Calculations have also been carried out for two radionuclides with different geochemical behaviour: (137)Cs and (239,240)Pu. The results indicate that all parameters are relevant, depending on the phase we are interested in obtaining the result and on the source term (instantaneous, continuous or due to sediments). However, parameters that are, in general, more influential are kinetic rates, mixing depth in the sediment and mean radius of suspended and sediment particles. This suggests that including several particle sizes in future radionuclide dispersion models could lead to an improvement in model results. Differences have also been found with respect to the relevance of some parameters depending on the geochemical behaviour of the radionuclide.     

Kinetics of the adsorption and desorption of radionuclides of Co, Mn, Cs, Fe, Ag and Cd in freshwater systems: experimental and modelling approaches

The sorption and release kinetics of 54Mn, 58Co, 59Fe, 109Cd, 110mAg and 134Cs by freshwater suspended particles were investigated to better identify the biogeochemical processes involved and to obtain suitable data for improving models describing radionuclide migration in freshwater streams. In order to observe any seasonal variability in the interaction of radionuclides with natural particles, experiments were performed both in winter and in summer during a phytoplanktonic bloom. Two kinetic models are compared in this paper: the "one-step reversible" model, based on the hypothesis that the transfer of radionuclides between water and suspended solids is governed by a reversible reaction, and the "two-successive-step reversible" model, which assumes two distinct types of sites or reactions on the solid phase. The "one-step reversible" model is generally unable to describe properly the exchange kinetics; this result shows that at least two processes are generally involved in radionuclide exchange between water and suspended particles. On the contrary, a model involving the existence of two successive reversible reactions properly simultes both the sorption and release kinetics. The determination of the kinetic coefficients allows quantitative assessment of the relative importance and kinetics of the processes. In particular, it has been shown that, except for Cs and Cd, major fractions of the radionuclides are associated at equilibrium with particulate sites involving strong interactions. The kinetics to reach this equilibrium depend on seasonal conditions, especially for Co and Mn: the transfer of Co and Mn to particulate sites involving strong interactions is much slower in winter. The distribution of the radionuclides between water and particulate sites involving weak interactions also shows seasonal variations for Co, Mn, Fe and Ag: the capacity to associate radionuclides is much higher in summer for Co and Mn, while the inverse tendency is observed for Fe and Ag. For Cs and Cd, no significant seasonal differences were observed.     

Modelling the physico-chemical speciation of plutonium in the eastern Irish Sea: a further development

A numerical full three-dimensional model previously developed to simulate the physicochemical speciation of plutonium in the eastern Irish Sea has been improved. The model solves simultaneously the hydrodynamic equations, the suspended matter equation and the equations that give the time evolution of Pu concentrations in water, suspended matter and bottom sediments. It is considered that Pu may exist in each phase in two different oxidation states. Redox reactions are also considered. In the earlier version of the model, a one-step kinetic model was used to describe the transfers of radionuclides between the dissolved and solid phases. Although with this kind of model the contamination of the sediments can be properly simulated, it is clearly not able to describe the re-dissolution of radionuclides from a contaminated sediment once the external source to the sea is reduced. Thus, the model has been improved by substituting the one-step model with a two-step kinetic model consisting of two consecutive reversible reactions. Now it is possible to simulate both the sediment contamination and the re-dissolution processes.     

A particle-tracking method for simulating the dispersion of non-conservative radionuclides in coastal waters.

A particle-tracking method has been used to simulate the dispersion of non-conservative radionuclides in the sea. Three dimensional turbulent diffusion and the interactions between water, suspended matter and bottom sediments are simulated using a stochastic method. Kinetic transfer coefficients, as in finite difference models, are used to describe the transfers between the liquid and solid phases. Deposition of suspended matter and erosion of sediment are also included in the model. The method has been applied to simulate the dispersion of 137Cs and (239,240)Pu in the English Channel and the results have been compared with those of a finite difference model. The results from both techniques are, in general, in good agreement.     

Modeling 137Cs migration processes in lake sediments

Lake sediments can be considered as the "diary" of the lake: new layers are continuously deposited on top of the sediments. The migration behavior of radionuclides, particularly of (137)Cs, can be analyzed by modeling the input into and the vertical distribution within the sediment. For this purpose, a model consisting of sedimentation-diffusion equations was developed. Solved with a finite element method, this model can cover the time period from the nuclear weapons testing to the present. It takes into account fixation and redissolution, compaction of sediments, and the influence of competing ions on the retarded diffusion within the sediments. The outcome of the model is compared to water and sediment measurements from Lago Maggiore. The results of an optimization process can produce the sedimentation rate and (137)Cs distribution coefficients which determine the uptake of activity into the sediment and also the retarded diffusion within the sediment.     

Fixation of Cs to marine sediments estimated by a stochastic modelling approach

Dumping of nuclear waste in the Kara Sea represents a potential source of radioactive contamination to the Arctic Seas in the future. The mobility of 137Cs ions leached from the waste will depend on the interactions with sediment particles. Whether sediments will act as a continuous permanent sink for released 137Cs, or contaminated sediments will serve as a diffuse source of 137Cs in the future, depends on the interaction kinetics and binding mechanisms involved. The main purpose of this paper is to study the performance of different stochastic models using kinetic information to estimate the time needed for Cs ions to become irreversibly fixed within the sediments. The kinetic information was obtained from 134Cs tracer sorption and desorption (sequential extractions) experiments, conducted over time, using sediments from the Stepovogo Fjord waste dumping site, on the east coast of Novaya Zemlya. Results show that 134Cs ions interact rapidly with the surfaces of the Stepovogo sediment, with an estimated distribution coefficient Kd(eq) of 300 ml/g (or 13m2/g), and the 134Cs ions are increasingly irreversibly fixed to the sediment over time. For the first time, stochastic theory has been utilised for sediment-seawater systems to estimate the mean residence times (MRTs) of Cs ions in operationally defined sediment phases described by compartment models. In the present work, two different stochastic models (i) a Markov process model (MP) being analogous to deterministic compartment models, and (ii) a semi-Markov process model (SMP) which should be physically more relevant for inhomogeneous systems, have been compared. As similar results were obtained using the two models, the less complicated MP model was utilised to predict the time needed for an average Cs ion to become irreversibly fixed in the Stepovogo sediments. According the model, approximately 1100 days of contact time between Cs ions and sediments is needed before 50% of the 134Cs ion becomes fixed in the irreversible sediment phase. while about 12.5 years are needed before 99.7% of the Cs ions are fixed. Thus, according to the model estimates the contact time between 137Cs ions leached from dumped waste and the Stepovogo Fjord sediment should be about 3 years before the sediment will act as an efficient permanent sink. Until then a significant fraction of 137Cs should be considered mobile. The stochastic modelling approach provides useful tools when assessing sediment-seawater interactions over time, and should be easily applicable to all sediment-seawater systems including a sink term.     

A review of factors affecting the release and bioavailability of contaminants during sediment disturbance events

The factors affecting the release and bioavailability of contaminants present in sediments during natural and anthropogenic disturbance events are discussed and our current state of understanding of these processes reviewed. Published data are focused on the distribution of contaminants within undisturbed sediment, their affinities to the various solid-phase fractions of sediment and the interaction of contaminants between sediment and pore water. Sediment disturbance can lead to changes in the chemical properties of sediment that stimulate the mobilisation of contaminants. Research shows that changes in both redox potential (Eh) and pH can accelerate desorption, partitioning, bacterial degradation and the oxidation of organic contaminants. However, these processes are both sediment- and compound-specific. By affecting the affinity of contaminants to sediments, disturbance events in turn can have a significant effect on their bioavailability. Few studies have examined this phenomenon, and it is clear from the data available that there are gaps in our understanding in a number of key areas when assessing the release of contaminants from sediments: the fate of contaminants in undisturbed sediments and those that are not subjected to major disturbances, the kinetic processes that regulate metal release during changes in redox potential, the release of organometallic compounds from sediments during resuspension, the bioavailability of organic and organometallic compounds and the processes affecting contaminant release.     

The dispersion of 137Cs and 239,240Pu in the Rhone River plume: a numerical model

A numerical three dimensional model to simulate the transport of Cs and Pu by the Rhone River plume has been developed. The model solves the hydrodynamic equations, including baroclinic terms (that account for density variations) and a turbulence model, the suspended matter equations, including several particle classes simultaneously, settling, deposition and erosion of the sediment, and the radionuclide dispersion equations. Exchanges of radionuclides between the liquid and solid phases are described in terms of kinetic transfer coefficients. The dependence of these coefficients with water salinity is explicitly included in the model since it changes from freshwater to seawater values in the model domain. Computed activity levels in water, suspended matter and bed sediments are, in general, in agreement with measurements in the area. The model can also give a wide amount of information, as distribution coefficients for total suspended matter and sediments and for each particle class, fractions of radionuclides fixed to solid particles, and vertical profiles of radionuclides and distribution coefficients.     

长江口南港北槽河床底质时空分布特征分析

在前人研究及大量长时间、连续、大范围河床底质现场采样资料的基础上,对长江口南港北槽河床底质时空分布特征进行了初步分析,并从河床底质的角度对长江口深水航道回淤物质来源进行了初步的探讨。研究表明:长江口河床质具有总体较细、上粗下细以及时空分布不均匀等特点;南港北槽河床质的变化与风浪掀沙、底沙过境、洪枯季变化等因素有关;南港段河床质季节性变化大于北槽;南港河段河床底质有细化的趋势;长江口深水航道回淤物质偏粗且与周边河床质组成相近,航道回淤应关注滩槽泥沙以近底高含沙水流方式的交换。     

A modelling study on 137Cs and 239,240Pu behaviour in the Alborán Sea, western Mediterranean

A model for simulating the dispersion processes of 137Cs and 239,240Pu in the Alborán Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of 137Cs and 239,240Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.     

大九湖泥炭藓湿地对磷、铜污染物净化作用的模拟研究

在大九湖泥炭藓沼泽湿地采用野外实地模拟方法,就泥炭藓湿地对铜、磷两种污染物的净化能力进行了研究。结果表明,磷污染物浓度分别为10,100,1 000 mg/L时,两小时后泥炭藓湿地对该污染物的净化率分别为939%,695%,663%;同样的浓度梯度下,对铜污染物的净化率分别为1000%,976%,880%。泥炭藓湿地对污染物具有很强的净化能力,其泥炭层部分在湿地净化污染物中起到重要作用。利用拟一级动力学模型、修改上限的拟一级动力学模型、拟二级动力学模型、Elovich模型、双常数速率模型、抛物线扩散模型等6个模型对泥炭藓湿地的净化进行动态研究,其中后4个模型均可模拟湿地净化的动态过程。长期预测以拟二级动力学模型为最佳。     

The influence of a whole-lake addition of stable cesium on the remobilization of aged 137Cs in a contaminated reservoir

To document the short-term dynamics of Cs, 4 kg of (133)Cs were introduced into an 11.4-ha, 157 000 m(3) reservoir previously contaminated with (137)Cs from past reactor operations at the US Department of Energy's Savannah River Site near Aiken, South Carolina, USA. The (133)Cs addition resulted in an increase of 6.1 MBq of (137)Cs (1.9 mug (137)Cs) in the water column over the following 260 days. Possible sources for the increased (137)Cs included (1) release from the sediments, (2) release from the approximately 26 000 kg of aquatic macrophytes that occupied 80% of the reservoir, and (3) wash-in from the pond's watershed. Data are presented to indicate that release from the sediments was the principal source of the (137)Cs increase. The fraction of (137)Cs released from the sediments (0.7%) is consistent with laboratory measurements of (137)Cs desorption from neighboring ponds on the Savannah River Site.     

Estimating biological half-lifes of radionuclides in marine compartments from environmental time-series measurements

Modelling radionuclide transfers between seawater and marine species on a short time scale basis requires being able to take into account the transfer kinetics. This means (1) to implement the effect of the biological half-lives of radionuclides together with the concentration factor in the calculation of transfers and (2), to get these kinetic parameters for each element and species. Biological half-lives are usually determined from laboratory labelling experiments with the challenge to match natural environmental conditions. The present work proposes a simple model that implements the effect of kinetic parameters in the calculation of transfers. This model is also used to derive the biological half-life and the concentration factor for 137Cs from time-series measurements of environmental concentrations in seawater and in the brown alga Fucus serratus, as an example. These transfer parameters are finally used to predict the Cs activities in Fucus serratus on the English Channel shores.     

典型城内过富营养湖泊沉积物和间隙水中各形态磷的相关性研究

研究了武汉市繁华市中心典型过富营养湖泊沉积物—间隙水体系磷形态的相关性。对沉积物—间隙水中磷形态的连续提取分析发现,自然粒度下,沉积物中有机质含量与沉积物中有机/细菌聚合磷存在很好的线性相关性,说明沉积物中有机质是有机/细菌聚合磷的源;沉积物中总磷决定间隙水中总溶解性磷和溶解性磷酸盐的含量,并且总磷与间隙水中总溶解性磷和溶解性磷酸盐存在很好的相关性;沉积物中Fe P和Al P分别与间隙水中的Eh和溶解性磷酸盐存在相关性,说明Eh的大小严重影响Fe P和Al P的含量,但是Fe P和Al P含量之和又主导着间隙水中溶解性磷酸盐的含量。对典型市内过富营养湖泊的沉积物－间隙水体系中形态磷的相关性研究,旨在为控制这种典型过富营养湖泊沉积物中磷向水体释放提供理论参考。     

The precautionary principle and chemicals management: The example of perfluoroalkyl acids in groundwater

Already in the late 1990s microgram-per-liter levels of perfluorooctane sulfonate (PFOS) were measured in water samples from areas where fire-fighting foams were used or spilled. Despite these early warnings, the problems of groundwater, and thus drinking water, contaminated with perfluoroalkyl and polyfluoroalkyl substances (PFASs) including PFOS are only beginning to be addressed. It is clear that this PFAS contamination is poorly reversible and that the societal costs of clean-up will be high. This inability to reverse exposure in a reasonable timeframe is a major motivation for application of the precautionary principle in chemicals management. We conclude that exposure can be poorly reversible; 1) due to slow elimination kinetics in organisms, or 2) due to poorly reversible environmental contamination that leads to continuous exposure. In the second case, which is relevant for contaminated groundwater, the reversibility of exposure is not related to the magnitude of a chemical's bioaccumulation potential. We argue therefore that all PFASs entering groundwater, irrespective of their perfluoroalkyl chain length and bioaccumulation potential, will result in poorly reversible exposures and risks as well as further clean-up costs for society. To protect groundwater resources for future generations, society should consider a precautionary approach to chemicals management and prevent the use and release of highly persistent and mobile chemicals such as PFASs.     

Environmental degradation by mud in tropical estuaries

In wet tropical countries, the intense rainfall and the lack of effective restrictions on human activities in the river catchment leads to increased rates of soil erosion. This has increased the sediment loads many times over from the natural level. As a result, estuarine and coastal waters are becoming increasingly muddy with associated losses for society in terms of increased flooding and a degradation of the environment, the fisheries and the economic use of these waters. It is suggested that science-based models be used to predict the fate of mud in estuaries and coastal waters when planning development in river catchments, particularly in wet tropical countries. This would help integrate land and water management. Modelling technology is demonstrated by a combination of field and model studies in four turbid tropical estuaries, namely the Fly River in Papua New Guinea, the Mekong River in Vietnam, the Cimanuk River in Indonesia, and Hinchinbrook Channel in Australia. The final model is adapted to local conditions and extensively uses data assimilation especially for open boundary conditions. There can be a feedback between the hydrodynamics and the mud dynamics when the system silts; in wet tropical countries this can occur rapidly, sometimes in only 30 years. Electronic Publication     

长江河口淡水资源利用与避咸蓄淡水库

开发利用长江口的淡水资源,首先要研究河口水质的污染程度以及咸潮入侵的时空变化规律。长江河口水质除边滩存在局部污染外,主槽水质良好。长江口南支、南港、北港盐水来源主要有北支倒灌和外海盐水直接入侵两种形式,盐水入侵具有周日、半月、季节和年际变化规律,由于北支倒灌咸水团的影响,低盐度值往往出现在大潮期和涨憩附近,通过修建边滩水库,达到控制引水时间、避咸蓄谈的目的。最长连续超标天数的推算是确定水库库容的关键问题,采用数理统计、二维数值模拟、ARMAX模型＋Markov模型等方法推算,几种方法相互印证,计算结果基本上符合实际情况。“避咸潮取水,蓄淡水保质”,这是宝钢干部、科技人员总结出来的长江河口引水经验。长江口取水工程由取水系统、调蓄水库和输水系统等三大部分组成。长江口避咸蓄淡水库的成功经验,对沿海潮汐河口的淡水资源开发利用具有示范作用。     

长江河口淡水资源利用与避咸蓄淡水库

开发利用长江口的淡水资源 ,首先要研究河口水质的污染程度以及咸潮入侵的时空变化规律。长江河口水质除边滩存在局部污染外 ,主槽水质良好。长江口南支、南港、北港盐水来源主要有北支倒灌和外海盐水直接入侵两种形式 ,盐水入侵具有周日、半月、季节和年际变化规律 ,由于北支倒灌咸水团的影响 ,低盐度值往往出现在大潮期和涨憩附近。通过修建边滩水库 ,达到控制引水时间、避咸蓄淡的目的。最长连续超标天数的推算是确定水库库容的关键问题 ,采用数理统计、二维数值模拟、ARMAX模型 +Markov模型等方法推算 ,几种方法相互印证 ,计算结果基本上符合实际情况。“避咸潮取水 ,蓄淡水保质” ,这是宝钢干部、科技人员总结出来的长江河口引水经验。长江口取水工程由取水系统、调蓄水库和输水系统等三大部分组成。长江口避咸蓄淡水库的成功经验 ,对沿海潮汐河口的淡水资源开发利用具有示范作用。     

A blind test of the MOIRA lake model for radiocesium for Lake Uruskul, Russia, contaminated by fallout from the Kyshtym accident in 1957

This paper presents results of a model-test carried out within the framework of the COMETES project (EU). The tested model is a new lake model for radiocesium to be used within the MOIRA decision support system (DSS; MOIRA and COMETES are acronyms for EU-projects). This model has previously been validated against independent data from many lakes covering a wide domain of lake characteristics and been demonstrated to yield excellent predictive power (see H?kanson, Modelling Radiocesium in Lakes and Coastal Areas. Kluwer, Dordrecht, 2000, 215 pp). However, the model has not been tested before for cases other than those related to the Chernobyl fallout in 1986, nor for lakes from this part of the world (Southern Urals) and nor for situations with such heavy fallout as this. The aims of this work were: (1) to carry out a blind test of the model for the case of continental Lake Uruskul, heavily contaminated with 90Sr and 137Cs as a result of the Kyshtym radiation accident (29 September 1957) in the Southern Urals, Russia, and (2) if these tests gave satisfactory results to reconstruct the radiocesium dynamics for fish, water and sediments in the lake. Can the model provide meaningful predictions in a situation such as this? The answer is yes, although there are reservations due to the scarcity of reliable empirical data. From the modelling calculations, it may be noted that the maximum levels of 137Cs in fish (here 400 g ww goldfish), water and sediments were about 100,000 Bq/kg ww, 600 Bq/l and 30,000 Bq/kg dw, respectively. The values in fish are comparable to or higher than the levels in fish in the cooling pond of the Chernobyl NPP. The model also predicts an interesting seasonal pattern in 137Cs levels in sediments. There is also a characteristic "three phase" development for the 137Cs levels in fish: first an initial stage when the 137Cs concentrations in fish approach a maximum value, then a phase with relatively short ecological half-lives followed by a final phase with long ecological half-lives more or less corresponding to the physical decay of radiocesium.