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1.
Estimating risks of groundwater contamination often require schemes for representing and propagating uncertainties relative to model input parameters. The most popular method is the Monte Carlo method whereby cumulative probability distributions are randomly sampled in an iterative fashion. The shortcoming of the approach, however, arises when probability distributions are arbitrarily selected in situations where available information is incomplete or imprecise. In such situations, alternative modes of information representation can be used, for example the nested intervals known as “possibility distributions”. In practical situations of groundwater risk assessment, it is common that certain model parameters may be represented by single probability distributions (representing variability) because there are data to justify these distributions, while others are more faithfully represented by possibility distributions (representing imprecision) due to the partial nature of available information. This paper applies two recent methods, designed for the joint-propagation of variability and imprecision, to a groundwater contamination risk assessment. Results of the joint-propagation methods are compared to those obtained using both interval analysis and the Monte Carlo method with a hypothesis of stochastic independence between model parameters. The two joint-propagation methods provide results in the form of families of cumulative distributions of the probability of exceeding a certain value of groundwater concentration. These families are delimited by an upper cumulative distribution and a lower distribution respectively called Plausibility and Belief after evidence theory. Slight differences between the results of the two joint-propagation methods are explained by the different assumptions regarding parameter dependencies. Results highlight the point that non-conservative results may be obtained if single cumulative probability distributions are arbitrarily selected for model parameters in the face of imprecise information and the Monte Carlo method is used under the assumption of stochastic independence. The proposed joint-propagation methods provide upper and lower bounds for the probability of exceeding a tolerance threshold. As this may seem impractical in a risk-management context, it is proposed to introduce “a-posteriori subjectivity” (as opposed to the “a-priori subjectivity” introduced by the arbitrary selection of single probability distributions) by defining a single indicator of evidence as a weighted average of Plausibility and Belief, with weights to be defined according to the specific context.  相似文献   

2.
In order to carry out efficient traffic and air quality management, validated models and PM emission estimates are needed. This paper compares current available emission factor estimates for PM10 and PM2.5 from emission databases and different emission models, and validates these against eight high quality street pollution measurements in Denmark, Sweden, Germany, Finland and Austria.The data sets show large variation of the PM concentration and emission factors with season and with location. Consistently at all roads the PM10 and PM2.5 emission factors are lower in the summer month than the rest of the year. For example, PM10 emission factors are in average 5–45% lower during the month 6–10 compared to the annual average.The range of observed total emission factors (including non-exhaust emissions) for the different sites during summer conditions are 80–130 mg km−1 for PM10, 30–60 mg km−1 for PM2.5 and 20–50 mg km−1 for the exhaust emissions.We present two different strategies regarding modelling of PM emissions: (1) For Nordic conditions with strong seasonal variations due to studded tyres and the use of sand/salt as anti-skid treatment a time varying emission model is needed. An empirical model accounting for these Nordic conditions was previously developed in Sweden. (2) For other roads with a less pronounced seasonal variation (e.g. in Denmark, Germany, Austria) methods using a constant emission factor maybe appropriate. Two models are presented here.Further, we apply the different emission models to data sets outside the original countries. For example, we apply the “Swedish” model for two streets without studded tyre usage and the “German” model for Nordic data sets. The “Swedish” empirical model performs best for streets with studded tyre use, but was not able to improve the correlation versus measurements in comparison to using constant emission factors for the Danish side. The “German” method performed well for the streets without clear seasonal variation and reproduces the summer conditions for streets with pronounced seasonal variation. However, the seasonal variation of PM emission factors can be important even for countries not using studded tyres, e.g. in areas with cold weather and snow events using sand and de-icing materials. Here a constant emission factor probably will under-estimate the 90-percentiles and therefore a time varying emission model need to be used or developed for such areas.All emission factor models consistently indicate that a large part (about 50–85% depending on the location) of the total PM10 emissions originates from non-exhaust emissions. This implies that reduction measures for the exhaust part of the vehicle emissions will only have a limited effect on ambient PM10 levels.  相似文献   

3.
The Norwegian Meteorological Institute (DNMI) has developed and implemented for operational use a real-time dispersion model Severe Nuclear Accident Program (SNAP) with capability for predicting concentrations and depositions of the radioactive debris from large accidental releases. SNAP has been closely linked to DNMI’s operational numerical weather prediction (NWP) models.How good are these predictions? Participation in ETEX has partly answered this question. DNMI used SNAP with LAM50S giving meteorological input for these real-time dispersion calculations. LAM50S Limited Area Model with 50 km grid squareswas DNMI’s operational NWP model in 1994 when ETEX took place.In this article we report on how SNAP performed in the first of the ETEX releases in near-real-time mode, using LAM50S—and in hindcast mode for ATMES II, using “ECMWF 1995: ETEX Data set (ATMES II)”as meteorological input data. These two input data sets came from NWP models with quite different characteristics but with similar resolution in time and space.The results from these dispersion simulations matched closely. Deviations early in the simulation period shrank to insignificant differences later on. Since both input data sets were based on “weather analysis” and had similar resolution in space and time, SNAP described the dispersion of the released material very similar in these two simulations.  相似文献   

4.
When disposing nuclear waste in clay formations it is expected that the most radiotoxic elements like Pu, Np or Am move only a few centimetres to meters before they decay. Only a few radionuclides are able to reach the biosphere and contribute to their long-term exposure risks, mainly anionic species like I129, Cl36, Se79 and in some cases C14 and Tc99, whatever the scenario considered. The recent OECD/NEA cosponsored international MOFAP workshop focussed on transport and chemical behaviour of these less toxic radionuclides. New research themes have been addressed, such as how to make use of molecular level information for the understanding of the problem of migration at large distances. Diffusion studies need to face mineralogical heterogeneities over tens to hundreds of meters. Diffusion rates are very low since the clay rock pores are so small (few nm) that electrostatic repulsion limits the space available for anion diffusion (anion exclusion). The large volume of traversed rock will provide so many retention sites that despite weak retention, even certain of these “mobile” nuclides may show significant retardation. However, the question how to measure reliably very low retention parameters has been posed. An important issue is whether redox states or organic/inorganic speciation change from their initial state at the moment of release from the waste during long term contact with surfaces, hydrogen saturated environments, etc.  相似文献   

5.
Geochemical processes leading to either mobilization or retention of radionuclides in an aquifer system are significantly influenced by their interaction with rock, sediment and colloid surfaces. Therefore, a sound safety assessment of nuclear waste disposal requires the elucidation and quantification of those processes. State-of-the-art analytical techniques as e.g. laser- and X-ray spectroscopy are increasingly applied to study solid–liquid interface reactions to obtain molecular level speciation insight.We have studied the sorption of trivalent lanthanides and actinides onto aluminium oxides, hydroxides and purified clay minerals by the time-resolved laser fluorescence spectroscopy and X-ray-absorption spectroscopy. Chemical constitution and structure of surface bound actinides are proposed based on spectroscopic information. Open questions still remain with regard to the exact nature of mineral surface ligands and the mineral/water interface. Similarities of spectroscopic data obtained for M(III) sorbed onto γ-alumina, and clay minerals suggest the formation of very comparable inner-sphere surface complexes such as S–O–An(III)(OH)x(2 − x)(H2O)5 − x at pH > 5. Those speciation data are found consistent with those predicted by surface complexation modelling. The applicability of data obtained for pure mineral phases to actinide sorption onto heterogeneously composed natural clay rock is examined by experiments and by geochemical modelling. Good agreement of experiment and model calculations is found for U(VI) and trivalent actinide/lanthanide sorption to natural clay rock. The agreement of spectroscopy, geochemical modelling and batch experiments with natural rock samples and purified minerals increases the reliability in model predictions.The assessment of colloid borne actinide migration observed in various laboratory and field studies calls for detailed information on actinide–colloid interaction. Kinetic stabilization of colloid bound actinides can be due to inclusion into inorganic colloid matrix or by macromolecular rearrangement in case of organic, humic/fulvic like colloids. Only a combination of spectroscopy, microscopy and classical batch sorption experiments can help to elucidate the actinide–colloid interaction mechanisms and thus contribute to the assessment of colloids for radionuclide migration.  相似文献   

6.
Analyses of sludge from graphite electrodes used in the chloralkali process show total levels of PCDFs as high as 650000 pg/g sludge. The levels of tetra-, penta-and hexaCDFs were found to be approximately the same. The levels for the corresponding PCDDs were below the detection level. The dominating congeners within each group are the toxic 2,3,7,8-substituted PCDFs at levels of 340000 pg/g, This typical pattern, called the “chloralkali pattern” can also be found in soil samples taken at another chloralkali plant. The typical pattern can also be identified in a solution of ferric chloride. Traces of “chloralkali pattern” are identified in a sludge sample from the drinking water purification plant, the source for PCDFs in the sludge is unknown.  相似文献   

7.
8.
An understanding of particle migration in fractured rock, required to assess the potential for colloid-facilitated transport of radionuclides, can best be evaluated when the results of laboratory experiments are demonstrated in the field. Field-scale migration experiments with silica colloids were carried out at AECL's Underground Research Laboratory (URL), located in southern Manitoba, to develop the methodology for large-scale migration experiments and to determine whether colloid transport is possible over distances up to 17 m. In addition, these experiments were designed to evaluate the effects of flow rate and flow path geometry, and to determine whether colloid tracers could be used to provide additional information on subsurface transport to that provided by conservative tracers alone. The colloid migration studies were carried out as part of AECL's Transport Properties in Highly Fractured Rock Experiment, the objective of which was to develop and demonstrate methods for evaluating the solute transport characteristics of zones of highly fractured rock. The experiments were carried out within fracture zone 2 as two-well recirculating, two-well non-recirculating, and convergent flow tests, using injection rates of 5 and 10 1 min−1. Silica colloids with a 20 nm size were used because they are potentially mobile due to their stability, small size and negative surface charge. The shapes of elution profiles for colloids and conservative tracers were similar, demonstrating that colloids can migrate over distances of 17 m. The local region of drawdown towards the URL shaft affected colloid migration and, to a lesser extent, conservative tracer migration within the flow field established by the two-well tracer tests. These results indicate that stable colloids, with sizes as small as 20 nm, have different migration properties from dissolved conservative tracers. - 1997 Atomic Energy of Canada.  相似文献   

9.
A three-site cation exchange model is proposed to describe the concentration dependent uptake of Cs on natural argillaceous rock systems. Major premises in the model are that the sorption of Cs is dominated by the illite mineral component in the rock and that there is a fixed relationship between the site capacities of the three site types denoted as frayed edge, type II and planar sites. The definition of a “reference illite” with a cation exchange capacity of 0.2 equiv. kg-1 allows the three site capacities to be fixed in the model calculations over the weight fraction of illite in the argillaceous rocks. Up to Cs equilibrium concentrations of 10-3 M sorption occurs predominantly on the frayed edge and type II sites (higher affinity sites), with the planar site type playing only a minor role. Competition with Cs for sorption on the former two site types arises predominantly from monovalent cations such as K, Rb and NH4 which have low hydration energies. H and Na (except at high concentrations) are considerably less competitive and bivalent cations such as Mg, Ca and Sr are effectively non-competitive. A consistent set of selectivity coefficients for Cs with respect to K, Rb, NH4 and Na was derived from analyses and modelling of a wide range of Cs sorption data available in the open literature on pure illites from many different sources. The model was tested against four Cs sorption isotherm data sets determined on argillaceous rocks: Boom clay, Oxford clay, Palfris marl and Opalinus clay. The water chemistries and illite contents given in these experiments allowed the Cs sorption isotherms to be predicted. It is concluded that the Cs sorption model presented here, in which there are no free parameters, can be used to predict the uptake of Cs at equilibrium concentrations below 10-3 M to within a factor of 2 to 3 in natural argillaceous rock systems.  相似文献   

10.
Emissions from fugitive dust due to erosion of “natural” wind-blown surfaces are an increasingly important part of PM10 (particulate matter with sizes of 10 μm aerodynamic diameter) emission inventories. These inventories are particularly important to State Implementation Plans (SIP), the plan required for each state to file with the Federal government indicating how they will comply with the Federal Clean Air Act (FCAA). However, techniques for determining the fugitive dust contribution to over all PM10 emissions are still in their developmental stages. In the past, the methods have included field monitoring stations, specialized field studies and field wind-tunnel studies. The measurements made in this paper allow for systematic determination of PM10 emission rates through the use of an environmental boundary layer wind tunnel in the laboratory. Near surface steady-state concentration profiles and velocity profiles are obtained in order to use a control volume approach to estimate emission rates. This methodology is applied to soils retrieved from the nation's single largest PM10 source, Owens (dry) Lake in California, to estimate emission rates during active storm periods. The estimated emission rates are comparable to those obtained from field studies and lend to the validity of this method for determining fugitive dust emission rates.  相似文献   

11.
The chlorine bound in chlorinated fatty acids (ClFAs) have been concluded to contribute to a major part of the extractable organically bound chlorine found in fish and other aquatic biota. Despite ClFAs giving rise to toxic effects they appear not to be recognised as “xenobiotic” compounds by the organism. They are readily accumulated via food and incorporated into complex lipids to approximately the same extent as unchlorinated fatty acids and may thus be transferred from prey to predator in the food chain. The ClFAs thus diverge from traditional environmental pollutants, such as PCBs, in several aspects and their fate in the environment can not be predicted by conventional risk assessment methods.  相似文献   

12.
Different studies indicate that 19–38% of the Swedish ringed Mute Swans (Cygnus olor) are killed by collision with electrical wires. The relative frequency of killed swans is not related to the density or type of electrical wires in the landscape, but to where in the landscape the wires are constructed, and to the time when mass movements of swans occur. Experience (age), bodyweight (“too heavy to raise”), breast muscle weakening (“engine problems”) and heavy metal (lead) loads strongly affect the chances of birds avoiding collision; but, swans not belonging to these risk-groups are also killed. Different skeletal injuries were found in dead birds after collision but many of them were not lethal. It was proved, however, that most collision-birds ultimately died from liver damage, probably caused by their heavy bodies hitting the ground.  相似文献   

13.
Coupling geochemistry and transport appears unavoidable since it is rare that either of these two phenomena alone can account for the movement of solutes in groundwater. The chemical model is based on thermodynamic equilibrium. The method used is a Gibbs free energy minimization constrained by mass balances. The model calculates the aqueous speciation, the precipitation and the dissolution of pure minerals or solid solutions. The transport equation is solved by the random walk technique which avoids the problem of numerical dispersion for transport, but may be more time consuming than finite differences or elements if a large number of particles are necessary in order to get a sufficiently “smooth” solution. However, when the chemistry deals with a realistic number of elements (e.g., > 10), the cost of the chemistry computation largely dominates that of transport. Special techniques had to be developed in order to solve problems linked to the conditions present in some of the CEC CHEMVAL tests (boundary with fixed concentrations and very low Péclet numbers). The coupling consists of calculating the exchanges of chemical elements between two populations. The first population is sedentary, constituted by a mesh of fixed cells representing the composition of the solid phase. The other population is nomadic, represented by a set of particles which are advected by groundwater flow. A vector of real numbers is associated with each mobile particle. This vector accounts for the mass of each element dissolved in the moving liquid phase. For this reason, the transport equation is only solved once for the whole set of elements. The main assumptions that were necessary to perform the coupling in a simple way are discussed. Two applications are presented: (1) a verification compared to an analytical solution; and (2) the simulation of a percolation experiment through a sandstone core.  相似文献   

14.
Reactions between ozone and terpenes have been shown to increase the concentrations of submicron particles in indoor settings. The present study was designed to examine the influence of air exchange rates on the concentrations of these secondary organic aerosols as well as on the evolution of their particle size distributions. The experiments were performed in a manipulated office setting containing a constant source of d-limonene and an ozone generator that was remotely turned “on” or “off” at 6 h intervals. The particle number concentrations were monitored using an optical particle counter with eight-channels ranging from 0.1–0.2 to>2.0 μm diameter. The air exchange rates during the experiments were either high (working hours) or low (non-working hours) and ranged from 1.6 to>12 h−1, with intermediate exchange rates. Given the emission rates of ozone and d-limonene used in these studies, at an air exchange rate of 1.6 h−1 particle number concentration in the 0.1–0.2 μm size-range peaked 1.2 h after the ozone generator was switched on. In the ensuing 4.8 h particle counts increased in successive size-ranges up to the 0.5–0.7 μm diameter range. At higher air exchange rates, the resulting concentrations of total particles and particle mass (calculated from particle counts) were smaller, and at exchange rates exceeding 12 h−1, no excess particle formation was detectable with the instrument used in this study. Particle size evolved through accretion and, in some cases, coagulation. There was evidence for coagulation among particles in the smallest size-range at low air exchange rates (high particle concentrations) but no evidence of coagulation was apparent at higher air exchange rates (lower particle concentrations). At higher air exchange rates the particle count or size distributions were shifted towards smaller particle diameters and less time was required to achieve the maximum concentration in each of the size-ranges where discernable particle growth occurred. These results illustrate still another way in which ventilation affects human exposures in indoor settings. However, the ultimate effects of these exposures on health and well being remain to be determined.  相似文献   

15.
Within the Swedish Dioxin Survey various samples from the pulp and paper industry and the chloralkali process have been analyzed by congener specific analytical methods. In addition to the generally discussed “bleaching pattern” of the tetrachlorinated congeners, these samples also contained higher chlorinated congeners like hexa-CDDs, hepta-CDFs, octa-CDD and octa-CDF. Consequently it is recommended that samples from the pulp industry should be analyzed for all PCDDs and PCDFs (tetra- through octa-). Counted as Nordic Toxic Equivalents (NTEQ), the recycled pulp samples had the highest contamination level followed by TMP, unbleached sulfite and bleached softwood and hardwood. In addition to the bleaching process, various chemicals used in the pulping, bleaching and wastewater treatment can contribute to the contamination.  相似文献   

16.
The objective of this study is to investigate the air ventilation impacts of the so called “wall effect” caused by the alignment of high-rise buildings in complex building clusters. The research method employs the numerical algorithm of computational fluid dynamics (CFD – FLUENT) to simulate the steady-state wind field in a typical Hong Kong urban setting and investigate pollutant dispersion inside the street canyon utilizing a pollutant transport model. The model settings of validation study were accomplished by comparing the simulation wind field around a single building block to wind tunnel data. The results revealed that our model simulation is fairly close to the wind tunnel measurements. In this paper, a typical dense building distribution in Hong Kong with 2 incident wind directions (0° and 22.5°) is studied. Two performance indicators are used to quantify the air ventilation impacts, namely the velocity ratio (VR) and the retention time (Tr) of pollutants at the street level. The results indicated that the velocity ratio at 2 m above ground was reduced 40% and retention time of pollutants increased 80% inside the street canyon when high-rise buildings with 4 times height of the street canyon were aligned as a “wall” upstream. While this reduction of air ventilation was anticipated, the magnitude is significant and this result clearly has important implications for building and urban planning.  相似文献   

17.
The code system containing the DELTA and the ADREA codes has been developed at the National Centre of Scientific Research (NCSR) “DEMOKRITOS” and performs mesoscale wind field calculations over terrains of high complexity. The code system follows a particular technique of discretization, according to which the ground can be treated with a resolution higher than the one used in the atmosphere. This technique, called “the high-resolution-ground-low-resolution-air” concept, offers to the code system the capability to reliably simulate the thermal air-ground interaction processes, keeping at the same time the computation storage and duration in reasonable levels. The above code system was applied to a high-resol ution representation of the Attika district, within a domain of 72 × 72 × 6.125 km3. Mesoscale wind field calculations were made within the framework of the APSIS Phase-A Intercomparison Exercise, using the atmospheric radiosonde and surface data of 25 May 1990. In this particular day, the greater Athens area was dominated by the daytime thermally driven local systems, generated along the coastlines of the peninsula. The application of the DELTA-ADREA system reproduced the above mesoscale influences and exhibited a favourable agreement with observations.  相似文献   

18.
Simultaneous size distributions and Fourier transform infrared (FTIR) extinction spectra have been measured for several representative components of mineral dust aerosol (quartz, calcite, and dolomite) in the fine particle size mode (D=0.1–1 μm). Optical constants drawn from the published literature have been used in combination with the experimentally determined size distributions to simulate the extinction spectra. In general, Mie theory does not accurately reproduce the peak position or band shape for the prominent IR resonance features in the 800–1600 cm−1 spectral range. The resonance peaks in the Mie simulation are consistently blue shifted relative to the experimental spectra by 20–50 cm−1. Spectral simulations, derived from a simple Rayleigh-based analytic theory for a “continuous distribution of ellipsoids” particle shape model, better reproduce the experimental spectra, despite the fact that the Rayleigh approximation is not strictly satisfied in these experiments. These results differ from our previous studies of particle shape effects in silicate clay mineral dust aerosols where a disk-shaped model for the particles was found to be more appropriate.  相似文献   

19.
Six years (1998–2003) of measurements of ambient air concentrations of total suspended particulate (TSP) measured at a rural background monitoring station in Tenerife (Canary Islands), the El Río station (ER, 28°08′35″N, 16°39′20″W, 500 m a.s.l.) were studied. African dust outbreaks were objectively identified using a new quantitative tool, called the African Index. This index indicates the percentage of time that an air mass remained over an African region at one of three possible height intervals of the lower troposphere. After identifying these episodes, a study of the background TSP levels at the ER station and of direct and indirect (those which cause vertical deposition of dust) African air mass intrusion impacts was performed. Taking into account both direct and indirect episodes, a total of 322 days of African dust intrusion were objectively identified (a mean of 54 episodes per year) in the period 1998–2003, some of them caused by “transition episodes” or “return African air masses”. A subjective method confirmed that 256 of these days were caused by direct impacts of African dust on the ER station. A mean TSP value of 21.6 μg m−3 was found at the station during this period. All the episodes occurred when the TSP concentration was >28.5 μg m−3. The TSP background (14 μg m−3) can be assumed to be representative of the MBL of the Eastern North Atlantic subtropical region. The highest number of dust gravitational settlement (or indirect) episodes occurs in summer, but the highest contribution of these episodes to the TSP levels is in March with a monthly mean TSP contribution of up to 30.5 μg m−3.  相似文献   

20.
Sorption of emitted gas-phase organic compounds onto material surfaces affects environmental tobacco smoke (ETS) composition and exposures indoors. We have introduced a new metric, the exposure relevant emission factor (EREF) that accounts for sorptive uptake and reemission to give the mass of individual ETS constituents available for exposure over a day in which smoking occurs. This paper describes month-long experiments to investigate sorption effects on EREFs and potential ETS exposures under habitual smoking conditions. Cigarettes were smoked in a 50-m3 furnished room over a 3-h period 6–7 days per week, with continuous ventilation at 0.3, 0.6, or 2.1 h−1. Organic gas concentrations were measured every few days over 4-h “smoking”, 10-h “post-smoking” and 10-h “background” periods. Concentration patterns of volatile ETS components including 1,3-butadiene, benzene and acrolein were similar to those calculated for a theoretical non-sorbing tracer, indicating limited sorption. Concentrations of ETS tracers, e.g. 3-ethenylpyridine (3-EP) and nicotine, and lower volatility toxic air contaminants including phenol, cresols, and naphthalene increased as experiments progressed, indicating mass accumulation on surfaces and higher desorption rates. Daily patterns stabilized after week 2, yielding a steady daily cycle of ETS concentrations associated with habitual smoking. EREFs for sorbing compounds were higher under steady cycle versus single-day smoking conditions by 50% for 3-EP, and by 2–3 times for nicotine, phenol, cresols, naphthalene, and methylnaphthalenes. Our results provide relevant information about potential indirect exposures from residual ETS (non-smoker enters room shortly after smoker finishes) and from reemission, and their importance relative to direct exposures (non-smoker present during smoking). Under the conditions examined, indirect exposures accounted for a larger fraction of total potential exposures for sorbing versus non-sorbing compounds, and at lower versus higher ventilation rates. Increasing ventilation can reduce indirect exposures to very low levels for non-sorbing ETS components, but indirect routes accounted for 50% of potential nicotine exposures during non-smoking periods at all ventilation rates.  相似文献   

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