Radionuclide transfer to freshwater biota species: review of Russian language studies

Around 130 publications reporting studies on radionuclide transfer to freshwater biota species conducted in the former USSR were reviewed to provide the concentration ratio values. None of these studies were available up to now in the English language reviews or publications. The values derived have been compared with the CR values used for freshwater systems in the International reviews. For some radionuclides reviewed in this paper, the data are in good agreement with the mean CR values presented earlier, however for some of them, in particular, for ²⁴¹Am (bivalve molluscs, gastropods and pelagic fish), ⁶⁰Co (gastropods, benthic fish and insect larvae), ⁹⁰Sr and ¹³⁷Cs (benthic fish and zooplankton), the mean values given here are substantially different from those presented earlier. The data reported in this paper for thirty five radionuclides and eleven groups of freshwater species markedly improve the extent of available data for evaluation of radiation impact on freshwater species.     

Short- and long-term patterns of ¹³⁷Cs in fish and other aquatic organisms of small forest lakes in southern Finland since the Chernobyl accident

We summarize the patterns of ¹³⁷Cs activity concentrations and transfer into fish and other biota in four small forest lakes in southern Finland during a twenty-year period following the Chernobyl accident in April 1986. The results from summer 1986 showed fastest accumulation of ¹³⁷Cs into planktivorous fishes, i.e. along the shortest food chains. Since 1987, the highest annual mean values of ¹³⁷Cs have been recorded in fish occupying the highest trophic levels, for perch (Perca fluviatilis) 13,600 Bq/kg (ww) and for pike (Esox lucius) 20,700 Bq/kg (ww). At the same time, activity concentrations of ¹³⁷Cs in crustacean zooplankton and Asellus aquaticus have ranged between 1000 and 19,500 Bq/kg (dw). In 2006, 5-28% of the 1987 ¹³⁷Cs activity concentration levels were still present in perch and pike. Since 1989 their ¹³⁷Cs activity concentrations in oligohumic seepage lakes have remained significantly higher than in polyhumic drainage lakes due to the increased transfer of ¹³⁷Cs into fish in the seepage lakes with lower electrolyte concentrations, longer water retention times and lower sedimentation rate.     

Derivation of hazardous doses for amphibians acutely exposed to ionising radiation

Derivation of effect benchmark values for each taxonomic group, which has been difficult due to lack of experimental effects data, is required for more adequate protection of the environment from ionising radiation. Estimation of effects doses from nuclear DNA mass and subsequent species sensitivity distribution (SSD) analysis were proposed as a method for such a derivation in acute irradiation situations for assumed nuclear accident scenarios. As a case study, 5% hazardous doses (HD₅s), at which only 5% of species are acutely affected at 50% or higher lethality, were estimated on a global scale. After nuclear DNA mass data were obtained from a database, 50% lethal doses (LD₅₀s) for 4.8 and 36% of the global Anura and Caudata species, respectively, were estimated by correlative equations between nuclear DNA mass and LD₅₀s. Differences between estimated and experimental LD₅₀s were within a factor of three. The HD₅s obtained by the SSD analysis of these estimated LD₅₀s data were 5.0 and 3.1 Gy for Anura and Caudata, respectively. This approach was also applied to the derivation of regional HD₅s. The respective HD₅s were 6.5 and 3.2 Gy for Anura and Caudata inhabiting Japan. This HD₅ value for the Japanese Anura was significantly higher than the global value, while Caudata had no significant difference in global and Japanese HD₅s. These results suggest that this approach is also useful for derivation of regional benchmark values, some of which are likely different from the global values.     

New best estimates for radionuclide solid–liquid distribution coefficients in soils. Part 2. Naturally occurring radionuclides

Predicting the transfer of radionuclides in the environment for normal release, accidental, disposal or remediation scenarios in order to assess exposure requires the availability of an important number of generic parameter values. One of the key parameters in environmental assessment is the solid liquid distribution coefficient, K_d, which is used to predict radionuclide–soil interaction and subsequent radionuclide transport in the soil column. This article presents a review of K_d values for uranium, radium, lead, polonium and thorium based on an extensive literature survey, including recent publications. The K_d estimates were presented per soil groups defined by their texture and organic matter content (Sand, Loam, Clay and Organic), although the texture class seemed not to significantly affect K_d. Where relevant, other K_d classification systems are proposed and correlations with soil parameters are highlighted. The K_d values obtained in this compilation are compared with earlier review data.     

The assumption of linearity in soil and plant concentration ratios: An experimental evaluation

We have evaluated one of the main assumptions in the use of concentration ratios to describe the transfer of elements in the environment. The ratios examined in detail were the ‘concentration ratio’ (CR) of leaf to soil and the ‘partition coefficient’ of (K_d) of solid- to liquid-phase concentrations in soil. The ‘translocation ratio’ of berry to leaf was also computed when possible. Use of these ratios implies a linear relationship between the concentrations. Soil was experimentally contaminated to evaluate this linearity over more than a 1000-fold range in concentration. A secondary objective was to determine CR and K_d values in a long-term (2 y) outdoor study using a peat soil and a slow-growing native plant species, specifically blueberries (Vaccinium angustifolium). The elements I, Se, CS, Pb and U wer chosen as environmentally important elements expected to provide a broad range in CR and K_d values. the reuslts indicated that relationships of leaf and leachate concentrations were not consistently linearly related to the total soil concentrations for each of the elements. The modelling difficulties implied by these concentration dependencies can be partially offset by including in the models the strong negative correlation between CR and K_d. The error introduced by using a mean value of the ratios for Se or U resulted in up to a ten-fold increase in variability for CR and a three-fold increase for K_d.     

Measurement of transuranic elements,chiefly 237Np (by neutron activation analysis), in the physical and biological compartments of the French shore of the English channel

The behaviour of transuranic elements in the marine environment has been studied via both in situ sampling and laboratory tracer experiments. In particular, the radionuclide ²³⁷Np was investigated and techniques for its quantitative determination are described. In the field investigations, a preliminary separation of Np from samples was performed prior to neutron activation analysis, with subsequent γ-ray spectrometry of ²³⁸Np. In the laboratory studies, ²³⁷Np was determined by a radiochemical method followed by α-spectrometry. The results obtained from the in situ study in the English Channel (sea water, seaweed, molluscs) and from laboratory-uptake experiments (water and mussels) are described. Levels of Pu, Am and Np are compared and the characteristics of neptunium transfer to molluscs are discussed.     

A study of the growth and decay of cigarette smoke NOx in ambient air under controlled conditions

The amount of NO₂ and NO produced by the machine smoking of cigarettes was determined for 15 commercial Canadian brands. Average yield of NO was 1.44 μmoles or about 13% of the average reported for American cigarettes. Levels of NO₂ were less than 12% of NO and were probably due to the oxidation of NO. In order to assess the contribution of tobacco smoke to levels of NO in ambient air, 5 brands of cigarettes were smoked in 27 cubic meter controlled environment room. Ventilation conditions were either 2.5 or 5.0 air changes per hour (ACH) and each experiment was replicated 3 times for a total of 30 experiments. Ventilation rates of 0.3 and 1.5 ACH were also selected in a second series of experiments in which only one brand of cigarette was smoked. Least squares estimates for the effective ventilation rates were obtained in the usual manner after linearizing the decay portion of the NO time curve. In each of the experiments, the regression explained at least 95% of the variation in the levels of NO with time. Loss of NO due to factors other than ventilation appeared to be constant within experimental error and averaged 2.22 ACH. Equilibrium values for NO were grossly underestimated when results from currently accepted proecedures for smoke analysis were used in modeling the growth and decay of NO. Goodness-of-fit was improved when equilibrium values were estimated based on observed levels in ambient air. This approach may be more suitable for evaluating the potential contribution of cigarette smoke to levels of indoor air pollutants.     

Effect of water pH and total dissolved solids on the species diversity of pelagic zooplankton in lakes: A statistical analysis

Statistical analysis of the combined influence of lake surface area (S), water pH, and total dissolved solids (TDS) on the formation of zooplankton communities in lakes has been made on the basis of available data on the number of species (N _sp ) of pelagic zooplankton in 256 lakes of the temperate zone of Europe, Asia, and North America. Graphic analysis and analysis of variance have shown that extremely high or extremely low values of pH and TDS inhibit lake zooplankton. If the value of one of these factors is extremely high, any increase in the other factor is favorable for the inhibited zooplankton, and this second factor determines the value of N _sp .     

Transfer parameter values in temperate forest ecosystems: a review

Compared to agricultural lands, forests are complex ecosystems as they can involve diverse plant species associations, several vegetative strata (overstorey, shrubs, herbaceous and other annual plant layer) and multi-layered soil profiles (forest floor, hemi-organic and mineral layers). A high degree of variability is thus generally observed in radionuclide transfers and redistribution patterns in contaminated forests. In the long term, the soil compartment represents the major reservoir of radionuclides which can give rise to long-term plant and hence food contamination. For practical reasons, the contamination of various specific forest products has commonly been quantified using the aggregated transfer factor (T_ag in m² kg⁻¹) which integrates various environmental parameters including soil and plant type, root distribution as well as nature and vertical distribution of the deposits. Long lasting availability of some radionuclides was shown to be the source of much higher transfer in forest ecosystems than in agricultural lands. This study aimed at reviewing the most relevant quantitative information on radionuclide transfers to forest biota including trees, understorey vegetation, mushrooms, berries and game animals. For both radiocaesium and radiostrontium in trees, the order of magnitude of mean T_ag values was 10⁻³ m² kg⁻¹ (dry weight). Tree foliage was usually 2–12 times more contaminated than trunk wood. Maximum contamination of tree components with radiocaesium was associated with (semi-)hydromorphic areas with thick humus layers. The transfer of radionuclides to mushrooms and berries is high, in comparison with foodstuffs grown in agricultural systems. Concerning caesium uptake by mushrooms, the transfer is characterized by a very large variability of T_ag, from 10⁻³ to 10¹ m² kg⁻¹ (dry weight). For berries, typical values are around 0.01–0.1 m² kg⁻¹ (dry weight). Transfer of radioactive caesium to game animals and reindeer and the rate of activity reduction, quantified as an ecological half-life, reflect the soil and pasture conditions at individual locations. Forests in temperate and boreal regions differ with respect to soil type and vegetation, and a faster decline of muscle activity concentrations in deer occurs in the temperate zone. However, in wild boar the caesium activity concentration shows no decline because of its special feeding habits. In the late phase, i.e. at least a few months since the external radionuclide contamination on feed plants has been removed, a T_ag value of 0.01 m² kg⁻¹ (fresh weight) is common for ¹³⁷Cs in the muscles of adult moose and terrestrial birds living in boreal forests, and 0.03 m² kg⁻¹ (fresh weight) for arctic hare. Radiocaesium concentrations in reindeer muscle in winter may exceed the summer content by a factor of more than two, the mean T_ag values for winter ranging from 0.02 to 0.8 m² kg⁻¹ (fresh weight), and in summer from 0.04 to 0.4 m² kg⁻¹. The highest values are found in the year of initial contamination, followed by a gradual reduction. In waterfowl a relatively fast decline in uptake of ¹³⁷Cs has been found, with T_ag values changing from 0.01 to 0.002 m² kg⁻¹ (fresh weight) in the three years after the contaminating event, the rate being determined by the dynamics of ¹³⁷Cs in aquatic ecosystems.     

Using the Q10 model to simulate E. coli survival in cowpats on grazing lands

Microbiological quality of surface waters can be affected by microbial load in runoff from grazing lands. This effect, with other factors, depends on the survival of microorganisms in animal waste deposited on pastures. Since temperature is a leading environmental parameter affecting survival, it indirectly impacts water microbial quality. The Q₁₀ model is widely used to predict the effect of temperature on rates of biological processes, including survival. Objectives of this work were to (i) evaluate the applicability of the Q₁₀ model to Escherichia coli inactivation in bovine manure deposited on grazing land (i.e., cowpats) and (ii) identify explanatory variables for the previously reported E. coli survival dynamics in cowpats. Data utilized in this study include published results on E. coli concentrations in natural and repacked cowpats from research conducted the U.S. (Virginia and Maryland), New Zealand, and the United Kingdom. Inspection of the datasets led to conceptualizing E. coli survival (in cowpats) as a two-stage process, in which the initial stage was due to growth, inactivation or stationary state of the population and the second stage was the approximately first-order inactivation. Applying the Q₁₀ model to these datasets showed a remarkable similarity in inactivation rates, using the thermal time. The reference inactivation rate constant of 0.042 (thermal days)^− 1 at 20 °C gave a good approximation (R² = 0.88) of all inactivation stage data with Q₁₀ = 1.48. The reference inactivation rate constants in individual studies were no different from the one obtained by pooling all data (P < 0.05). The rate of logarithm of the E. coli concentration change during the first stage depended on temperature. Duration of the first stage, prior to the first-order inactivation stage and the initial concentration of E. coli in cowpats, could not be predicted from available data. Diet and age are probable factors affecting these two parameters however, until their environmental and management predictors are known, microbial water quality modeling must treat them as a stochastic source of uncertainty in simulation results.     

A survey of parabens in commercial pharmaceuticals from China and its implications for human exposure

Parabens are widely used as antimicrobial preservatives during pharmaceutical production. However, little information is available regarding the occurrence of parabens in commercial pharmaceuticals and their implications for human exposure. In this study, six commonly used parabens were analyzed by ultra-performance liquid chromatography-tandem mass spectrometry with 100 commercial pharmaceuticals collected from China. Almost all of the pharmaceutical samples contained at least one kind of parabens with the detection frequency of 97%. The concentrations of Σ₆parabens (sum of the six parabens) ranged from below MDL to 1256 ng/g, with mean and median values of 94.8 and 119 ng/g, respectively. Methyl paraben (MeP), ethyl paraben (EtP) and propyl paraben (PrP) were the predominant compounds. Significant positive correlation was observed between concentrations of MeP and PrP, indicating their co-applications in pharmaceuticals. Levels of Σ₆parabens varied in different categories of pharmaceuticals and increased with their shelf lives. Based on the measured concentrations and daily ingestion rates of pharmaceuticals, the estimated daily intake (EDI) of parabens was calculated. The median values of EDI_{pharmaceutical} for male adults, female adults and children were 4.05, 4.75 and 9.73 ng/kg-bw/day, respectively, which were three orders of magnitude lower than those from foodstuffs and personal care products (PCPs). It was firstly reported that the total exposure dose was 0.326 mg/kg-bw/day via foodstuffs, PCPs, and pharmaceuticals for Chinese female adults.     

Evaluation of in vitro vs. in vivo methods for assessment of dermal absorption of organic flame retardants: A review

There is a growing interest to study human dermal exposure to a large number of chemicals, whether in the indoor or outdoor environment. Such studies are essential to predict the systemic exposure to xenobiotic chemicals for risk assessment purposes and to comply with various regulatory guidelines. However, very little is currently known about human dermal exposure to persistent organic pollutants. While recent pharmacokinetic studies have highlighted the importance of dermal contact as a pathway of human exposure to brominated flame retardants, risk assessment studies had to apply assumed values for percutaneous penetration of various flame retardants (FRs) due to complete absence of specific experimental data on their human dermal bioavailability. Therefore, this article discusses the current state-of-knowledge on the significance of dermal contact as a pathway of human exposure to FRs. The available literature on in vivo and in vitro methods for assessment of dermal absorption of FRs in human and laboratory animals is critically reviewed. Finally, a novel approach for studying human dermal absorption of FRs using in vitro three-dimensional (3D) human skin equivalent models is presented and the challenges facing future dermal absorption studies on FRs are highlighted.     

Comparison of distribution coefficients for americium and curium: Effects of pH and naturally occurring colloids

Distribution coefficients (K_D) were measured by a batch technique for sorption of americium-243 and curium-244 to Lake Michigan sediment from four different natural surface waters. The dependences of K_D values on pH and on the concentrations of naturally occurring colloidal organic carbon (COC) were studied. The comparison of K_D values showed that, while changes in pH and in COC concentrations cause significant changes in sorption for both americium and curium, neither variable causes a significant difference in sorption between these two elements.     

Assessment of surface area normalisation for interpreting distribution coefficients (Kd) for uranium sorption

Adsorption of radionuclides on soils and sediments is commonly quantified by distribution coefficients (K_d values). This paper examines the relationship between K_d values for uranium(VI) adsorption and the specific surface area (SSA) of geologic materials. We then investigate the potential applicability of normalising uranium (U) K_d measurements using the SSA, to produce ‘K_a values’ as a generic expression of the affinity of U for the surface. The data for U provide a reasonably coherent set of K_a values on various solid phases, both with and without ligands. The K_a representation provides a way of harmonising datasets obtained for materials having different specific surface areas, and accounting for the effects of ligands in different systems. In addition, this representation may assist in developing U sorption models for complex materials. However, a significant limitation of the K_a concept is that sorption of radionuclides at trace levels can be dominated by interactions with specific surface sites, whose abundances are not reflected by the SSA. Therefore, calculated K_a values should be interpreted cautiously.     

Sorption of selenate on soils and pure phases: kinetic parameters and stabilisation

This study was conducted to identify the principle selenate carrier phases for two selected soils, by comparing their reactivity with selenate to that of pure phases of the solids. Silica, calcium carbonate, aluminium hydroxide, goethite, bentonite and humic acid were selected as the main soil carrier phases. Comparisons were made first on the parameter values obtained with the best fit of a kinetic sorption model which can discriminate instantaneous sorption from kinetically limited sorption. Then comparisons were made of the ability for each solid to stabilise selenate by measuring the ratio of the partition coefficient for sorption (Kd_sorption) over that of the desorption (Kd_desorption). Kinetics and stabilisation were used to help elucidate the nature of interactions with the test solid phases for a large range of selenate concentrations. The experiments were conducted over 165 h in batch reactors, the solid being isolated from the solution by dialysis tubing, at two pH (5.4 and 8) and three selenate concentrations (1 × 10⁻³, 1 × 10⁻⁶ and 1 × 10⁻⁸ mol L⁻¹). The results obtained showed that only aluminium hydroxide can sorb selenate throughout the studied pH range (pH 5.4 to 8.0). The sorption capacity on this mineral was high (Kd_sorption > 100 to 1 × 10⁴ L kg⁻¹) and the selenate was mainly stabilized by the formation of inner sphere complexes. The sorption on goethite occurred at pH 5.4 (Kd_sorption 52 L kg⁻¹), mainly as outer sphere complexes, and was null at pH 8. On silica, a weak sorption was observed only at pH 5.4 and at 165 h (Kd_sorption 4 L kg⁻¹). On bentonite, calcium carbonate and humic acid no significant sorption was observed. Concerning the two soils studied, different behaviours were observed for selenate. For soil Ro (pH 5.4), Kd_sorption was low (8 L kg⁻¹) compared to soil Bu (pH 8) (70 L kg⁻¹). The sorption behaviour of selenate on soil Ro was mainly due to outer sphere complexes, as for goethite, whereas for soil Bu the sorption was mainly attributed to inner sphere complexes followed by reduction mechanisms, probably initiated by microorganisms, in which no steady state was reached at the end of the 165 h experiments. The sorption of selenate decreased when concentrations reached 1 × 10⁻³ mol L⁻¹, due to solid saturation, except for aluminium hydroxide. Reduction of selenate seemed also to occur on goethite and soil Ro, for the same concentration, but without preventing a decrease in sorption. Thus, this work shows that the comparison of selenate behaviour between soil and pure phases helps to elucidate the main carrier phases and sorption mechanisms in soil.     

Experimental studies of the transfer of neptunium from sea water to sediments and organisms (annelids and molluscs)

This paper deals with the physico-chemical behaviour of neptunium in sea water and with its capacity for transfer to coastal or deep-sea sediments and for uptake by two benthic species, Arenicola marina (L.) and Cerastoderma edule (L.). We used the ²³⁹Np isotope with mass concentrations in sea water of about 2·5 × 10⁻¹⁰−5·4×10⁻¹² g litre⁻¹, which are close to the concentrations observed in the environment for ²³⁷Np. The experimental results show that Np occurs in solution mainly as the neptunyl ion NpO₂⁺, but soluble anionic and neutral complexes and particulate forms were also detected. The distribution coefficients for the sediments varied from 350 to 6500. The carbonate phase plays a decisive role in neptunium transfer but other fixation processes are also possible. Concentration factors after 13 days were found to have values of 40 and 14 for the shells and soft parts of cockles, respectively, while polychaetes had a concentration factor of 2. Thus Np has a smaller probability of transfer to sediments and organisms than have plutonium and americium.     

Bioaccumulation of PCDD/Fs,PCBs and PBDEs by earthworms in field soils of an E-waste dismantling area in China

A total of 60 paired samples of earthworm, corresponding soil and wormcast were collected to investigate the bioaccumulation tendency of polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) in earthworms from a typical E-waste dismantling area in east China. Significant correlations were observed for the total concentrations among different matrix types except for PCDD/Fs in soil and earthworm. The bioaccumulation tendency showed some differences among the contaminants. Calculated biota–soil accumulation factors (BSAFs) indicated that PCBs and PBDEs had higher bioaccumulation potential compared to PCDD/Fs, which was somewhat different from laboratory studies. The plot of mean BSAFs versus log K_ow values for PCBs and PBDEs was well fitted by a second-order polynomial with the maximum BSAF at approximately log K_ow of 6.5. While for PCDD/Fs, only a slightly decreasing trend was observed with increasing log K_ow. Composition analysis indicated that tetra-, penta- and hexa-halogenated homologs had higher bioaccumulation levels, indicating that medium-halogenated congeners with log K_ow around 6.5 are more easily accumulated by earthworms. Furthermore, the ratios of BDE-47/-99 and BDE-99/-100 showed some discrepancies with the technical products and other biotic species, suggesting different bioaccumulation potential of PBDEs in earthworm.     

Influence of fertilizing on the Cs soil–plant transfer in a spruce forest of Southern Germany

Fertilization with 2.5 t/ha limestone: (83% CaCO₃, 8% MgO, 6% K₂O, 3% P₂O₅) reduces the ¹³⁷Cs transfer from spruce forest soil into plants like fern (Dryopteris carthusiana) and blackberry (Rubus fruticosus) by a factor of 2–5 during at least 11 years as measured by the aggregated transfer factor T_ag. In 1997 and 2006 these results were confirmed by additional measurements of the ¹³⁷Cs transfer factor TF, related to the root zone (O_h horizon), which were explained by the selective sorption of ¹³⁷Cs in the root zone by measurements of the Radiocaesium Interception Potential (RIP) in fertilized (RIP > 179 meq/kg) and non-fertilized soils (RIP < 74 meq/kg).     

The Kinetics of Caesium absorption by roots of winter wheat and the possible consequences for the derivation of soil-to-plant transfer factors for radiocaesium

Caesium (Cs) uptake in roots of winter wheat was found to follow a dual pattern similar to that established for potassium uptake in barley roots. This suggests the operation of two discrete uptake systems for Cs, as for potassium. The ‘System 1’ (low concentration) uptake mechanism for caesium, however, can be resolved into two hyperbolic components which both obey Michaelis-Menten kinetics. The Michaelis-Menten equation was used to derive a function which describes the variation in solution-to-root transfer factor for any element for which the appropriate root uptake constants (K_m andV_max) can be determined. This function successfully described available data for root uptake of caesium and potassium, predicting that the solution-to-root transfer factor decreases in relation to an increase in the substrate concentration of each respective element. At substrate concentrations equivalent to carrier-free radiocaesium concentrations, however, the solution-to-root transfer factor predicted by the function and by empirical data suggests that the relationship between root uptake and solution concentration of caesium is linear. These findings are discussed in relation to the comparative physiology of caesium and potassium uptake by plant roots and with respect to the application of the soil-to-plant transfer factor concept to radioecological studies.     

Distributions of radionuclide sorption coefficients (Kd) in sub-surface sediments and the implications for transport calculations

The effect of the spatial variability of K_d on calculations of contaminant travel time in the vadose zone was determined. Depth discrete measurements of K_d were made for a suite of radionuclides (¹⁰⁹Cd, ⁵⁷Co, ⁶⁰Co, ⁸⁵Sr, ¹³⁷Cs, and ⁸⁸Y) utilizing a sediment core from the E-Area at the Savannah River Site. The K_d’s were ordered as ⁸⁵Sr²⁺ < ¹³⁷Cs⁺ < ¹⁰⁹Cd²⁺ < ⁵⁷Co²⁺ = ⁶⁰Co²⁺ << ⁸⁸Y³⁺ and the values generally fell below or near the lowest quartile of values reported in the literature. Correlations were generally weak between soil properties and K_d values. Most importantly, all of the K_d distributions could be reasonably approximated as log-normal. Deterministic and stochastic calculations of contaminant travel time to the water table were made. The deterministic calculations were based on each of three conceptual models of the vadose zone: complete stratification (17 strata, each with a different K_d), two strata (two sections of the vadose zone, each characterized by a single, average K_d), and unstratified (a single zone with an average K_d). Stochastic calculations were based on log-normal fits to the K_d data. The two strata model generally yielded travel times 2× greater than those in the completely stratified model. The unstratified model yielded travel times that were between 3 and 5 times greater than the completely stratified model. The stochastic mean travel times were comparable to those of the two strata model.