Solute transport in crystalline rocks at Äspö — I: Geological basis and model calibration

Water-conducting faults and fractures were studied in the granite-hosted Äspö Hard Rock Laboratory (SE Sweden). On a scale of decametres and larger, steeply dipping faults dominate and contain a variety of different fault rocks (mylonites, cataclasites, fault gouges). On a smaller scale, somewhat less regular fracture patterns were found. Conceptual models of the fault and fracture geometries and of the properties of rock types adjacent to fractures were derived and used as input for the modelling of in situ dipole tracer tests that were conducted in the framework of the Tracer Retention Understanding Experiment (TRUE-1) on a scale of metres. After the identification of all relevant transport and retardation processes, blind predictions of the breakthroughs of conservative to moderately sorbing tracers were calculated and then compared with the experimental data. This paper provides the geological basis and model calibration, while the predictive and inverse modelling work is the topic of the companion paper [J. Contam. Hydrol. 61 (2003) 175].The TRUE-1 experimental volume is highly fractured and contains the same types of fault rocks and alterations as on the decametric scale. The experimental flow field was modelled on the basis of a 2D-streamtube formalism with an underlying homogeneous and isotropic transmissivity field. Tracer transport was modelled using the dual porosity medium approach, which is linked to the flow model by the flow porosity. Given the substantial pumping rates in the extraction borehole, the transport domain has a maximum width of a few centimetres only. It is concluded that both the uncertainty with regard to the length of individual fractures and the detailed geometry of the network along the flowpath between injection and extraction boreholes are not critical because flow is largely one-dimensional, whether through a single fracture or a network. Process identification and model calibration were based on a single uranine breakthrough (test PDT3), which clearly showed that matrix diffusion had to be included in the model even over the short experimental time scales, evidenced by a characteristic shape of the trailing edge of the breakthrough curve. Using the geological information and therefore considering limited matrix diffusion into a thin fault gouge horizon resulted in a good fit to the experiment. On the other hand, fresh granite was found not to interact noticeably with the tracers over the time scales of the experiments.While fracture-filling gouge materials are very efficient in retarding tracers over short periods of time (hours–days), their volume is very small and, with time progressing, retardation will be dominated by altered wall rock and, finally, by fresh granite. In such rocks, both porosity (and therefore the effective diffusion coefficient) and sorption K_ds are more than one order of magnitude smaller compared to fault gouge, thus indicating that long-term retardation is expected to occur but to be less pronounced.     

Numerical analysis of water and solute transport in variably-saturated fractured clayey till

This study numerically investigates the influence of initial water content and rain intensities on the preferential migration of two fluorescent tracers, Acid Yellow 7 (AY7) and Sulforhodamine B (SB), through variably-saturated fractured clayey till. The simulations are based on the numerical model HydroGeoSphere, which solves 3D variably-saturated flow and solute transport in discretely-fractured porous media. Using detailed knowledge of the matrix, fracture, and biopore properties, the numerical model is calibrated and validated against experimental high-resolution tracer images/data collected under dry and wet soil conditions and for three different rain events. The model could reproduce reasonably well the observed preferential migration of AY7 and SB through the fractured till, although it did not capture the exact depth of migration and the negligible impact of the dead-end biopores in a near-saturated matrix. A sensitivity analysis suggests fast flow mechanisms and dynamic surface coating in the biopores, and the presence of a plough pan in the till.     

Tracer transport model at Japan meteorological agency and its application to the ETEX data

This paper describes the JMA tracer transport model and its sensitivity to model physics and initial conditions by using the ETEX data. Compared with observations, the model overestimates ground-level concentration in the early stage within about one day from the emission, possibly due to underestimation of vertical diffusion. In the early stage, the enhanced vertical diffusion effectively transports the tracer upward and decreases the ground-level concentration, while in the later stage, it enhances downward transports from the upper layer and increases the ground-level concentration. A conceptual model is given for understanding the vertical transport due to vertical diffusion. The horizontal diffusion introduced to the model has preferable impacts on forecasts especially in the early stage. Finally, we discuss the predictability of this model based on sensitivity to initial conditions of emission time and height.     

Mesoscale influence on long-range transport — evidence from ETEX modelling and observations

During the first European Tracer Experiment (ETEX) tracer gas was released from a site in Brittany, France, and subsequently observed over a range of 2000 km. Hourly measurements were taken at the National Environmental Research Institute (NERI) located at Risø, Denmark, using two measurement techniques. At this location, the observed concentration time series shows a double-peak structure occurring between two and three days after the release. By using the Danish Emergency Response Model of the Atmosphere (DERMA), which is developed at the Danish Meteorological Institute (DMI), simulations of the dispersion of the tracer gas have been performed. Using numerical weather-prediction data from the European Centre for Medium-Range Weather Forecast (ECMWF) by DERMA, the arrival time of the tracer is quite well predicted, so also is the duration of the passage of the plume, but the double-peak structure is not reproduced. However, using higher-resolution data from the DMI version of the HIgh Resolution Limited Area Model (DMI-HIRLAM), DERMA reproduces the observed structure very well. The double-peak structure is caused by the influence of a mesoscale anti-cyclonic eddy on the tracer gas plume about one day earlier.     

Incorporating layer- and local-scale heterogeneities in numerical simulation of unsaturated flow and tracer transport

This study characterizes layer- and local-scale heterogeneities in hydraulic parameters (i.e., matrix permeability and porosity) and investigates the relative effect of layer- and local-scale heterogeneities on the uncertainty assessment of unsaturated flow and tracer transport in the unsaturated zone of Yucca Mountain, USA. The layer-scale heterogeneity is specific to hydrogeologic layers with layerwise properties, while the local-scale heterogeneity refers to the spatial variation of hydraulic properties within a layer. A Monte Carlo method is used to estimate mean, variance, and 5th, and 95th percentiles for the quantities of interest (e.g., matrix saturation and normalized cumulative mass arrival). Model simulations of unsaturated flow are evaluated by comparing the simulated and observed matrix saturations. Local-scale heterogeneity is examined by comparing the results of this study with those of the previous study that only considers layer-scale heterogeneity. We find that local-scale heterogeneity significantly increases predictive uncertainty in the percolation fluxes and tracer plumes, whereas the mean predictions are only slightly affected by the local-scale heterogeneity. The mean travel time of the conservative and reactive tracers to the water table in the early stage increases significantly due to the local-scale heterogeneity, while the influence of local-scale heterogeneity on travel time gradually decreases over time. Layer-scale heterogeneity is more important than local-scale heterogeneity for simulating overall tracer travel time, suggesting that it would be more cost-effective to reduce the layer-scale parameter uncertainty in order to reduce predictive uncertainty in tracer transport.     

Analytical model of solute transport by unsteady unsaturated gravitational infiltration

Penetration of reactive solute into a soil during a cycle of water infiltration and redistribution is investigated by deriving analytical closed form solutions for fluid flux, moisture content and contaminant concentration. The solution is developed for gravitational flow and advective transport and is applied to two scenarios of solute applications encountered in the applications: a finite pulse of solute dissolved in irrigation water and an instantaneous pulse broadcasted onto the soil surface. Through comparison to simulations of Richards' flow, capillary suction is shown to have contrasting effects on the upper and lower boundaries of the fluid pulse, speeding penetration of the wetting front and reducing the rate of drying. This leads to agreement between the analytical and numerical solutions for typical field and experimental conditions. The analytical solution is further incorporated into a stochastic column model of flow and transport to compute mean solute concentration in a heterogeneous field. An unusual phenomenon of plume contraction is observed at long times of solute propagation during the drying stage. The mean concentration profiles match those of the Monte-Carlo simulations for capillary length scales typical of sandy soils.     

Impact of varying soil structure on transport processes in different diagnostic horizons of three soil types

When soil structure varies in different soil types and the horizons of these soil types, it has a significant impact on water flow and contaminant transport in soils. This paper focuses on the effect of soil structure variations on the transport of pesticides in the soil above the water table. Transport of a pesticide (chlorotoluron) initially applied on soil columns taken from various horizons of three different soil types (Haplic Luvisol, Greyic Phaeozem and Haplic Cambisol) was studied using two scenarios of ponding infiltration. The highest infiltration rate and pesticide mobility were observed for the Bt₁ horizon of Haplic Luvisol that exhibited a well-developed prismatic structure. The lowest infiltration rate was measured for the Bw horizon of Haplic Cambisol, which had a poorly developed soil structure and a low fraction of large capillary pores and gravitational pores. Water infiltration rates were reduced during the experiments by a soil structure breakdown, swelling of clay and/or air entrapped in soil samples. The largest soil structure breakdown and infiltration decrease was observed for the Ap horizon of Haplic Luvisol due to the low aggregate stability of the initially well-aggregated soil. Single-porosity and dual-permeability (with matrix and macropore domains) flow models in HYDRUS-1D were used to estimate soil hydraulic parameters via numerical inversion using data from the first infiltration experiment. A fraction of the macropore domain in the dual-permeability model was estimated using the micro-morphological images. Final soil hydraulic parameters determined using the single-porosity and dual-permeability models were subsequently used to optimize solute transport parameters. To improve numerical inversion results, the two-site sorption model was also applied. Although structural changes observed during the experiment affected water flow and solute transport, the dual-permeability model together with the two-site sorption model proved to be able to approximate experimental data.     

有机磷通过弱透水层的迁移转化规律研究

在地下水超量开采区,上层劣质潜水可以越过弱透水层补给承压水.有机磷能否随水迁移进入深层地下水构成水质污染是极为关注的问题.采用施压条件下将一定浓度的有机磷溶液渗透通过粘性土柱的模拟实验,对有机磷在饱和粘性土层中降解转化的各种因子及其影响机制进行分析,探讨有机磷在弱透水层环境中的降解转化和迁移的规律.结果表明:(1)粘性...     

Effects of biofilm growth on flow and transport through a glass parallel plate fracture

The effects of biofilm growth on flow and solute transport through a sandblasted glass parallel plate fracture was investigated. The fracture was inoculated using soil microorganisms. Glucose, oxygen and other nutrients were supplied to support growth. The biomass initially formed discrete clusters attached to the glass surfaces, but over time formed a continuous biofilm. From dye tracer tests conducted during biofilm growth, it was observed that channels and low-permeability zones dominated transport. The hydraulic conductivity of the fracture showed a sigmoidal decrease with time. The hydraulic conductivity was reduced by a factor of 0.033, from 18 to 0.6 cm/s, corresponding to a 72% decrease in the hydraulic aperture, from 500 to 140 microm. In contrast, the mass balance aperture, determined from fluoride tracer tests, remained relatively constant, indicating that the impact of biomass growth on effective fracture porosity was much less than the effect on hydraulic conductivity. Analyses of pre-biofilm tracer tests revealed that both Taylor dispersion and macrodispersion were influencing transport. During biofilm growth, only macrodispersion was dominant. The macrodispersion coefficient alpha(macro) was found to increase logarithmically with hydraulic conductivity reduction.     

Characterization of flow and transport processes within the unsaturated zone of Yucca Mountain, Nevada, under current and future climates

This paper presents a large-scale modeling study characterizing fluid flow and tracer transport in the unsaturated zone of Yucca Mountain, Nevada, a potential repository site for storing high-level radioactive waste. The study has been conducted using a three-dimensional numerical model, which incorporates a wide variety of field data and takes into account the coupled processes of flow and transport in the highly heterogeneous, unsaturated fractured porous rock. The modeling approach is based on a dual-continuum formulation of coupled multiphase fluid and tracer transport through fractured porous rock. Various scenarios of current and future climate conditions and their effects on the unsaturated zone are evaluated to aid in the assessment of the proposed repository's system performance using different conceptual models. These models are calibrated against field-measured data. Model-predicted flow and transport processes under current and future climates are discussed.     

The effect of export to the deep sea on the long-range transport potential of persistent organic pollutants

BACKGROUND: Export to the deep sea has been found to be a relevant pathway for highly hydrophobic chemicals. The objective of this study is to investigate the influence of this process on the potential for long-range transport (LRT) of such chemicals. METHODS: The spatial range as a measure of potential for LRT is calculated for seven PCB congeners with the multimedia fate and transport model ChemRange. Spatial ranges for cases with and without deep sea export are compared. RESULTS AND DISCUSSION: Export to the deep sea leads to increased transfer from the air to the surface ocean and, thereby, to lower spatial ranges for PCB congeners whose net deposition rate constant is similar to or greater than the atmospheric degradation rate constant. This is fulfilled for the PCB congeners 101, 153, 180, and 194. The spatial ranges of the congeners 8, 28, and 52, in contrast, are not affected by deep sea export. With export to the deep sea included in the model, the spatial ranges of the heavier congener are similar to those of the lighter ones, while the intermediate congeners 101 and 153 have the highest potential for long-range transport. CONCLUSIONS: Transfer to the deep ocean affects the mass balance and the potential for LRT of highly hydrophobic chemicals and should be included in multimedia fate models containing a compartment for ocean water.     

Influence of indoor transport and mixing time scales on the performance of sensor systems for characterizing contaminant releases

Optimizing real-time sensor systems to detect and identify relevant characteristics of an indoor contaminant event is a challenging task. The interpretation of incoming sensor data is confounded by uncertainties in building operation, in the forces driving contaminant transport, and in the physical parameters governing transport. In addition, simulation tools used by the sensor interpretation algorithm introduce modeling uncertainties. This paper explores how the time scales inherent in contaminant transport influence the information that can be extracted from real-time sensor data. In particular, we identify three time scales (within room mixing, room-to-room transport, and removal from the building) and study how they affect the ability of a Bayesian Monte Carlo (BMC) sensor interpretation algorithm to identify the release location and release mass from a set of experimental data, recorded in a multi-floor building. The research shows that some limitations in the BMC approach do not depend on details of the models or the algorithmic implementation, but rather on the physics of contaminant transport. These inherent constraints have implications for the design of sensor systems.     

垂直流人工湿地中基质组合对污水的处理效果及模型模拟

选择石砾、粗砂、细砂作为垂直流人工湿地的基质在实验室内研究不同粒径的基质在不同的水力负荷和对不同浓度污水对污染物的去除效果,根据实验结果选取基质应用于示范基地,利用人工湿地模型Subwet2.0对人工湿地示范基地进行模型模拟,为农村生活污水人工湿地系统的处理设计及模拟出水水质提供参考。研究结果表明:石砾、粗砂、细砂为基质对污染物去除率较好的水力负荷分别为小于0.9、0.6和0.3 m/d时;石砾基质对COD的最佳污染负荷为970 mg/L,粗砂、细砂基质为468~970 mg/L;粗砂和细砂基质对NH4+-N去除效果相似;在北方地区垂直流人工湿地主体基质建议使用粗砂或石砾以减少堵塞的风险;利用Subwet2.0模型模拟人工湿地示范基地的出水水质,根据当地条件在反应参数的取值范围内调整了相应的参数值,模拟的结果符合性很高。     

Effects of degree of water saturation on dispersivity and immobile water in sandy soil columns

Three natural nonaggregated soil samples, with similar grain-size distributions, have been used to determine the dispersive behavior of porous media under steady, saturated and unsaturated flow conditions. Tritium was used as a tracer and was found to have no sorption on the solid matrix. Generated breakthrough curves (BTCs) for the unsaturated experiments were symmetrical with no evidence of tailing. The unsaturated experiments for two of the soils were adequately described by considering all the water in the pore volume as mobile. However, about 10% of the pore water, independent of the degree of saturation, was found to be immobile in the case of the third soil during unsaturated flow. For this soil, there was no mass transfer between the two water regions, indicating that the immobile water is essentially isolated from the flowing water fraction. For all three soils, dispersivity under unsaturated conditions was found to be higher, independent of the degree of water saturation, than the value determined for the saturated experiments. This is inconsistent with what would be expected from the simple bundle-of-capillary-tubes model and does not agree well with a more sophisticated conceptualization of the porous medium. The data, however, clearly indicate a wider range in pore-water velocities when these soils are desaturated.     

Influence of variable chemical conditions on EDTA-enhanced transport of metal ions in mildly acidic groundwater

Adsorption of Ni and Pb on aquifer sediments from Cape Cod, Massachusetts, USA increased with increasing pH and metal-ion concentration. Adsorption could be described quantitatively using a semi-mechanistic surface complexation model (SCM), in which adsorption is described using chemical reactions between metal ions and adsorption sites. Equilibrium reactive transport simulations incorporating the SCMs, formation of metal-ion-EDTA complexes, and either Fe(III)-oxyhydroxide solubility or Zn desorption from sediments identified important factors responsible for trends observed during transport experiments conducted with EDTA complexes of Ni, Zn, and Pb in the Cape Cod aquifer. Dissociation of Pb-EDTA by Fe(III) is more favorable than Ni-EDTA because of differences in Ni- and Pb-adsorption to the sediments. Dissociation of Ni-EDTA becomes more favorable with decreasing Ni-EDTA concentration and decreasing pH. In contrast to Ni, Pb-EDTA can be dissociated by Zn desorbed from the aquifer sediments. Variability in adsorbed Zn concentrations has a large impact on Pb-EDTA dissociation.     

Effects of heavy metals on the nitrogen metabolism of the aquatic moss Fontinalis antipyretica L. ex Hedw. A 15N tracer study

The assessment of pollution in aquatic systems necessitates an accurate indication of toxicity of heavy metals for organisms and ecosystems. We used the stable nitrogen isotope 15N to estimate the influence of the heavy metals Cd, Pb and Zn on the synthesis of nitrogen-containing fractions in the aquatic moss Fontinalis antipyretica. This method permits conclusions concerning inhibitory effects of these heavy metals on the assimilation of nitrogen and the biosynthesis of amino acids and proteins. The moss was exposed to metal concentrations of 25-500 microM over a period of 5-10 days. 15N abundance of exposed plants was compared with that of control plants. Similar to a loss of vitality determined using a fluorometric assay, a decrease of the 15N abundance in the N fractions of Fontinalis antipyretica was measured in dependence on the metal concentration. Nevertheless, the individual inhibition by the distinct metals was different, so that the following order of toxicity was derived: Cd > Pb > Zn.     

环境因子对雁鸣湖沉积物氮磷释放的影响

为探明环境因子对雁鸣湖沉积物-上覆水界面间氮磷释放的影响,通过单因子实验和响应面实验分析探究了温度、溶解氧及pH对氮磷释放通量的影响。单因子实验结果表明：雁鸣湖沉积物-上覆水界面间氮磷通量随着温度的升高而增加;随溶解氧浓度的升高而减小;当pH为中性时,氮磷通量最小,氮通量在pH=5时达到最大值,磷通量在pH=9时达到最大值。BBD模型拟合结果显示,各环境因子与氮磷通量间拟合关系均为二次多项式。响应面实验结果表明：温度和pH交互作用对TN通量影响显著;温度和溶解氧交互作用对TP通量影响显著;温度和溶解氧交互作用、温度和pH交互作用对${{\rm{NH}}_4^{+}}$-N通量影响均为显著;温度和溶解氧交互作用对${{\rm{PO}}_4^{3 - }}$-P通量影响极显著;雁鸣湖底泥释放的最不利条件为T=10 ℃、DO=7.87 mg·L⁻¹、pH=7.13,此时的TN交换通量为3.956 mg·(m²·h)⁻¹,TP交换通量为0.471 mg·(m²·h)⁻¹,${{\rm{NH}}_4^{+}}$-N交换通量为1.469 mg·(m²·h)⁻¹,${{\rm{PO}}_4^{3 - }}$-P交换通量为0.146 mg·(m²·h)⁻¹。以上研究结果可为雁鸣湖富营养化防治提供参考。     

Effects of Strength and Position of Pollutant Source on Pollutant Dispersion Within an Urban Street Canyon

A two-dimensional numerical model for simulating airflow and pollutant dispersion inside an urban street canyon was first developed using the FLUENT code, and then it was validated against a wind tunnel experiment. Then the effects of strength and position of pollutant sources on pollutant dispersion within an urban street canyon were investigated numerically. The numerical results showed that the dimensionless pollutant concentrations within the urban street canyon were independent from the source strength. The results also revealed that the pollutant distributions inside the urban street canyon with a two-lane road were influenced significantly by the positions of the two sources: 1) the closer the two sources were to the street center of the canyon, the lower the pollutant concentrations on the leeward wall and at the human respiration level in the leeward footpath became; 2) the pollutant concentrations on the windward wall and at the human respiration level in the windward footpath were not sensitive to the locations of the two sources as long as the source on the windward lane was situated outside the small recirculation zone at the bottom corner of the canyon windward wall; 3) the pollutant concentrations on the lower parts of the windward and leeward walls as well as in the two footpaths increased greatly when the two sources were moved from outside into the small recirculation zones.     

Elevated CO2 response of photosynthesis depends on ozone concentration in aspen

The effect of elevated CO₂ and O₃ on apparent quantum yield (?), maximum photosynthesis (P_max), carboxylation efficiency (V_cmax) and electron transport capacity (J_max) at different canopy locations was studied in two aspen (Populus tremuloides) clones of contrasting O₃ tolerance. Local light climate at every leaf was characterized as fraction of above-canopy photosynthetic photon flux density (%PPFD). Elevated CO₂ alone did not affect ? or P_max, and increased J_max in the O₃-sensitive, but not in the O₃-tolerant clone. Elevated O₃ decreased leaf chlorophyll content and all photosynthetic parameters, particularly in the lower canopy, and the negative impact of O₃ increased through time. Significant interaction effect, whereby the negative impact of elevated O₃ was exaggerated by elevated CO₂ was seen in Chl, N and J_max, and occurred in both O₃-tolerant and O₃-sensitive clones. The clonal differences in the level of CO₂ × O₃ interaction suggest a relationship between photosynthetic acclimation and background O₃ concentration.