Transport of Escherichia coli in 25 m quartz sand columns

To help improve the prediction of bacteria travel distances in aquifers laboratory experiments were conducted to measure the distant dependent sticking efficiencies of two low attaching Escherichia coli strains (UCFL-94 and UCFL-131). The experimental set up consisted of a 25 m long helical column with a diameter of 3.2 cm packed with 99.1% pure-quartz sand saturated with a solution of magnesium sulfate and calcium chloride. Bacteria mass breakthrough at sampling distances ranging from 6 to 25.65 m were observed to quantify bacteria attachment over total transport distances (α(L)) and sticking efficiencies at large intra-column segments (α(i)) (>5m). Fractions of cells retained (F(i)) in a column segment as a function of α(i) were fitted with a power-law distribution from which the minimum sticking efficiency defined as the sticking efficiency of 0.001% bacteria fraction of the total input mass retained that results in a 5 log removal were extrapolated. Low values of α(L) in the order 10(-4) and 10(-3) were obtained for UCFL-94 and UCFL-131 respectively, while α(i)-values ranged between 10(-6) to 10(-3) for UCFL-94 and 10(-5) to 10(-4) for UCFL-131. In addition, both α(L) and α(i) reduced with increasing transport distance, and high coefficients of determination (0.99) were obtained for power-law distributions ofα(i) for the two strains. Minimum sticking efficiencies extrapolated were 10(-7) and 10(-8) for UCFL-94 and UCFL-131, respectively. Fractions of cells exiting the column were 0.19 and 0.87 for UCFL-94 and UCL-131, respectively. We concluded that environmentally realistic sticking efficiency values in the order of 10(-4) and 10(-3) and much lower sticking efficiencies in the order 10(-5) are measurable in the laboratory, Also power-law distributions in sticking efficiencies commonly observed for limited intra-column distances (<2m) are applicable at large transport distances(>6m) in columns packed with quartz grains. High fractions of bacteria populations may possess the so-called minimum sticking efficiency, thus expressing their ability to be transported over distances longer than what might be predicted using measured sticking efficiencies from experiments with both short (<1m) and long columns (>25 m). Also variable values of sticking efficiencies within and among the strains show heterogeneities possibly due to variations in cell surface characteristics of the strains. The low sticking efficiency values measured express the importance of the long columns used in the experiments and the lower values of extrapolated minimum sticking efficiencies makes the method a valuable tool in delineating protection areas in real-world scenarios.     

Two-site kinetic modeling of bacteriophages transport through columns of saturated dune sand

Breakthrough curves, on a semi-log scale, from tests in porous media with block-input of viruses, bacteria, protozoa and colloidal particles often exhibit a typical skewness: a rather slowly rising limb and a smooth transition of a declining limb to a very long tail. One-site kinetic models fail to fit the rising and declining limbs together with the tail satisfactorily. Inclusion of an equilibrium adsorption site does not seem to improve simulation results. This was encountered in the simulation of breakthrough curves from a recent field study on the removal of bacteriophages MS2 and PRD1 by passage through dune sand. In the present study, results of laboratory experiments for the study of this issue are presented. Breakthrough curves of salt and bacteriophages MS2, PRDI, and phiX174 in 1 D column experiments have been measured. One- and two-site kinetic models have been applied to fit and predict breakthrough curves from column experiments. The two-site model fitted all breakthrough curves very satisfactorily, accounting for the skewness of the rising limb as well as for the smooth transition of the declining limb to the tail of the breakthrough curve. The one-site model does not follow the curvature of the breakthrough tail, leading to an overestimation of the inactivation rate coefficient for attached viruses. Interaction with kinetic site 1 is characterized by relatively fast attachment and slow detachment, whereas attachment to and detachment from kinetic site 2 is fast. Inactivation of viruses and interaction with kinetic site 2 provide only a minor contribution to removal. Virus removal is mainly determined by the attachment to site 1. Bacteriophage phiX174 attached more than MS2 and PRD1, which can be explained by the greater electrostatic repulsion that MS2 and PRD1 experience compared to the less negatively charged phiX174.     

Effects of water content on reactive transport of 85Sr in Chernobyl sand columns

It is known that under unsaturated conditions, the transport of solutes can deviate from ideal advective-dispersive behaviour even for macroscopically homogeneous porous materials. Causes may include physical non-equilibrium, sorption kinetics, non-linear sorption, and the irregular distribution of sorption sites. We have performed laboratory experiments designed to identify the processes responsible for the non-ideality of radioactive Sr transport observed under unsaturated flow conditions in an Aeolian sandy deposit from the Chernobyl exclusion zone. Miscible displacement experiments were carried out at various water contents and corresponding flow rates in a laboratory model system. Results of our experiments have shown that breakthrough curves of a conservative tracer exhibit a higher degree of asymmetry when the water content decreases than at saturated water content and same Darcy velocity. It is possible that velocity variations caused by heterogeneities at the macroscopic scale are responsible for this situation. Another explanation is that molecular diffusion drives the solute mass transfer between mobile and immobile water regions, but the surface of contact between these water regions is small. At very low concentrations, representative of a radioactive Sr contamination of the pore water, sorption and physical disequilibrium dominate the radioactive Sr transport under unsaturated flow conditions. A sorption reaction is described by a cation exchange mechanism calibrated under fully saturated conditions. The sorption capacity, as well as the exchange coefficients are not affected by desaturation. The number of accessible exchange sites was calculated on the basis that the solid remained in contact with water and that the fraction of solid phase in contact with mobile water is numerically equal to the proportion of mobile water to total water content. That means that for this type of sandy soil, the nature of mineral phases is the same in advective and non-advective domains. So sorption reaction parameters can be estimated from more easily conducted saturated experiments, but hydrodynamic behaviour must be characterized by conservative tracer experiments under unsaturated flow conditions.     

Transport of Escherichia coli through variably saturated sand columns and modeling approaches

A sand column leaching system with well-controlled suction and flow rate was built to investigate the effects on bacterial transport of air-water interface effects (AWI) correlated to water content, particle size, and column length. Adsorption of Escherichia coli strain D to silica sands was measured in batch tests. The average % adsorption for coarse and fine sands was 45.9+/-7.8% and 96.9+/-3.2%, respectively. However, results from static batch adsorption experiments have limited applicability to dynamic bacterial transport in columns. The early breakthrough of E. coli relative to bromide was clear for all columns, namely c. 0.15 to 0.3 pore volume earlier. Column length had no significant effects on the E. coli peak concentration or on total recovery in leachate, indicating retention in the top layer of sands. Tailing of breakthrough curves was more prominent for all fine sand columns than their coarse sand counterparts. Bacterial recovery in leachate from coarse and saturated sand columns was significantly higher than from fine and unsaturated columns. Observed data were fitted by the convection-dispersion model, amended for one-site and two-site adsorption to particles, and for air-water interface (AWI) adsorption. Among all models, the two-site+AWI model achieved consistently high model efficiency for all experiments. Thus it is evident from experimental and modeling results that AWI adsorption plays an important role in E. coli transport in sand columns.     

Application of an empirical transport model to simulate retention of nanocrystalline titanium dioxide in sand columns

Nanocrystalline titanium dioxide was injected into sand columns to simulate subsurface injection for creation of a permeable treatment barrier. Past usage of this material as an ex situ pilot scale treatment filter has shown that it has a high adsorption capacity for a number of heavy metals and therefore would be a good candidate for injection technology. Three suspension concentrations (50, 75 and 100 mg l(-1)) were pumped through packed sand columns at different flow velocities (3.0, 6.8 and 14.1 cm min(-1)). Little to no particles was detected in the effluent. Most of the nanoparticles remained in the sand columns, with an increasing then decreasing retained solids pattern. Application of a one-dimensional advection-dispersion flow model, that included two empirical kinetic terms to account for particle retention in the porous media, produced data fits that followed the general trend of the data, but did not truly capture the concentration maxima in the data sets. Discussion of these results highlights the limited ability of existing models to aid in predicting particle retention of non-ideal materials for engineering purposes.     

U-series disequilibria in a groundwater flow route as an indicator of uranium migration processes

U-series data relating to groundwater, fracture coatings and the adjoining rock matrix in a groundwater flow system at the Palmottu natural analogue site was examined. The aim was to obtain an experimental reference for migration modelling in a transport section defined within the flow system. The U-series reference obtained turned out to be a very useful tool for fine tuning the flow route and for migration mechanism considerations. The U-series data are well in line with other interpretations of the migration system.     

Transport and transformation of sulfadiazine in soil columns packed with a silty loam and a loamy sand

Concerning the transport of the veterinary antibiotic sulfadiazine (SDZ) little is known about its possible degradation during transport. Also its sorption behaviour is not yet completely understood. We investigated the transport of SDZ in soil columns with a special emphasis on the detection of transformation products in the outflow of the soil columns and on modelling of the concentration distribution in the soil columns afterwards. We used disturbed soil columns near saturation, packed with a loamy sand and a silty loam. SDZ was applied as a 0.57 mg L(-1) solution at a constant flow rate of 0.25 cm h(-1) for 68 h. Breakthrough curves (BTC) of SDZ and its transformation products 4-(2-iminopyrimidin-1(2H)-yl)aniline and 4-hydroxy-SDZ were measured for both soils. For the silty loam we additionally measured a BTC for an unknown transformation product which we only detected in the outflow samples of this soil. After the leaching experiments the (14)C-concentration was quantified in different layers of the soil columns. The transformation rates were low with mean SDZ mass fractions in the outflow samples of 95% for the loamy sand compared to 97% for the silty loam. The formation of 4-(2-iminopyrimidin-1(2H)-yl)aniline appears to be light dependent and did probably not occur in the soils, but afterwards. In the soil columns most of the (14)C was found near the soil surface. The BTCs in both soils were described well by a model with one reversible (kinetic) and one irreversible sorption site. Sorption kinetics played a more prominent role than sorption capacity. The prediction of the (14)C -concentration profiles was improved by applying two empirical models other than first order to predict irreversible sorption, but also these models were not able to describe the (14)C concentration profiles correctly. Irreversible sorption of sulfadiazine still is not well understood.     

Cesium migration in saturated silica sand and Hanford sediments as impacted by ionic strength

Large amounts of 137Cs have been accidentally released to the subsurface from the Hanford nuclear site in the state of Washington, USA. The cesium-containing liquids varied in ionic strengths, and often had high electrolyte contents, mainly in the form of NaNO3 and NaOH, reaching concentrations up to several moles per liter. In this study, we investigated the effect of ionic strengths on Cs migration through two types of porous media: silica sand and Hanford sediments. Cesium sorption and transport was studied in 1, 10, 100, and 1000 mM NaCl electrolyte solutions at pH 10. Sorption isotherms were constructed from batch equilibrium experiments and the batch-derived sorption parameters were compared with column breakthrough curves. Column transport experiments were analyzed with a two-site equilibrium-nonequilibrium model. Cesium sorption to the silica sand in batch experiments showed a linear sorption isotherm for all ionic strengths, which matched well with the results from the column experiments at 100 and 1000 mM ionic strength; however, the column experiments at 1 and 10 mM ionic strength indicated a nonlinear sorption behavior of Cs to the silica sand. Transport through silica sand occurred under one-site sorption and equilibrium conditions. Cesium sorption to Hanford sediments in both batch and column experiments was best described with a nonlinear Freundlich isotherm. The column experiments indicated that Cs transport in Hanford sediments occurred under two-site equilibrium and nonequilibrium sorption. The effect of ionic strength on Cs transport was much more pronounced in Hanford sediments than in silica sands. Effective retardation factors of Cs during transport through Hanford sediments were reduced by a factor of 10 when the ionic strength increased from 100 to 1000 mM; for silica sand, the effective retardation was reduced by a factor of 10 when ionic strength increased from 1 to 1000 mM. A two order of magnitude change in ionic strength was needed in the silica sand to observe the same change in Cs retardation as in Hanford sediments.     

Virus retention and transport through Al-oxide coated sand columns: effects of ionic strength and composition

Knowledge of the factors that influence the fate and transport of viruses in porous media is very important for accurately determining groundwater vulnerability and for developing protective regulations. In this study, six saturated sand column experiments were performed to examine the effects of a positively charged Al-oxide, which was coated on sand particles, on the retention and transport of viruses (phiX174 and MS-2) in background solutions of different ionic strength and composition. We found that the Al-oxide coating on sand significantly removed viruses during their transport in a phosphate buffered saline (PBS) solution. Mass balance calculations showed that 34% of the input MS-2 was inactivated/irreversibly sorbed on the surface of Al-oxide coated sand whereas 100% of phiX174 was recovered. Results from this study also indicated that higher ionic strength facilitated the transport of both phiX174 and MS-2 through the Al-oxide coated sand. This was attributed to the effect of ion shielding, which at higher ionic strength decreased the electrostatic attraction between the viral particles and the sand surface and consequently decreased virus sorption. Strong effect of the ionic strength indicates that an outer-sphere complexation mechanism was responsible for the virus sorption on the Al-oxide coated sand. Ion composition of the background solutions was also found to be a significant factor in influencing virus retention and transport. Virus transport was enhanced in the presence of phosphate (HPO(4)(2-)) as compared to bicarbonate (HCO(3)(-)), and the effect of HPO(4)(2-) was more significant on MS-2 than on phiX174. The presence of bivalent cations (Ca(2+) and Mg(2+)) increased virus transport because the cations partially screened the negative charges on the viruses therefore decreased the electrostatic attraction between the positively charged sand surface and the negatively charged viruses. Mass recovery data indicated that bivalent cations gave rise to a certain degree of inactivation/irreversibly sorption of phiX174 on the surface of Al-oxide coated sand. On the contrary, the bivalent cations appeared to have protected MS-2 from inactivation/irreversibly sorption. This study provides some insights into the mechanisms responsible for virus retention and transport in porous media.     

Reactive transport of uranium(VI) and phosphate in a goethite-coated sand column: an experimental study

The migration of uranium(VI) in subsurface environments is strongly influenced by its adsorption/desorption reactions at the solid/solution interface. Phosphate is often present in subsurface systems and was shown to significantly affect U(VI) adsorption in previous batch experiments. In this study, column experiments were conducted to investigate the effects of phosphate on U(VI) adsorption and transport under flow conditions. The adsorption of U(VI) and phosphate was very low on pure quartz sand with negligible effects on U(VI) and phosphate transport. However, U(VI) and phosphate transport was retarded in a column packed with goethite-coated sand. The presence of phosphate, either as a co-solute with U(VI) or pre-adsorbed, greatly increased U(VI) adsorption and retardation. U(VI) and phosphate adsorption in our column experiments were rate-limited, and the adsorption of U(VI) and phosphate was not reversible, with kinetic limitations more pronounced for desorption than for adsorption. This study demonstrated the importance of phosphate in controlling U(VI) mobility in subsurface environments and helped illustrate some phenomena potentially applicable to U(VI) adsorption and transport in natural systems, especially where U(VI) adsorption is rate-limited.     

Effect of goethite coating and humic acid on the transport of bacteriophage PRD1 in columns of saturated sand

The transport of bacteriophage PRD1, a model virus, was studied in columns containing sediment mixtures of quartz sand with goethite-coated sand and using various solutions consisting of monovalent and divalent salts and humic acid (HA). Without HA and in the absence of sand, the inactivation rate of PRD1 was found to be as low as 0.014 day(-1) (at 5+/-3 degrees C), but in the presence of HA it was much lower (0.0009 day(-1)), indicating that HA helps PRD1 to survive. When the fraction of goethite in the sediment was increased, the removal of PRD1 also increased. However, in the presence of HA, C/C0 values of PRD1 increased by as much as 5 log units, thereby almost completely eliminating the effect of addition of goethite. The sticking efficiency was not linearly dependent on the amount of goethite added to the quartz sand; this is apparently due to surface charge heterogeneity of PRD1. Our results imply that, in the presence of dissolved organic matter (DOM), viruses can be transported for long distances thanks to two effects: attachment is poor because DOM has occupied favourable sites for attachment and inactivation of virus may have decreased. This conclusion justifies making conservative assumptions about the attachment of viruses when calculating protection zones for groundwater wells.     

Transport of biocolloids in water saturated columns packed with sand: Effect of grain size and pore water velocity

The main objective of this study was to evaluate the combined effects of grain size and pore water velocity on the transport in water saturated porous media of three waterborne fecal indicator organisms (Escherichia coli, MS2, and ΦX174) in laboratory-scale columns packed with clean quartz sand. Three different grain sizes and three pore water velocities were examined and the attachment behavior of Escherichia coli, MS2, and ΦX174 onto quartz sand was evaluated. The mass recoveries of the biocolloids examined were shown to be highest for Escherichia coli and lowest for MS2. However, no obvious relationships between mass recoveries and water velocity or grain size could be established from the experimental results. The observed mean dispersivity values for each sand grain size were smaller for bacteria than coliphages, but higher for MS2 than ΦX174. The single collector removal and collision efficiencies were quantified using the classical colloid filtration theory. Furthermore, theoretical collision efficiencies were estimated only for E. coli by the Interaction-Force-Boundary-Layer, and Maxwell approximations. Better agreement between the experimental and Maxwell theoretical collision efficiencies were observed.     

Intercomparison of reactive transport models applied to UO2 oxidative dissolution and uranium migration

Oxidative dissolution of uranium dioxide (UO(2)) and the subsequent migration of uranium in a subsurface environment and an underground waste disposal have been simulated with reactive transport models. In these systems, hydrogeological and chemical processes are closely entangled and their interdependency has been analyzed in detail, notably with respect to redox reactions, kinetics of mineralogical evolution and hydrodynamic migration of species of interest. Different codes, where among CASTEM, CHEMTRAP and HYTEC, have been used as an intercomparison and verification exercise. Although the agreement between codes is satisfactory, it is shown that the discretization method of the transport equation (i.e. finite elements (FE) versus mixed-hybrid FE and finite differences) and the sequential coupling scheme may lead to systematic discrepancies.     

Influence of detergent formulation on nutrient movement through sand columns simulating mound and conventional septic system drainfields

The effects of phosphate (P) and zeolite (Z) -built detergents on leaching of N and P through sand columns simulating septic system drainfields were examined in laboratory columns. To simulate mound septic system drainfields, paired sets of columns were dosed intermittently with septic tank effluent from households using P- or Z-built detergent. Two other paired sets of columns were flooded with P- or Z-effluent to simulate new conventional septic system drainfields; after clogging mats or “crusts” developed at infiltration surface, the subsurfaces of the columns were aerated to simulate mature (crusted) conventional septic system drainfields. NO₃ loading in leachate was 1.1 times higher and ortho-P loading was 4.3 times lower when columns were dosed with Z- than with P-effluent. Dosed columns removed P poorly; total phosphorus (TP) loading in leachate was 81 and 19 g m⁻² yr⁻¹ with P- and Z-effluent, respectively. In flooded columns 1.3, 2.0 and 1.8 times more NH₄, organic nitrogen (ON) and total nitrogen (TN) respectively, were leached with Z- than with P-effluent; NO₃ leaching was similar. Flooded columns removed P efficiently; TP leached through flooded systems was 2.5 and 1.4 g m⁻² yr⁻¹ with P- and Z effluent, respectively. Crusted columns fed Z-effluent leached 1.2, 2.6, 1.4 and 2.1 times more NH₄, NO₃, ON and TN, respectively, than those with P-effluent but 1.8 times less TP. Crusted columns removed P satisfactorily: 8.2 and 4.6 g m⁻² yr⁻¹ TP with P- and Z-effluent, respectively. The P-built detergent substantially improves the efficiency of N removal with satisfactory P removal in columns simulating conventional septic system drainfield. Simultaneous removal of N and P under flooded conditions might be explained by precipitation of struvite-type minerals. Dosed system drainfields were less efficient in removing N and P compared to flooded and crusted system drainfelds.     

Migration of uranium(IV)/(VI) in the presence of humic acids in quartz sand: a laboratory column study

The migration behavior of U(IV) and U(VI) in the presence of humic acid was studied in a quartz sand system. Laboratory column experiments were performed using humic acid, U(VI) in humic acid absence, U(IV) and U(VI) in humic acid presence, and for comparison a conservative tracer. In experiments using humic acid, both redox species of U migrate nearly as fast as the conservative tracer. Humic acid accelerates the U(VI) breakthrough compared to the humic acid-free system. There are strong indications for a similar effect on the U(IV) transport. At the same time, a part of U(IV) and U(VI) associated with the humic acid is immobilized in the quartz sand due to humic colloid filtration thus producing a delaying effect. Tailing at a low concentration level was observed upon tracer elution. The experimental breakthrough curves were described by reactive transport modeling using equations for equilibrium and kinetic reactions. The present study demonstrates that humic acids can play an important role in the migration of actinides. As natural organic matter is ubiquitous in aquifer systems, the humic colloid-borne transport of actinides is of high relevance in performance assessment.     

Assessment of uranium migration and pollution sources in river sediments of the Ili River Basin using multiply statistical techniques

Environmental Science and Pollution Research - Uranium (U) is a highly toxic radioactive element and limited to &lt; 30 μg/L in drinking water by the World Health Organization. In this...     

Intercomparison of reactive transport models applied to UO2 oxidative dissolution and uranium migration

Oxidative dissolution of uranium dioxide (UO₂) and the subsequent migration of uranium in a subsurface environment and an underground waste disposal have been simulated with reactive transport models. In these systems, hydrogeological and chemical processes are closely entangled and their interdependency has been analyzed in detail, notably with respect to redox reactions, kinetics of mineralogical evolution and hydrodynamic migration of species of interest.Different codes, where among CASTEM, CHEMTRAP and HYTEC, have been used as an intercomparison and verification exercise. Although the agreement between codes is satisfactory, it is shown that the discretization method of the transport equation (i.e. finite elements (FE) versus mixed-hybrid FE and finite differences) and the sequential coupling scheme may lead to systematic discrepancies.     

Influence of trivalent electrolytes on the humic colloid-borne transport of contaminant metals: competition and flocculation effects

With the objective to assess the relevance of competitive effects in respect of the humic colloid-borne migration of actinides in case of release, the influence of Al(III) on humate complexation of La(III) as an analogue of trivalent actinides was investigated for various humic materials by using 140La as a radioactive tracer, allowing measurements in very dilute systems to simulate realistic settings. Generally, competition by aluminium is not detectable unless the metal-loading capacity of the humic colloids is nearly exhausted. For average contents of organic carbon, a threshold value of 10(-6) M Al(III) can be specified. The metal exchange turned out to be kinetically hindered. Effects on co-adsorption of La(III) and humic acid were found to be less important. Immobilization by the concomitantly induced flocculation process outweighs the role of displacement effects. Comparative studies on complexation and flocculation of humic acid with Al(III), Ga(III), In(III), Sc(III), Y(III), and La(III) were undertaken in order to evaluate the influence of specific properties apart from ion charge and to characterize the mechanism of flocculation. In spite of considerable variations in the binding affinities among these metals, it can be inferred that the possibility of significant competitive effects in natural aquatic systems is confined to Al(III). Complex stabilities and flocculation efficiencies proved to be interrelated. Precipitation is thus attributed to homocoagulation of humic colloids induced by charge compensation, which is further supported by flocculation experiments with Al(III) depending on pH, ionic strength, and humic acid concentration.     

The migration of uranium into peat-rich soils at Broubster, Caithness, Scotland, U.K.

Uranium is being actively transported from uraniferous sedimentary rocks into a peat bog at the Broubster natural analogue site in Caithness, Scotland. Massive calcareous sandstone within the Caithness Flags sequence is the main source of uranium which resides primarily within diagenetic apatite and dispersed U---Si---Ti phases. Supergene weathering processes have decalcified the sandstone and are effective in mobilising uranium by groundwater leaching, primarily along a fault zone. Uranium transport in solution by means of groundwater and surface flows is effectively terminated by retardation within 4-kyr-old peat deposits laid down on boulder clay. This process of secondary fixation has resulted in a young uranium anomaly in the peat which comprises in excess of 0.1 wt% U. The site has been investigated comprehensively to define the geometry of the anomaly together with the hydrogeology, hydrochemistry, petrology, mineralogy and the nature of the peat sink-term. The main physical and geochemical properties of the system, including the uranium decay series radionuclide distributions in water and solid samples, are documented in this paper. From these data, the processes governing the distribution of uranium have been quantified using a three-dimensional groundwater flow package and an equilibrium speciation model incorporating a recently developed electrostatic surface complexation model to account for cation-organic interactions. The results described form part of a coordinated project on natural radionuclide migration undertaken to improve confidence in predictive methods used for radiological assessment.