Transport of Escherichia coli in saturated porous media: dual mode deposition and intra-population heterogeneity

Because of heterogeneity among members of a bacteria population, deposition rates of bacteria may decrease upon the distance bacteria are transported in an aquifer. Such deposition rate decreases may result in retained bacteria concentrations, which decrease hyper-exponentially as a function of transport distance, and may therefore significantly affect the transport of colloids in aquifers. We investigated the occurrence of hyper-exponential deposition of Escherichia coli, an important indicator for fecal contamination, and the causes for such behavior. In a series of column experiments with glass beads of various sizes, we found that attachment of E. coli decreased hyper-exponentially, or, on logarithmic scale in a bimodal way, as a function of the transported distance from the column inlet. From data fitting of the retained bacteria concentration profiles, the sticking efficiency of 40% of the E. coli population was high (alpha=1), while the sticking efficiency of 60% was low (alpha=0.01). From the E. coli total population, an E. coli subpopulation consisting of slow attachers could be isolated by means of column passage. In subsequent column experiments this subpopulation attached less than the E. coli total population, consisting of both slow and fast attachers. We concluded that the main driver for the observed dual mode deposition was heterogeneity among members of the bacteria population. Intra-population may result in some microbes traveling surprisingly high distances in the subsurface. Extending the colloid filtration theory with intra-population variability may provide a valuable framework for assessing the transport of bacteria in aquifers.     

Aggregation and deposition kinetics of carboxymethyl cellulose-modified zero-valent iron nanoparticles in porous media

Transport and deposition of carboxymethyl cellulose (CMC)-modified nanoparticles of zero-valent iron (NZVI) were investigated in laboratory-scale sand packed columns. Aggregation resulted in a change in the particle size distribution (PSD) with time, and the changes in average particle size were determined by nanoparticle tracking analysis (NTA). The change in PSD over time was influenced by the CMC-NZVI concentration in suspension. A particle-particle attachment efficiency was evaluated by fitting an aggregation model with NTA data and subsequently used to predict changes in PSD over time. Changes in particle sizes over time led to corresponding changes in single-collector contact efficiencies, resulting in altered particle deposition rates over time. A coupled aggregation-colloid transport model was used to demonstrate how changes in PSD can reduce the transport of CMC-NZVI in column experiments. The effects of particle concentrations in the range of 0.07 g L⁻¹ to 0.725 g L⁻¹ on the transport in porous media were evaluated by comparing the elution profiles of CMC-NZVI from packed sand columns. Changes in PSD over time could reasonably account for a gradual increase in effluent concentration between 1 and 5 pore volumes (PVs). Processes such as detachment of deposited particles also likely contributed to the gradual increase in effluent concentrations. The particle-collector attachment efficiency increased with CMC-NZVI particle concentration due to a rise in dissolved Na⁺ concentration with increased addition of Na-CMC. This inadvertent change in ionic strength led to decreased effluent concentrations at higher CMC-NZVI concentrations.     

Transport and fate of Cryptosporidium parvum oocysts in intermittent sand filters.

The transport potential of Cryptosporidium parvum (C. parvum) through intermittent, unsaturated, sand filters used for water and wastewater treatment was investigated using a duplicated, 2³ factorial design experiment performed in bench-scale, sand columns. Sixteen columns (dia=15 cm, L=60 cm) were dosed eight times daily for up to 61 days with 65,000 C. parvum oocysts per liter at 15°C. The effects of water quality, media grain size, and hydraulic loading rates were examined. Effluent samples were tested for pH, turbidity, and oocyst content. C. parvum effluent concentrations were determined by staining oocysts on polycarbonate filters and enumerating using epifluorescent microscopy. At completion, the columns were dismantled and sand samples were taken at discrete depths within the columns. These samples were washed in a surfactant solution and the oocysts were enumerated using immunomagnetic separation techniques.

The fine-grained sand columns (d₅₀=0.31 mm) effectively removed oocysts under the variety of conditions examined with low concentrations of oocysts infrequently detected in the effluent. Coarse-grained media columns (d₅₀=1.40 mm) yielded larger numbers of oocysts which were commonly observed in the effluent regardless of operating conditions. Factorial design analysis indicated that grain size was the variable which most affected the oocyst effluent concentrations in these intermittent filters. Loading rate had a significant effect when coarse-grained media was used and lesser effect with fine-grained media while the effect of feed composition was inconclusive. No correlations between turbidity, pH, and effluent oocyst concentrations were found. Pore-size calculations indicated that adequate space for oocyst transport existed in the filters. It was therefore concluded that processes other than physical straining mechanisms are mainly responsible for the removal of C. parvum oocysts from aqueous fluids in intermittent sand filters used under the conditions studied in this research.     

Transport and fate of Cryptosporidium parvum oocysts in intermittent sand filters

The transport potential of Cryptosporidium parvum (C. parvum) through intermittent, unsaturated, sand filters used for water and wastewater treatment was investigated using a duplicated, 2³ factorial design experiment performed in bench-scale, sand columns. Sixteen columns (dia=15 cm, L=60 cm) were dosed eight times daily for up to 61 days with 65,000 C. parvum oocysts per liter at 15°C. The effects of water quality, media grain size, and hydraulic loading rates were examined. Effluent samples were tested for pH, turbidity, and oocyst content. C. parvum effluent concentrations were determined by staining oocysts on polycarbonate filters and enumerating using epifluorescent microscopy. At completion, the columns were dismantled and sand samples were taken at discrete depths within the columns. These samples were washed in a surfactant solution and the oocysts were enumerated using immunomagnetic separation techniques.The fine-grained sand columns (d₅₀=0.31 mm) effectively removed oocysts under the variety of conditions examined with low concentrations of oocysts infrequently detected in the effluent. Coarse-grained media columns (d₅₀=1.40 mm) yielded larger numbers of oocysts which were commonly observed in the effluent regardless of operating conditions. Factorial design analysis indicated that grain size was the variable which most affected the oocyst effluent concentrations in these intermittent filters. Loading rate had a significant effect when coarse-grained media was used and lesser effect with fine-grained media while the effect of feed composition was inconclusive. No correlations between turbidity, pH, and effluent oocyst concentrations were found. Pore-size calculations indicated that adequate space for oocyst transport existed in the filters. It was therefore concluded that processes other than physical straining mechanisms are mainly responsible for the removal of C. parvum oocysts from aqueous fluids in intermittent sand filters used under the conditions studied in this research.     

Aggregation and transport of nano-TiO2 in saturated porous media: effects of pH, surfactants and flow velocity

Transport of manufactured nano-TiO₂ in saturated porous media was investigated as a function of morphology characteristics, pH of solutions, flow velocity, and the presence of anionic and non-ionic surfactants in different concentrations. Surfactants enhanced the transport of nano-TiO₂ in saturated porous media while a pH approaching the point of zero charge of nano-TiO₂ limited their transport. The deposition process, a retention mechanism of nano-TiO₂ in saturated porous media was impacted by surfactant and pH. In Dispersion 1 systems (pH 7), the size of the nano-TiO₂ aggregates was directly related to the presence of surfactants. The presence of non-ionic surfactant (Triton X-100) induced a size reduction of nano-TiO₂ aggregates that was dependent on the critical micelle concentration. In Dispersion 2 systems (pH 9), the stability provided by the pH had a significant effect on the size of nano-TiO₂ aggregates; the addition of surfactants did impact the size of the nano-TiO₂ aggregates but in less significance as compared to Dispersion 1 systems. The electrostatic and steric repulsion forces in connection with the size of nano-TiO₂ aggregates and flow velocity impacted the single-collector efficiency and attachment efficiency which dictated the maximum transport distance of nano-TiO₂ for the Dispersion 1 and Dispersion 2 systems. By doubling the flow velocity at pH 9, the No Surfactant, 50% CMC Triton X-100, 100% CMC Triton X-100 and 100% CMC SDBS dispersion systems allowed nano-TiO₂ to attain maximum transport distances of 0.898, 2.17, 2.29 and 1.12 m, respectively. Secondary energy minima played a critical role in the deposition mechanisms of nano-TiO₂. Nano-TiO₂ deposited in the secondary energy wells may be released because of changes in solution chemistry. The deposition of nano-TiO₂ in primary and secondary energy minima, the reversibility of their deposition should be characterized to analyze the transport of nanoparticles in porous media. This is necessary to assess the risk of nanoparticles to the environment and public health.     

Vertical migration of chlorinated organic compounds in porous media

The migration behavior of trichloroethylene through porous media made of glass beads of 5, 3 and 1 mm dia is described. Experiments were carried out in three hydraulic conditions: (1) unsaturated (completely dry), (2) saturated and (3) two layers (the upper portion of the porous media being unsaturated and the lower portion being saturated). In the case of the dry condition (1) trichloroethylene easily flows through the porous media regardless of the size of the glass beads, while it remains in the pore space in the saturated medium in the saturated condition (2). The stagnation of test liquid in the saturated medium increases with decreasing glass bead diameter. With 5 mm glass beads, in the case of condition (3), all the liquid coming from the upper portion moved into the saturated zone, whereas with 3 and 1 mm glass beads, the liquid seemed to stagnate on the surface of the saturated zone. With 1 mm glass beads, especially, almost all the liquid remained stagnant in the boundary region between the unsaturated and the saturated zone. The difference of the trichloroethylene behavior in the capillary zone can be qualitatively explained from the results of the visualized testing by means of the Hele-Shaw model.     

多孔介质中氚的滞留及对相关试验的影响

在进行氚在黏土矿物中的滞留试验基础上,对试验结果进行了总结,分析了滞留现象对相关水文地质、环境地质参数试验的影响。结果表明:氚在蒙脱石、高岭石、伊利石等孔隙介质中的平均分配系数分别为0.15 ml/g、0.10 ml/g、0.12ml/g;氚的绝对吸附量随氚水比活度的增加而增大,绝对吸附量的对数与相应氚水比活度的对数呈直线相关关系;氚的滞留将使野外弥散试验获得的弥散度和弥散系数减小,使得室内示踪试验获得的孔隙水流速比实际孔隙水流速减小5%~25%,使得按照3H测龄方法获得的亚砂土等含水层中地下水年龄增大5%~20%,按照3H-3He测龄方法获得的地下水年龄比实际情况增大4%~18%。     

On the role of metabolic activity on the transport und deposition of Pseudomonas fluorescens in saturated porous media

A study was conducted to understand the role of cell concentration and metabolic state in the transport and deposition behaviour of Pseudomonas fluorescens with and without substrate addition. Column experiments using the short-pulse technique (pulse was equivalent to 0.028 pore volume) were performed in quartz sand operating under saturated conditions. For comparison, experiments with microspheres and inactive (killed) bacteria were also conducted. The effluent concentrations, the retained particle concentrations and the cell shape were determined by fluorescent microscopy. For the transport of metabolically-active P. fluorescens without substrate addition a bimodal breakthrough curve was observed, which could be explained by the different breakthrough behaviour of the rod-shaped and coccoidal cells of P. fluorescens. The 70:30 rod/coccoid ratio in the influent drastically changed during the transport and it was about 20:80 in the effluent and in the quartz sand packing. It was assumed that the active rod-shaped cells were subjected to shrinkage into coccoidal cells. The change from active rod-shaped cells to coccoidal cells could be explained by oxygen deficiency which occurs in column experiments under saturated conditions. Also the substrate addition led to two consecutive breakthrough peaks and to more bacteria being retained in the column. In general, the presence of substrate made the assumed stress effects more pronounced. In comparison to microspheres and inactive (killed) bacteria, the transport of metabolically-active bacteria with and without substrate addition is affected by differences in physiological state between rod-shaped and the formed stress-resistant coccoidal cells of P. fluorescens.     

The effects of biofilm on the transport of stabilized zerovalent iron nanoparticles in saturated porous media

The transport of stabilized zerovalent iron nanoparticles (nZVI) has recently been the topic of extensive research due to its proven potential as an in situ remediation tool. However, these studies have ignored the effects of biofilms—complex aggregations of bacterial cells and excreted extracellular polymeric substances present in nearly all aquatic systems—on the transport of these particles. This study examines the effects of Pseudomonas aeruginosa (PAO1) biofilm, at a cell concentration similar to that reported for saturated aquifers, on the transport of commercially available, poly (acrylic acid) stabilized nZVI (pnZVI) in 14 cm long columns packed with saturated glass beads at salt concentrations of 1 and 25 mM NaCl. Compared to retention on uncoated columns, in the presence of biofilm the retention of pnZVI increased at higher ionic strength, while ionic strength played no role in retention of these nanoparticles in the absence of biofilm. The Tufenkji-Elimelech correlation equation predicts lower retention of pnZVI on biofilm coated columns compared to uncoated columns due to a lower Hamaker constant, and DLVO energy considerations predict the most favorable attachment to uncoated porous media at higher ionic strength. A steric (polymer-mediated) model that considers the combined influence of steric effects of polymers and DLVO interactions is shown to adequately describe particle retention in columns.     

Non-equilibrium partitioning tracer transport in porous media: 2-D physical modelling and imaging using a partitioning fluorescent dye

This paper describes an investigation into non-equilibrium partitioning tracer transport and interaction with non-aqueous-phase liquid (NAPL) contaminated water-saturated porous media using a two-dimensional (2-D) physical modelling methodology. A fluorescent partitioning tracer is employed within a transparent porous model which when imaged by a CCD digital camera can provide full spatial tracer concentrations and tracer breakthrough curves. Quasi one-dimensional (1-D) benchmarking tests in models packed with various combinations of clean quartz sand and NAPL are described. These modelled residual NAPL saturations, S_n, of 0–15%. Results demonstrated that the fluorescent partitioning tracer was able to detect and quantify the presence of NAPL at low flow rates. At larger flow rates and/or higher NAPL saturations, the tracer increasingly underpredicted the NAPL volume as expected and this is attributed primarily to non-equilibrium partitioning. Despite little change in permeability, change in NAPL saturations from 4% to 8% resulted in significant NAPL saturation underestimates at the same flow rates implying coalescence of NAPL into wider separated but larger ganglia. A 2-D investigation of an idealised heterogeneous residual NAPL contaminated flow field indicated little permeability change in the NAPL contaminated zone and thus little flow bypassing, leading to reduced underpredictions of NAPL saturations than for equivalent quasi 1-D cases. This was attributed to increased ‘sampling’ of the NAPL by the tracer. The process is clearly visually identifiable from the experimental images. This rapid and relatively inexpensive experimental method is of value in laboratory studies of partitioning tracer behaviour in porous media; in particular, the ability to observe full field concentrations makes it valuable for the study of complex heterogeneous systems.     

Fate and transport of elemental copper (Cu0) nanoparticles through saturated porous media in the presence of organic materials

Column experiments were performed to assess the fate and transport of nanoscale elemental copper (Cu⁰) particles in saturated quartz sands. Both effluent concentrations and retention profiles were measured over a broad range of physicochemical conditions, which included pH, ionic strength, the presence of natural organic matter (humic and fulvic acids) and an organic buffer (Trizma). At neutral pHs, Cu⁰ nanoparticles were positively charged and essentially immobile in porous media. The presence of natural organic matter, trizma buffer, and high pH decreased the attachment efficiency facilitating elemental copper transport through sand columns. Experimental results suggested the presence of both favourable and unfavourable nanoparticle interactions causes significant deviation from classical colloid filtration theory.     

Interactions between laponite and microbial biofilms in porous media: implications for colloid transport and biofilm stability

Quartz sand columns and sand-filled microscope flow cells were used to investigate the transport characteristics of the clay colloid laponite, and a biofilm-forming bacterium, Pseudomonas aeruginosa SG81. Separate experiments were performed with each particle to determine their individual transport characteristics in clean sand columns. In a second set of experiments, bacterial biofilms were formed prior to introduction of the clay colloids. In the independent transport experiments, bacteria and laponite each conformed to known physicochemical principles. A sodium chloride concentration of 7 x 10(-2) M caused complete retention of the laponite within the sand columns. P. aeruginosa SG81 was generally less influenced by ionic strength effects; it showed relatively low mobility at all ionic strengths tested and some (albeit reduced) mobility when introduced to the columns in 1M NaCl, the highest concentration tested, but nevertheless showed reproducible trends. Under conditions favourable to laponite retention and biofilm stability (7 x 10(-2) MNaCl), laponite suspensions were able to remobilise a portion of the attached bacterial biomass. At low ionic strength, the profile of laponite elution was also altered in the presence of a P. aeruginosa biofilm. These observations suggest that while a reduction in ionic strength has a dominant influence on the mobilisation of biological and inorganic colloids, the presence of laponite and biomass can have a distinct influence on the mobility of both types of colloids. Since these events are likely to occur in subsurface environments, our results suggest that colloid-biofilm interactions will have implications for colloid-bound contaminant transport and the remobilisation of pathogens.     

考虑多孔介质迂回曲折效应的幂律流体柱形渗透注浆机制

多孔介质的迂回曲折效应对浆液在其中的渗透扩散与注浆效果具有非常重要的影响.采用理论分析,研究考虑多孔介质迂回曲折效应的幂律流体渗流运动方程,推导考虑多孔介质迂回曲折效应的幂律流体柱形渗透注浆机制;基于计算机编程技术,依托COMSOL Multiphysics平台与达西定律,二次开发得到考虑多孔介质迂回曲折效应的幂律流体...     

Transport of two metal oxide nanoparticles in saturated granular porous media: role of water chemistry and particle coating

The growing use of nanosized titanium dioxide (nTiO₂) and zinc oxide (nZnO) in a large number of commercial products raises concerns regarding their release and subsequent mobility in natural aquatic environments. Laboratory-scale sand-packed column experiments were conducted with bare and polymer-coated nTiO₂ and nZnO to improve our understanding of the mobility of these nanoparticles in natural or engineered water saturated granular systems. The nanoparticles are characterized over a range of environmentally relevant water chemistries using multiple complimentary techniques: dynamic light scattering, nanoparticle tracking analysis, transmission electron microscopy, and scanning electron microscopy. Overall, bare (uncoated) nanoparticles exhibit high retention within the water saturated granular matrix at solution ionic strengths (IS) as low as 0.1 mM NaNO₃ for bare nTiO₂ and 0.01 mM NaNO₃ for bare nZnO. Bare nTiO₂ and nZnO also display dynamic (time-dependent) deposition behaviors under selected conditions. In contrast, the polymer-coated nanoparticles are much less likely to aggregate and exhibit significant transport potential at IS as high as 100 mM NaNO₃ or 3 mM CaCl₂. These findings illustrate the importance of considering the extent and type of surface modification when evaluating metal oxide contamination potential in granular aquatic environments.     

混凝土中介质迁移表观动力学初探

基于 Fick 第二定律和 Darcy 定律,对混凝土中介质迁移表观动力学模型进行了理论推导,讨论了该模型对钢筋混凝土耐久性研究与设计的意义.     

Transport of microsporidium Encephalitozoon intestinales spores in sandy porous media

The retention and transport of microsporidium Encephalitozoon intestinales spores in two water-saturated sandy porous media was investigated in this study. The initial breakthrough of the spores in the column effluent occurred essentially simultaneously with that of a non-reactive tracer, indicating no significant velocity enhancement. A large fraction (45-73%) of the spores injected into the columns was not recovered in the effluent, indicating removal from solution through colloid retention processes of attachment and/or straining. The relative significance of attachment and straining to total retention was evaluated in additional experiments. An experiment was conducted with a sieved coarse fraction of porous media for which straining is unlikely to be of significance based on the relative diameters of the spores and porous-medium pores. The spore recovery for this experiment was similar to the recoveries obtained for microsporidia transport in the un-sieved parent porous medium. An additional experiment was conducted with a subsample of the coarse fraction that was acid-washed to reduce potential surface attachment sites. Spore recovery was complete for this experiment. These results suggest surface deposition was the primary removal mechanism in our system. This conclusion is supported by the results of an experiment wherein deionized water was flushed through a column that was previously flushed with electrolyte solution. The effluent spore concentrations were observed to increase upon injection of deionized water, indicating re-mobilization of spores upon a change in water chemistry. The measured data were successfully simulated using a mathematical model incorporating colloid filtration. The results of this study suggest that the transport of microspordia in sandy porous media is governed by established colloid-transport processes.     

Coupling of physical and chemical mechanisms of colloid straining in saturated porous media

Filtration theory does not include the potential influence of pore structure on colloid removal by straining. Conversely, previous research on straining has not considered the possible influence of chemical interactions. Experimental and theoretical studies were therefore undertaken to explore the coupling of physical and chemical mechanisms of colloid straining under unfavorable attachment conditions (pH=10). Negatively charged latex microspheres (1.1 and 3mum) and quartz sands (360, 240, and 150mum) were used in packed column studies that encompassed a range in suspension ionic strengths (6-106mM) and Darcy water velocities (0.1-0.45cmmin(-1)). Derjaguin-Landau-Verwey-Overbeek (DLVO) calculations and torque analysis suggests that attachment of colloids to the solid-water interface was not a significant mechanism of deposition for the selected experimental conditions. Effluent concentration curves and hyperexponential deposition profiles were strongly dependent on the solution chemistry, the system hydrodynamics, and the colloid and collector grain size, with greater deposition occurring for increasing ionic strength, lower flow rates, and larger ratios of the colloid to the median grain diameter. Increasing the solution ionic strength is believed to increase the force and number of colloids in the secondary minimum of the DLVO interaction energy profile. These weakly associated colloids can be funneled to small regions of the pore space formed adjacent to grain-grain junctions. For select systems, the ionic strength of the eluant solution was decreased to 6mM following the recovery of the effluent concentration curve. In this case, only a small portion of the deposited colloids was recovered in the effluent and the majority was still retained in the sand. These observations suggest that the extent of colloid removal by straining is strongly coupled to solution chemistry.     

Transport of E. coli in columns of geochemically heterogeneous sediment

To elucidate the parameters determining the transport of Escherichia coli in aquifers, the attachment of E. coli in low concentrations to column sediments was investigated. The sediments comprised 0.18-0.50mm quartz sand, grains coated with goethite, calcite grains or grains of activated carbon (AC), in varying fractions (lambda=0, 0.05, 0.1, 0.2, 0.4, 0.7, 1.0) and all of similar diameter to the quartz sand. The weighted sum of favourable and unfavourable sticking efficiencies (alpha(total)) showed that upon increasing the fraction of favourable mineral grains (lambda) there was an initial rapid increase, which then slowed down. This was most pronounced in the AC experiments, followed by the calcite experiments and then the goethite experiments. We ascribe this non-linear relation to surface charge and hydrophobic heterogeneity of the E. coli population.     

Influence of biofilm on the transport of fullerene (C60) nanoparticles in porous media

The significance of biofilm on fullerene C₆₀ nanoparticles transport and deposition were examined both in porous media and quartz crystal microbalance with dissipation (QCM-D) systems under a variety of environmentally relevant ionic strength (1-25 mM in NaCl and 0.1-5 mM in CaCl₂) and flow conditions (4-8 m day⁻¹). The magnitudes of deposition rate coefficients (k_d) were compared between porous media with and without biofilm extracellular polymeric substances (EPS) coating under equivalent fluid velocities and solution chemistries. The observed k_d were greater in porous media with biofilm EPS coating relative to those without biofilm EPS coating across the entire solution ionic strengths and fluid velocities examined, demonstrating that the enhancement of C₆₀ deposition by the biofilm EPS coating is relevant to a wide range of environmental conditions. This greater deposition was also observed on silica surfaces with biofilm EPS coating in QCM-D system. The results clearly showed that biofilm EPS have a great influence on C₆₀ deposition. Derjaguin-Landau-Verwey-Overbeek (DLVO) theory could not explain the enhanced C₆₀ deposition by biofilm EPS. Biochemical and physical characteristics of biofilm EPS were responsible for the increased C₆₀ deposition.