Publications

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The potential to treat non-traditional water sources using power plant waste heat in conjunction with membrane distillation is assessed. Researchers and power plant designers continue to search for ways to use that waste heat from Rankine cycle power plants to recover water thereby reducing water net water consumption. Unfortunately, waste heat from a power plant is of poor quality. Membrane distillation (MD) systems may be a technology that can use the low temperature waste heat (<100 F) to treat water. By their nature, they operate at low temperature and usually low pressure. This study investigates the use of MD to recover water from typical power plants. It looks at recovery from three heat producing locations (boiler blow down, steam diverted from bleed streams, and the cooling water system) within a power plant, providing process sketches, heat and material balances and equipment sizing for recovery schemes using MD for each of these locations. It also provides insight into life cycle cost tradeoffs between power production and incremental capital costs.

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Nanofiltration (NF) can effectively treat cooling-tower water to reduce water consumption and maximize water usage efficiency of thermoelectric power plants. A pilot is being run to verify theoretical calculations. A side stream of water from a 900 gpm cooling tower is being treated by NF with the permeate returning to the cooling tower and the concentrate being discharged. The membrane efficiency is as high as over 50%. Salt rejection ranges from 77-97% with higher rejection for divalent ions. The pilot has demonstrated a reduction of makeup water of almost 20% and a reduction of discharge of over 50%.

Nanofiltration (NF) can effectively treat cooling-tower water to reduce water consumption and maximize water usage efficiency of thermoelectric power plants. A pilot is being run to verify theoretical calculations. A side stream of water from a 900 gpm cooling tower is being treated by NF with the permeate returning to the cooling tower and the concentrate being discharged. The membrane efficiency is as high as over 50%. Salt rejection ranges from 77-97% with higher rejection for divalent ions. The pilot has demonstrated a reduction of makeup water of almost 20% and a reduction of discharge of over 50%.

The market for polyamide desalination membranes is expected to continue to grow during the coming decades. Purification of alternative water sources will also be necessary to meet growing water demands. Purification of produced water, a byproduct of oil and gas production, is of interest due to its dual potential to provide water for beneficial use as well as to reduce wastewater disposal costs. However, current polyamide membranes are prone to fouling, which decreases water flux and shortens membrane lifetime. This research explored surface modification using poly(ethylene glycol) diglycidyl ether (PEGDE) to improve the fouling resistance of commercial polyamide membranes. Characterization of commercial polyamide membrane performance was a necessary first step before undertaking surface modification studies. Membrane performance was found to be sensitive to crossflow testing conditions. Concentration polarization and feed pH strongly influenced NaCl rejection, and the use of continuous feed filtration led to higher water flux and lower NaCl rejection than was observed for similar tests performed using unfiltered feed. Two commercial polyamide membranes, including one reverse osmosis and one nanofiltration membrane, were modified by grafting PEGDE to their surfaces. Two different PEG molecular weights (200 and 1000) and treatment concentrations (1% (w/w) and 15% (w/w)) were studied. Water flux decreased and NaCl rejection increased with PEGDE graft density ({micro}g/cm{sup 2}), although the largest changes were observed for low PEGDE graft densities. Surface properties including hydrophilicity, roughness and charge were minimally affected by surface modification. The fouling resistance of modified and unmodified membranes was compared in crossflow filtration studies using model foulant solutions consisting of either a charged surfactant or an oil in water emulsion containing n-decane and a charged surfactant. Several PEGDE-modified membranes demonstrated improved fouling resistance compared to unmodified membranes of similar initial water flux, possibly due to steric hindrance imparted by the PEG chains. Fouling resistance was higher for membranes modified with higher molecular weight PEG. Fouling was more extensive for feeds containing the cationic surfactant, potentially due to electrostatic attraction with the negatively charged membranes. However, fouling was also observed in the presence of the anionic surfactant, indicating hydrodynamic forces are also responsible for fouling.

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Scoping studies have demonstrated that ceragenins, when linked to water-treatment membranes have the potential to create biofouling resistant water-treatment membranes. Ceragenins are synthetically produced molecules that mimic antimicrobial peptides. Evidence includes measurements of CSA-13 prohibiting the growth of and killing planktonic Pseudomonas fluorescens. In addition, imaging of biofilms that were in contact of a ceragenin showed more dead cells relative to live cells than in a biofilm that had not been treated with a ceragenin. This work has demonstrated that ceragenins can be attached to polyamide reverse osmosis (RO) membranes, though work needs to improve the uniformity of the attachment. Finally, methods have been developed to use hyperspectral imaging with multivariate curve resolution to view ceragenins attached to the RO membrane. Future work will be conducted to better attach the ceragenin to the RO membranes and more completely test the biocidal effectiveness of the ceragenins on the membranes.

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The formation of silica scale is a problem for thermoelectric power generating facilities, and this study investigated the potential for removal of silica by means of chemical coagulation from source water before it is subjected to mineral concentration in cooling towers. In Phase I, a screening of many typical as well as novel coagulants was carried out using concentrated cooling tower water, with and without flocculation aids, at concentrations typical for water purification with limited results. In Phase II, it was decided that treatment of source or make up water was more appropriate, and that higher dosing with coagulants delivered promising results. In fact, the less exotic coagulants proved to be more efficacious for reasons not yet fully determined. Some analysis was made of the molecular nature of the precipitated floc, which may aid in process improvements. In Phase III, more detailed study of process conditions for aluminum chloride coagulation was undertaken. Lime-soda water softening and the precipitation of magnesium hydroxide were shown to be too limited in terms of effectiveness, speed, and energy consumption to be considered further for the present application. In Phase IV, sodium aluminate emerged as an effective coagulant for silica, and the most attractive of those tested to date because of its availability, ease of use, and low requirement for additional chemicals. Some process optimization was performed for coagulant concentration and operational pH. It is concluded that silica coagulation with simple aluminum-based agents is effective, simple, and compatible with other industrial processes.

Biofouling, the unwanted growth of biofilms on a surface, of water-treatment membranes negatively impacts in desalination and water treatment. With biofouling there is a decrease in permeate production, degradation of permeate water quality, and an increase in energy expenditure due to increased cross-flow pressure needed. To date, a universal successful and cost-effect method for controlling biofouling has not been implemented. The overall goal of the work described in this report was to use high-performance computing to direct polymer, material, and biological research to create the next generation of water-treatment membranes. Both physical (micromixers - UV-curable epoxy traces printed on the surface of a water-treatment membrane that promote chaotic mixing) and chemical (quaternary ammonium groups) modifications of the membranes for the purpose of increasing resistance to biofouling were evaluated. Creation of low-cost, efficient water-treatment membranes helps assure the availability of fresh water for human use, a growing need in both the U. S. and the world.

The drift-shadow effect describes capillary diversion of water flow around a drift or cavity in porous or fractured rock, resulting in lower water flux directly beneath the cavity. This paper presents computational simulations of drift-shadow experiments using dual-permeability models, similar to the models used for performance assessment analyses of flow and seepage in unsaturated fractured tuff at Yucca Mountain. Results show that the dual-penneability models capture the salient trends and behavior observed in the experiments, but constitutive relations (e.g., fracture capillary-pressure curves) can significantly affect the simulated results. An evaluation of different meshes showed that at the grid refinement used, a comparison between orthogonal and unstructured meshes did not result in large differences.

The drift-shadow effect describes capillary diversion of water flow around a drift or cavity in porous or fractured rock, resulting in lower water flux directly beneath the cavity. This paper presents computational simulations of drift-shadow experiments using dual-permeability models, similar to the models used for performance assessment analyses of flow and seepage in unsaturated fractured tuff at Yucca Mountain. Results show that the dual-penneability models capture the salient trends and behavior observed in the experiments, but constitutive relations (e.g., fracture capillary-pressure curves) can significantly affect the simulated results. An evaluation of different meshes showed that at the grid refinement used, a comparison between orthogonal and unstructured meshes did not result in large differences.

Scoping studies have demonstrated that ceragenins, when linked to water-treatment membranes have the potential to create biofouling resistant water-treatment membranes. Ceragenins are synthetically produced molecules that mimic antimicrobial peptides. Evidence includes measurements of CSA-13 prohibiting the growth of and killing planktonic Pseudomonas fluorescens. In addition, imaging of biofilms that were in contact of a ceragenin showed more dead cells relative to live cells than in a biofilm that had not been treated with a ceragenin. This work has demonstrated that ceragenins can be attached to polyamide reverse osmosis (RO) membranes, though work needs to improve the uniformity of the attachment. Finally, methods have been developed to use hyperspectral imaging with multivariate curve resolution to view ceragenins attached to the RO membrane. Future work will be conducted to better attach the ceragenin to the RO membranes and more completely test the biocidal effectiveness of the ceragenins on the membranes.

There is strong interest in the detection and monitoring of bio-fouling. Bio-fouling problems are common in numerous water treatments systems, medical and dental apparatus and food processing equipment. Current bio-fouling control protocols are time consuming and costly. New early detection techniques to monitor bio-forming contaminates are means to enhanced efficiency. Understanding the unique dielectric properties of biofilm development, colony forming bacteria and nutrient background will provide a basis to the effectiveness of controlling or preventing biofilm growth. Dielectric spectroscopy measurements provide values of complex permittivity, {var_epsilon}*, of biofilm formation by applying a weak alternating electric field at various frequencies. The dielectric characteristic of the biofilm, {var_epsilon}{prime}, is the real component of {var_epsilon}* and measures the biofilm's unique ability to store energy. Graphically observed dependencies of {var_epsilon}{prime} to frequency indicate dielectric relaxation or dielectric dispersion behaviors that mark the particular stage of progression during the development of biofilms. In contrast, any frequency dependency of the imaginary component, {var_epsilon}{double_prime} the loss factor, is expressed as dielectric losses from the biofilm due to dipole relaxation. The tangent angle of these two component vectors is the ratio of the imaginary component to the real component, {var_epsilon}{double_prime}/{var_epsilon}{prime} and is referred to as the loss angle tangent (tan {delta}) or dielectric loss. Changes in tan {delta} are characteristic of changes in dielectric losses during various developmental stages of the films. Permittivity scans in the above figure are of biofilm growth from P. Fluorescens (10e7 CFU's at the start). Three trends are apparent from these scans, the first being a small drop in the imaginary permittivity over a 7 hours period, best seen in the Cole-Cole plot (a). The second trend is observed two hours after inoculation when the permittivity begins to increase slightly over the next 20 hours, best seen in the shift from 1000 Hz to 5000 Hz in tan {delta} at the high frequencies (c). Because of similar dielectric relaxation properties noted by the comparable size of the semicircles, plot (a), and the height of tan {delta}, plot (c), within the first 29 hours, cell activity levels did not appreciably change. The third trend is observed when the complex permittivity value drops by orders of magnitude between 29 hours and 37 hours, best seen in the log [E] plot (b), and in the drop of the dielectric loss, tan {delta}, to 0. This change in the dielectric properties in the bio environment is nearly independent of all frequencies (c) and dissimilar from the original condition when only bacteria and nutrient was present in the biofilm chambers. The semicircles in plot (a) for this period decreased below the resolution of the graph, implying a large difference in the dielectric behavior of the cells/biofilms consisting of low dielectric losses. We believe these large changes are related to the on-set of biofilms.

Features (micromixers) that promote chaotic mixing were fabricated on reverse-osmosis membrane surfaces and evaluated using computational models and laboratory experiments to determine their effectiveness in reducing biofouling. Computational fluid dynamics models of membrane feed channels were developed using different patterns of micromixers on the membrane surface. The shear-stress distribution along the membrane surface was simulated for steady flows along the different micromixer configurations. In addition, the hypothetical mass transfer of a tracer from the membrane surface was used as a metric to compare the amount of scouring and mixing in configurations with and without micromixers. Epoxy micromixers were printed directly onto membrane surfaces, and different patterns were evaluated experimentally. Fluorescence hyperspectral imaging results showed that regions of simulated high shear stress on the membrane corresponded to regions of lower bacterial growth in the experiments, while regions of simulated low shear stress corresponded to regions of higher bacterial growth. In addition, the presence of the micromixers appeared to reduce the overall biofouling concentration in one series of experiments, but the results were inconclusive in another series of experiments. These results indicate that while the enhancement of mixing and shear stress via micromixers may delay or mitigate the onset of localized membrane fouling from biofilms or other contaminants. the impact of micromixers on the overall performance of reverse-osmosis membranes needs further investigation. © 2008 American Institute of Chemical Engineers.

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Basic research is needed to better understand the potential risk of dangerous biological agents that are unintentionally or intentionally introduced into a water distribution system. We report on our capabilities to conduct such studies and our preliminary investigations. In 2004, the Biofilms Laboratory was initiated for the purpose of conducting applied research related to biofilms with a focus on application, application testing and system-scale research. Capabilities within the laboratory are the ability to grow biofilms formed from known bacteria or biofilms from drinking water. Biofilms can be grown quickly in drip-flow reactors or under conditions more analogous to drinking-water distribution systems in annular reactors. Biofilms can be assessed through standard microbiological techniques (i .e, aerobic plate counts) or with various visualization techniques including epifluorescent and confocal laser scanning microscopy and confocal fluorescence hyperspectral imaging with multivariate analysis. We have demonstrated the ability to grow reproducible Pseudomonas fluorescens biofilms in the annular reactor with plate counts on the order of 10{sup 5} and 10{sup 6} CFU/cm{sup 2}. Stationary phase growth is typically reached 5 to 10 days after inoculation. We have also conducted a series of pathogen-introduction experiments, where we have observed that both polystyrene microspheres and Bacillus cereus (as a surrogate for B. anthracis) stay incorporated in the biofilms for the duration of our experiments, which lasted as long as 36 days. These results indicated that biofilms may act as a safe harbor for bio-pathogens in drinking water systems, making it difficult to decontaminate the systems.

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A single-well injection-withdrawal (SWIW) test is evaluated as a tool to differentiate between single- and double-porosity conceptualizations of a system. Results from single-porosity simulations incorporating plume drift are also compared to observed data from a recent series of SWIW tests conducted in a fractured dolomite unit, for which a double-porosity conceptualization has been proposed. We evaluate the difficulty of differentiating the response for a double-porosity conceptualization from that for a heterogeneous, single-porosity conceptualization incorporating plume drift. Results of sensitivity studies on multiple, stochastically generated, heterogeneous transmissivity fields indicate that to simulate extremely slow mass-recovery rates for a SWIW test with a single-porosity conceptualization, the following conditions must be present: plume drift, extreme heterogeneities (high {sigma}InT), and an unusual configuration of the high and low transmissivity regions relative to the well location. A compilation of existing data suggests that the high degree of heterogeneity necessary is rare at the SWIW test scale.The observed data from the SWIW tracer tests cannot be matched to numerical simulation results when a single-porosity conceptualization is assumed. A signature of significant drift is less than 100% mass recovery with a zero derivative with respect to time of the late-time normalized cumulative mass curve indicating mass transported outside the capture zone of the withdrawal well. To minimize the risk of misinterpretation, an important design feature for SWIW tests is the collection of late-time data so that percent total mass recovery can be calculated.

In 1983, high-level radioactive waste repository performance requirements related to groundwater travel time were defined by NRC subsystem regulation 10 CFR 60.113. Although DOE is not presently attempting to demonstrate compliance with that regulation, understanding of the prevalence of fast paths in the groundwater flow system remains a critical element of any safety analyses for a potential repository system at Yucca Mountain, Nevada. Therefore, this analysis was performed to allow comparison of fast-path flow against the criteria set forth in the regulation. Models developed to describe the conditions for initiation, propagation, and sustainability of rapid groundwater movement in both the unsaturated and saturated zones will form part of the technical basis for total- system analyses to assess site viability and site licensability. One of the most significant findings is that the fastest travel times in both unsaturated and saturated zones are in the southern portion of the potential repository, so it is recommended that site characterization studies concentrate on this area. Results support the assumptions regarding the importance of an appropriate conceptual model of groundwater flow and the incorporation of heterogeneous material properties into the analyses. Groundwater travel times are sensitive to variation/uncertainty in hydrologic parameters and in infiltration flux at upper boundary of the problem domain. Simulated travel times are also sensitive to poorly constrained parameters of the interaction between flow in fractures and in the matrix.

Unsaturated flow has been modeled through four cross-sections at Yucca Mountain, Nevada, for the purpose of determining groundwater particle travel times from the potential repository to the water table. This work will be combined with the results of flow modeling in the saturated zone for the purpose of evaluating the suitability of the potential repository under the criteria of 10CFR960. One criterion states, in part, that the groundwater travel time (GWTT) from the repository to the accessible environment must exceed 1,000 years along the fastest path of likely and significant radionuclide travel. Sensitivity analyses have been conducted for one geostatistical realization of one cross-section for the purpose of (1) evaluating the importance of hydrological parameters having some uncertainty and (2) examining conceptual models of flow by altering the numerical implementation of the conceptual model (dual permeability (DK) and the equivalent continuum model (ECM). Results of comparisons of the ECM and DK model are also presented in Ho et al.