In-Situ Bioremediation of Organic Compounds: Coupling of Mass-transfer and Biodegradation

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1 HIGHLIGHTS In-Situ Bioremediation of Organic Compounds: Coupling of Mass-transfer and Biodegradation Aqueous Absorption and Kinetics of NO by Strong Oxidizing Agents Surfactant Selection Protocol for Ex-Situ Soil Washing Preconcentration, Speciation and Determination of Dissolved Heavy Metals in Natural Waters, using Ion Exchange and Graphite Furnace Atomic Absorption Spectrometry In-Situ Reductive Dehalogenation of Aliphatic Compounds by Fermentative Heterotrophic Bacteria Removal of Volatile Organic Compounds (VOCs) from Contaminated Groundwater and Soils by Pervaporation Development of Sampling Systems for Continuous Monitoring of Volatile Organic Compounds (VOCs) Determination of Adsorption and Desorption Behavior of Petroleum Products on Soils In-Situ Bioremediation of Organic Compounds: Coupling of Mass-transfer and Biodegradation: Gordon A. Lewandowski, New Jersey Institute of Technology and Edward J. Bouwer Johns Hopkins University A mathematical model was further developed for bioremediation in the saturated zone, which is analogous to a porous catalyst model used in chemical process engineering. The model includes interactions between soil aggregates and groundwater, involving several non-linear, coupled partial differential equations describing biomass growth and decay, sorption, and oxygen availability, as well as pollutant profiles, and the equations were solved numerically. The model is used to determine parameter sensitivity, and uncover physical relationships that might not otherwise be apparent on an intuitive basis. Reliable engineering models can lead to more reliable estimates of cost and treatment times prior to the irreversible commitment of resources, and can also diagnose problems that arise during field tests (thus saving unnecessary expenditure of operating funds). At present, a critical deficiency in existing models is their inability to adequately assess the relative importance of mass transfer (bioavailability) vs. kinetic (biodegradation) effects. Dr. Bouwer has been conducting an ongoing study of the potential for natural and enhanced (engineered) in-situ biotransformation of certain mono- and polycyclic aromatic hydrocarbons at the Baltimore Gas & Electric Co., Spring Gardens Facility, in Baltimore, Maryland. This is the site of a former manufactured gas plant, which is contaminated with coal tars and petroleum hydrocarbons,

2 including: BTXs (benzene, toluene, ethylbenzene, xylenes), and PAHs (naphthalene, acenaphthylene, acenaphthene, fluorene, phenanthrene, anthracene, fluoranthrene, and pyrene). Most of the contamination is contained within two sand and gravel aquifers at the 72 acre site. Aquifer sediments collected from several boreholes across the site contain bacteria capable of aerobically mineralizing the principal aromatic compounds in the groundwater plume (benzene, toluene, naphthalene, and phenanthrene). Laboratory studies were also conducted with composite sediment samples to evaluate the intrinsic biodegradation rates, sorption partition coefficients, and sorption rates for naphthalene and phenanthrene. Laboratory and field data provide insight into the extent of mass transfer control on biodegradation at the site, and are used to calibrate and verify the proposed model. Aqueous Absorption and Kinetics of NO by Strong Oxidizing Agents: Yusuf G. Adewuyi, North Carolina A&T State University and Henry Shaw, New Jersey Institute of Technology The scrubbing technique was recently tested with Air Purification, Inc. (API) Rotorfilter TM technology known for its high efficiency in removing particulates and the results were positive. This initial testing phase with the Rotorfilter TM technology was conducted at the Electric Power Research Institute (EPRI) Environmental Control Technology Center (ECTC) in Barker, New York. The ECTC test on pulverized bituminous coal derived flue gas demonstrated that the Rotorfilter TM system with our chemical systems (NaClO 2 with NaOH and buffers) achieved simultaneous removal efficiencies up to 99% for particulate, 93% for SO 2 and 80% for NO x. For particulate and SO 2 simultaneous removal efficiencies of 99%+ were also achieved. Surfactant Selection Protocol for Ex-Situ Soil Washing: David Sabatini and Jeffrey Harwell, University of Oklahoma Surfactant enhance in situ remediation has progressed from the laboratory to field demonstrations in the past seven years. This has largely been an outgrowth of the inefficiency of water-based pump and treat remediation. A key factor in this development has been identification of surfactants with desirable operating characteristics. Research conducted in this project has built upon this foundation while considering additional factors important to ex situ soil washing. Our results demonstrate that soil washing can be significantly enhanced by surfactant addition, and has helped provide guidance for surfactant selection. This work has also demonstrated that, in certain systems, even low surfactant concentrations (sub-cmc) can achieve dramatic improvements (due to the soil rollup mechanism, which does not function in subsurface systems). The economic advantages are even greater when this approach can be utilized. Thus, it appears that surfactant enhanced soil washing (ex-situ) has the potential to

3 significantly improve soil decontamination. Preconcentration, Speciation and Determination of Dissolved Heavy Metals in Natural Waters, using Ion Exchange and Graphite Furnace Atomic Absorption Spectrometry: Victor Ososkov and Barbara Kebbekus, New Jersey Institute of Technology The techniques of batch ion exchange pre-concentration and direct stabilized slurry GFAAS analysis have been combined and applied to the determination of toxic free metal ions in aqueous samples. These new analytical methods allow the measurement of the concentration of free ions, which have greater biological effects, rather than total concentrations including ions bound to colloidal particles, as other current methods do. It is applicable to the separation of Cr(III) from Cr(VI) and to preconcentration of these or other metal species. A sampling system suitable for carrying out the preconcentration on fine ion exchange beads and separation of the beads from the water in the field has been developed. This minimizes sample preservation and transportation problems. These methods are applicable to the determination of metals in various natural aqueous media, e.g. tapwater, lake and river water, and groundwater. The sorption of metal ions on chelating resins and ion exchange resins allows preconcentration for spectrometric analysis, separation from interfering substances, and straight forward analysis by graphite furnace spectrometry. The methods allow speciation of the metals into dissolved and insoluble species and the dissolved species into complexed and free ions. In-Situ Reductive Dehalogenation of Aliphatic Compounds by Fermentative Heterotrophic Bacteria: David Kafkewitz, Rutgers University and Piero Armenante, New Jersey Institute of Technology Microcosm studies have been performed with soil obtained from an industrial site that had a long history of contamination by tetrachloroethene (PCE) in order to determine the conditions under which biodegradation of PCE or its dehalogenation products i.e., trichloroethene (TCE), dichloroethene (DCE), vinyl chloride (VC), and ethene, can occur. At this site PCE contamination ceased about fifteen years ago and neither PCE nor TCE is currently detectable. However, DCE is present and has not declined in concentration for many years. A number of electron donors were used to stimulate biodegradation, namely ethanol, butanol, acetate and butyrate. These compounds were selected because they are known to be fermentation products. The most striking finding in this study was that none of four potential electron donors tested stimulated significant dehalogenation of the cis 1,2-DCE that was present in the soil unless PCE was added to the microcosms. However, when PCE was added to the soil slurry at the start of incubation, degradation was observed. More significantly, only the microcosms that contained an alcohol

4 (ethanol or butanol) as the electron donor displayed dehalogenation of DCE to ethene. TCE was not detected as an intermediate in the dehalogenation sequence, with the exception of the acetate cultures in which trace amounts of TCE were produced and consumed. Neither VC nor ethane was detected in any cultures. These results indicate that ethanol or butanol, but not acetate or butyrate, support complete dehalogenation in soil samples, but only if additional PCE is added to the microcosms. Since PCE is a common environmental pollutant the causes of incomplete dehalogenation are of considerable practical as well as fundamental interest. This is particularly true for sites in which dehalogenation stops at VC, a compound that is considered to be far more toxic than any of its precursors. These results have implications for in situ remediation projects, in that they suggest that the dehalogenation pathway in some populations is inducible, and that the redox potential of the primary electron donors may determine the population of dehalogenators that is ultimately selected. Removal of Volatile Organic Compounds (VOCs) from Contaminated Groundwater and Soils by Pervaporation: I. Abou-Nemeh, S. Chandra, A. Saraf and K. K. Sirkar, New Jersey Institute of Technology. A new hollow fiber membrane-based pervaporation process has been developed to remove volatile organic compounds (VOCs) from simulated surfactant-flushed groundwater. The basic process parameters such as the temperature, feed flow rate, 1,1,1 trichloroethylene (TCE) and surfactant sodium dodecyl sulfate (SDS) concentrations were subjects of systematic and extensive study. The results of the experimental trials have shown almost complete removal (more than 99.9%) of TCE. Several types of modules of different characteristics were studied in various configurations, such as two or three modules in series, to screen the best performance for this particular system. Finally, a 36-hour run was conducted using a specific feed which contains apart from VOCs, isopropyl alcohol (IPA) and hydrophilic polymer Xanthan gum; the aim was to test the long term performance of the module at various flow rates and feed conditions. The hollow fiber module showed good performance and reproducibility. An additional goal of this project was to demonstrate this technology at a pilot-plant scale using large hollow fiber modules and an actual surfactant-flushed groundwater from a remediation site. The results of the pilot plant runs at RREL, EPA-Cincinnati using surfactant-flushed groundwater from Hill Air Force Base, Utah, have shown an outstanding performance at different feed flow rates and temperature. The results of the pilot plant runs concerning flux of VOCs and their removal on simulated and real feed were identical. Mass transfer coefficients of VOCs were estimated and showed good agreement with the ones obtained on a laboratory scale; using the present data one can predict the performance of a larger scale plant. Development of Sampling Systems for Continuous Monitoring of Volatile Organic Compounds (VOCs): S. Mitra, New Jersey Institute of Technology A very sensitive instrument has been developed that can monitor ppb levels of NMOC with high accuracy and precision. It exhibits a linear calibration curve and is free from interference from moisture, CO2 and CH4. The detection limits were

5 as low as 0.8 ppb. The instrument is being evaluated by monitoring the outlet of a catalytic incinerator. Preliminary studies show promising results. This is the first instrument of its kind, and industry has shown considerable interest in further developing and marketing it. Determination of Adsorption and Desorption Behavior of Petroleum Products on Soils: Charles E. Schaefer, Rolf R. Arands and David S. Kosson, Rutgers, The State University of New Jersey Soil surface area, organic matter content, and contaminant type appeared to be the dominant factors affecting sorption of petroleum contaminants in the presence of a non-aqueous phase liquid (NAPL). Other experiments were carried out to examine the applicability of binary partitioning parameters when applied to a multiphase system. Results indicated that binary parameters (from 2-phase systems) were sufficient to predict equilibrium partitioning of contaminants in multiphase systems. Experiments were carried out to examine diffusion through NAPL and vapor phase in a porous medium with NAPL present. The effective diffusivity was measured as a function of NAPL content, moisture content, and pore size distribution. Mercury intrusion and extrusion experiments were used to estimate pore connectivity at various pore diameters. Results indicated that all three factors were important for soils with a broad pore size distribution and near the NAPL content at which the NAPL first became continuous. These results were combined with a previously developed model to predict the overall diffusional resistance through the NAPL. For diffusion through the vapor phase in the presence of NAPL, results indicated that filling of soil pores by either liquid water or liquid dodecane had a similar effect on gas phase diffusion. A previously developed vapor phase diffusion model was modified to account for total liquid (water and NAPL) relative saturation and compared favorably to experimental data. The diffusion of 14 C-labeled phenanthrene through soil was measured as a function of moisture content, dissolved organic carbon (DOC) concentration, and contaminant contact time with the soil (aging). The DOC concentration of the pore water appeared to be the dominant factor controlling contaminant partitioning and mobility. Results indicated sorption kinetics were faster in pore waters than in adsorption isotherms which were carried out at higher liquid-solid ratios.

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