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Terrestrial fate of coal-liquid constituents: behavior of alkyl anilines in soil

Description: The low molecular weight aromatic amines (anilines) are important water soluble constituents of coal liquids. The impact of anilines released to the terrestrial environment will largely depend on their mobility and persistence. Studies were conducted to investigate those processes governing the mobility and persistence of the alkylanilines, namely, soil sorption and chemical/microbial degradation. Soil sorption measurements were conducted on aniline and several methyl substituted anilines on A and B horizons of a soil profile collected from Davies County, Kentucky. The magnitude of sorption was large in all horizons. Sorption in the B horizons was larger than in the A horizon for many of the anilines studied, indicating the importance of both the mineral matrix and organic carbon content of the soil in determining the magnitude of sorption. Results of these measurements indicate that movement of the anilines through the soil would be significantly attenuated by sorption reactions. Aniline sorption measurement in the A horizon after removal of the organic matter and in the B/sub 22/ horizon after removal of amorphous iron oxides and crystalline iron oxides indicate that organic matter largely controls aniline sorption in the A horizon, while crystalline iron oxides and phyllosilicates are important in the B horizons. The effects of pH on aniline sorption was also examined and shown to have significant effects on the magnitude of sorption in both A and B horizons. Soil degradation studies using /sup 14/C-3-methylaniline as a model for alkyl aniline degradation show that 3-methylaniline is readily metabolized by soil microorganisms during the 32-day period examined.
Date: July 1, 1982
Creator: Felice, L.J.; Zachara, J.M. & Rogers, J.E.
Partner: UNT Libraries Government Documents Department

Chemical contaminants on DOE lands and selection of contaminant mixtures for subsurface science research

Description: This report identifies individual contaminants and contaminant mixtures that have been measured in the ground at 91 waste sites at 18 US Department of Energy (DOE) facilities within the weapons complex. The inventory of chemicals and mixtures was used to identify generic chemical mixtures to be used by DOE`s Subsurface Science Program in basic research on the subsurface geochemical and microbiological behavior of mixed contaminants (DOE 1990a and b). The generic mixtures contain specific radionuclides, metals, organic ligands, organic solvents, fuel hydrocarbons, and polychlorinated biphenyls (PCBs) in various binary and ternary combinations. The mixtures are representative of in-ground contaminant associations at DOE facilities that are likely to exhibit complex geochemical behavior as a result of intercontaminant reactions and/or microbiologic activity stimulated by organic substances. Use of the generic mixtures will focus research on important mixed contaminants that are likely to be long-term problems at DOE sites and that will require cleanup or remediation. The report provides information on the frequency of associations among different chemicals and compound classes at DOE waste sites that require remediation.
Date: April 1, 1992
Creator: Riley, R. G. & Zachara, J. M.
Partner: UNT Libraries Government Documents Department

Metal cation/anion adsorption on calcium carbonate: Implications to metal ion concentrations in groundwater

Description: This chapter evaluates the sorption behavior of metallic ions on specimen calcite as a basis for determining the importance of calcite relative to other subsurface sorbents, such as layer silicates and oxides, in controlling metal ion concentration in calcareous groundwaters. A review of the literature shows the sorption of both metallic cations and anions on calcite over ranges in pH and CO{sub 2} partial pressure to be consistent with a surface-exchange process where cations exchange with surface Ca and anions exchange with surface CO{sub 3}. A general surface-exchange model was developed to account for the effects of Ca and CO{sub 3} concentrations, pH, and calcite surface area on cation and anion sorption onto calcite. The model was applied to recently developed experimental sorption data of Zn and SeO{sub 3} on specimen calcite in equilibrium CaCO{sub 3}(aq) suspensions. The surface-exchange model was able to describe the effects of pH on both cation and anion sorption, and provided good predictions of the effects of variable CO{sub 2}(g) pressure on Zn sorption and of PO{sub 4} on SeO{sub 3} sorption. The surface-exchange model, combined with sorption constants for other phases, was used to calculate Cd sorption to a hypothetical aquifer material containing a mixture of sorbents. The sorbent concentrations were fixed to those expected in groundwater zones. The multi-sorbent calculation documented the importance of calcite as a sorbent for metallic ions in groundwater.93 refs., 18 figs., 5 tabs.
Date: May 1, 1990
Creator: Zachara, J.M.; Cowan, C.E. & Resch, C.T.
Partner: UNT Libraries Government Documents Department

MININR: a geochemical computer program for inclusion in water flow models - an application study

Description: MININR is a reduced form of the computer program MINTEQ which calculates equilibrium precipitation/dissolution of solid phases, aqueous speciation, adsorption, and gas phase equilibrium. The user-oriented features in MINTEQ were removed to reduce the size and increase the computational speed. MININR closely resembles the MINEQL computer program developed by Westall (1976). The main differences between MININR and MINEQL involve modifications to accept an initial starting mass of solid and necessary changes for linking with a water flow model. MININR in combination with a simple water flow model which considers only dilution was applied to a laboratory column packed with retorted oil shale and percolated with distilled water. Experimental and preliminary model simulation results are presented for the constituents K/sup +/, Na/sup +/, SO/sub 4//sup 2 -/, Mg/sup 2 +/, Ca/sup 2 +/, CO/sub 3//sup 2 -/ and pH.
Date: February 1, 1984
Creator: Felmy, A.R.; Reisenauer, A.E.; Zachara, J.M. & Gee, G.W.
Partner: UNT Libraries Government Documents Department

Mineral surface processes responsible for the decreased retardation (or enhanced mobilization) of {sup 137}Cs from HLW tank discharges. 1998 annual progress report

Description: 'Cesium (137) is a major component of high level weapons waste. At Hanford, single shell tanks (SST''s) with high level wastes (HLW) have leaked supernate containing over 10{sup 6} Ci of 137 Cs and other co-contaminants into the vadose zone. In select locations, 137 Cs has migrated further than expected from retardation experiments and performance assessment calculations. Deep 137 Cs migration has been observed beneath the SX tank farm at Hanford with REDOX wastes as the carrier causing regulatory and stakeholder concern. The causes for expedited migration are unclear. This research is investigating how the sorption chemistry of Cs on Hanford vadose zone sediments changes after contact with solutions characteristic of HLW. The central scientific hypothesis is that the high Na concentration of HLW will suppress surface-exchange reactions of Cs, except those to highly-selective frayed edge sites (FES) of the micaceous fraction. The authors further speculate that the concentrations, ion selectivity, and structural aspects of the FES will change after contact with HLW and that these changes will be manifest in the macroscopic sorption behavior of Cs. The authors believe that migration predictions of Cs can be improved substantially if such changes are understood and quantified. The research has three objectives: (1.) identify how the multi-component surface exchange behavior of Cs on Hanford sediments changes after contact with HLW simulants that span a range of relevant chemical (Na, OH, Al, K) and temperature conditions (23-80 C); (2) reconcile changes in sorption chemistry with microscopic and molecular changes in site distribution, chemistry, mineralogy, and surface structure of the micaceous fraction; (3) integrate mass-action-solution exchange measurements with changes in the structure/site distribution of the micaceous fraction to yield a multicomponent exchange model relevant to high ionic strength and hydroxide for prediction of environmental Cs sorption.'
Date: June 1, 1998
Creator: Zachara, J.M.; Ellis, P.D.; Serne, R.J. & Bertsch, P.M.
Partner: UNT Libraries Government Documents Department

Chemical contaminants on DOE lands and selection of contaminant mixtures for subsurface science research

Description: This report identifies individual contaminants and contaminant mixtures that have been measured in the ground at 91 waste sites at 18 US Department of Energy (DOE) facilities within the weapons complex. The inventory of chemicals and mixtures was used to identify generic chemical mixtures to be used by DOE's Subsurface Science Program in basic research on the subsurface geochemical and microbiological behavior of mixed contaminants (DOE 1990a and b). The generic mixtures contain specific radionuclides, metals, organic ligands, organic solvents, fuel hydrocarbons, and polychlorinated biphenyls (PCBs) in various binary and ternary combinations. The mixtures are representative of in-ground contaminant associations at DOE facilities that are likely to exhibit complex geochemical behavior as a result of intercontaminant reactions and/or microbiologic activity stimulated by organic substances. Use of the generic mixtures will focus research on important mixed contaminants that are likely to be long-term problems at DOE sites and that will require cleanup or remediation. The report provides information on the frequency of associations among different chemicals and compound classes at DOE waste sites that require remediation.
Date: April 1, 1992
Creator: Riley, R.G. & Zachara, J.M. (Pacific Northwest Lab., Richland, WA (United States))
Partner: UNT Libraries Government Documents Department

The sorption of humic acids to mineral surfaces and their roles in contaminant binding

Description: Humic substances dissolved in groundwater may adsorb to certain mineral surfaces, rendering hydrophilic surfaces hydrophobic and making them sorbents for hydrophobic organic compounds (HOC). The sorption of humic and fulvic acids (International Humic Substance Society, IHSS, reference samples) on hematite and kaolinite was investigated to determine how natural organic coatings influence HOC sorption. The sorption behavior of the humic substances was consistent with a ligand-exchange mechanism, and the amount of sorption depended on the concentration of hydroxylated surface sites on the mineral and the properties of the humic substance. The sorption of the humic substances to two solids was proportional to their aromatic carbon content and inversely proportional to the O/C ratio. Increasing quantities of sorbed humic substances (f{sub oc}0.01 to 0. 5%) increased the sorption of carbazole, dibenzothiophene, and anthracene. Peat humic acid, the most aromatic coating, showed the greatest sorption enhancement of HOC when sorbed to hematite. In addition, HOC sorption was greater on organic coating formed at low ionic strength (I = 0.005) as compared to higher ionic strength (I = 0.1). We suggest that both the mineral surface and the ionic strength of the electrolyte affect the interfacial configuration of the sorbed humic substance, altering the size or accessibly of hydrophobic domains on the humic molecule to HOC. 30 refs., 5 figs.
Date: November 1, 1990
Creator: Murphy, E.M.; Zachara, J.M.; Smith, S.C. & Phillips, J.L.
Partner: UNT Libraries Government Documents Department

KEMOD: A mixed chemical kinetic and equilibrium model of aqueous and solid phase geochemical reactions

Description: This report presents the development of a mixed chemical Kinetic and Equilibrium MODel in which every chemical species can be treated either as a equilibrium-controlled or as a kinetically controlled reaction. The reaction processes include aqueous complexation, adsorption/desorption, ion exchange, precipitation/dissolution, oxidation/reduction, and acid/base reactions. Further development and modification of KEMOD can be made in: (1) inclusion of species switching solution algorithms, (2) incorporation of the effect of temperature and pressure on equilibrium and rate constants, and (3) extension to high ionic strength.
Date: January 1, 1995
Creator: Yeh, G. T.; Iskra, G. A.; Szecsody, J. E.; Zachara, J. M. & Streile, G. P.
Partner: UNT Libraries Government Documents Department

HYDROBIOGEOCHEM: A coupled model of HYDROlogic transport and mixed BIOGEOCHEMical kinetic/equilibrium reactions in saturated-unsaturated media

Description: The computer program HYDROBIOGEOCHEM is a coupled model of HYDROlogic transport and BIOGEOCHEMical kinetic and/or equilibrium reactions in saturated/unsaturated media. HYDROBIOGEOCHEM iteratively solves the two-dimensional transport equations and the ordinary differential and algebraic equations of mixed biogeochemical reactions. The transport equations are solved for all aqueous chemical components and kinetically controlled aqueous species. HYDROBIOGEOCHEM is designed for generic application to reactive transport problems affected by both microbiological and geochemical reactions in subsurface media. Input to the program includes the geometry of the system, the spatial distribution of finite elements and nodes, the properties of the media, the potential chemical and microbial reactions, and the initial and boundary conditions. Output includes the spatial distribution of chemical and microbial concentrations as a function of time and space, and the chemical speciation at user-specified nodes.
Date: July 1, 1998
Creator: Yeh, G.T.; Salvage, K.M.; Gwo, J.P.; Zachara, J.M. & Szecsody, J.E.
Partner: UNT Libraries Government Documents Department

Migration of radionuclides in geologic media: Fundamental research needs

Description: An assessment of the fundamental research needs in understanding and predicting the migration of radionuclides in the subsurface is provided. Emphasis is on the following three technical areas: (1) aqueous speciation of radionuclides, (2) the interaction of radionuclides with substrates, and (3) intermediate-scale interaction studies. This research relates to important issues associated with environmental restoration and remediation of DOE sites contaminated with mixed radionuclide-organic wastes. 64 refs., 1 fig., 1 tab.
Date: January 1, 1990
Creator: Reed, D.T. (Argonne National Lab., IL (USA)); Zachara, J.M.; Wildung, R.E. (Pacific Northwest Lab., Richland, WA (USA)) & Wobber, F.J. (USDOE, Washington, DC (USA))
Partner: UNT Libraries Government Documents Department