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Abiotic degradation rates for carbon tetrachloride and chloroform: Final report.

Description: This report documents the objectives, technical approach, and progress made through FY 2012 on a project initiated in FY 2006 to help address uncertainties related to the rates of hydrolysis in groundwater for carbon tetrachloride (CT) and chloroform (CF). The project also sought to explore the possible effects of contact with minerals and sediment (i.e., heterogeneous hydrolysis) on these rates. We conducted 114 hydrolysis rate experiments in sealed vessels across a temperature range of 20-93 °C for periods as long as 6 years, and used the Arrhenius equation to estimate activation energies and calculate half-lives for typical Hanford groundwater conditions (temperature of 16 °C and pH of 7.75). We calculated a half-life of 630 years for hydrolysis for CT under these conditions and found that CT hydrolysis was unaffected by contact with sterilized, oxidized minerals or Hanford sediment within the sensitivity of our experiments. In contrast to CT, hydrolysis of CF was generally slower and very sensitive to pH due to the presence of both neutral and base-catalyzed hydrolysis pathways. We calculated a half-life of 3400 years for hydrolysis of CF in homogeneous solution at 16 °C and pH 7.75. Experiments in suspensions of Hanford sediment or smectite, the dominant clay mineral in Hanford sediment, equilibrated to an initial pH of 7.2, yielded calculated half-lives of 1700 years and 190 years, respectively, at 16 °C. Experiments with three other mineral phases at the same pH (muscovite mica, albite feldspar, and kaolinite) showed no change from the homogeneous solution results (i.e., a half-life of 3400 years). The strong influence of Hanford sediment on CF hydrolysis was attributed to the presence of smectite and its ability to adsorb protons, thereby buffering the solution pH at a higher level than would otherwise occur. The project also determined liquid-vapor partition coefficients for CT under ...
Date: December 1, 2012
Creator: Amonette, James E.; Jeffers, Peter M.; Qafoku, Odeta; Russell, Colleen K.; Humphrys, Daniel R.; Wietsma, Thomas W. et al.
Partner: UNT Libraries Government Documents Department

Abiotic Degradation Rates for Carbon Tetrachloride and Chloroform: Progress in FY 2010

Description: This report documents the progress made through FY 2010 on a project initiated in FY 2006 to help address uncertainties related to the rates of hydrolysis in groundwater at the Hanford Site for carbon tetrachloride (CT) and chloroform (CF). The study also explores the possible effects of contact with minerals and sediment (i.e., heterogeneous hydrolysis) on these rates. The research was initiated to decrease the uncertainties in abiotic degradation rates of CT and chloroform CF associated with temperature and possible heterogeneous effects. After 2 years of data collection, the first evidence for heterogeneous effects was identified for hydrolysis of CT, and preliminary evidence for the effects of different mineral types on CF hydrolysis rates also was reported. The CT data showed no difference among mineral types, whereas significant differences were seen in the CF results, perhaps due to the fact that CF hydrolyzes by both neutral and base-catalyzed mechanisms whereas CT follows only the neutral hydrolysis path. In this report, we review the project objectives, organization, and technical approaches taken, update the status and results of the hydrolysis-rate experiments after 4 years of experimentation (i.e., through FY 2010), and provide a brief discussion of how these results add to scientific understanding of the behavior of the CT/CF plume at the Hanford Site.
Date: December 8, 2010
Creator: Amonette, James E.; Jeffers, Peter M.; Qafoku, Odeta; Russell, Colleen K.; Humphrys, Daniel R.; Wietsma, Thomas W. et al.
Partner: UNT Libraries Government Documents Department