Plutonium / ModelingSummary The solubility of Pu(OH) 3 is determined in deionized water and in chloride brines that contained Fe powder to maintain Pu in the Pu(III) oxidation state. The presence of aqueous Pu(III) was verified experimentally. The solubility of Pu(OH) 3 is several orders of magnitude greater in brines than in deionized water at the same hydrogen ion concentration. The logarithm of the equilibrium constant, extrapolated to zero ionic strength from experiments in deionized water, for the reaction Pu(OH) 3 Pu 3 + + 3 OH" is determined to be -26.2 ± 0.8. The data for solubility in brines are interpreted in terms of the ion-interaction model of Pitzer and coworkers for the excess solution free energy. These solubility data can be explained to within experimental error by a relatively simple ion-interaction model that includes only binary interactions between Pu 3+ and Cl~. Ion pairs or ternary interaction parameters for Pu 3+ were not required in order to predict the solubility of Pu(OH) 3 in natural chloridedominated brines at -log[H + ] values of <9, where brackets represent concentration.
Microorganisms present in deep Atlantic coastal plain sediments affect the geochemical evolution of groundwater and its chemical and isotopic composition, yet the factors controlling their origin, distribution, and diversity are poorly understood. The evolution of the groundwater chemistry, the fractionation of stable carbon isotopes, and the groundwater age are all indicators of the inorganic and microbial reactions occurring along a given flow path from groundwater recharge to groundwater discharge. In this study, tritium, 14C, and groundwater chemistry along three flow paths of the Middendoff aquifer in South Carolina were analyzed. The !4C ranged from 89 percent modern carbon (pmC) in the recharge zone to 9.9 pmC in the distal borehole; the/•3C remained relatively constant at ----22%•, suggesting microbial oxidation of organic carbon. Carbon isotope analyses of particulate organic carbon from core sediments and groundwater chemistry were used to model the carbon chemistry; the groundwater ages obtained from •4C ranged from modem to 11,500 years B.P. The highest frequencies of occurrence, numbers, and diversity of aerobic and anaerobic bacteria were found in boreholes near the recharge zone where the calculated ages were <1000 years B.P. The transport of microorganisms from the recharge zone may be responsible for this distribution as well as the electron acceptors necessary to support this diverse community of bacteria. The presence of both aerobic heterotrophs and anaerobic sulfate-and iron-reducing bacteria in the core sediments suggested the occurrence of anaerobic microsites throughout this otherwise aerobic aquifer. The highest in situ microbial respiration rate, as determined by modeling, was found along a flow path near the recharge area. It is likely that the electron acceptors necessary for supporting a diverse microbial community are depleted by the time the groundwater residence time in the Middendoff aquifer exceeds several hundred years. INTRODUCTION Abundant and diverse populations of microorganisms were found at depths of over 400 m in Atlantic coastal plain sediments at and near the U.S. Department of Energy's (DOE's) Savannah River Site (SRS) in South Carolina [Balkwill, 1989; Fredrickson .et al., 1989; Jones et al., 1989]. These microorganisms are capable of affecting both the chemical and isotopic composition of groundwater and its geochemical evolution [Chapelle et al., 1987, 1988; Murphy et al., 1989; Plumruer et al., 1990; Chapelle and Lovley, 1990a; McMahon et al., 1990; Lovley et al., 1990a; McMahon and ½hapelle, 1991]. The complex interaction between microorganisms and organic carbon in the subsurface is perhaps most evident when the inorganic and isotopic chemistry of groundwater are modeled along a flow path from groundwater recharge to groundwater discharge. Reaction-path modeling of the chemical evolution and the change in stable isotopes along a flow path requires an understanding of the role of aerobic and anaerobic microorganisms in the carbon cycle and the nature of particulat...
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