The coprecipitation of Sr into calcite precipitates induced by bacterial ureolysis in artificial groundwater: Temperature and kinetic dependence

摘要

A suite of experiments was performed to investigate the partitioning of Sr2+ (to mimic the radionuclide Sr-90) between calcite and artificial groundwater in response to the hydrolysis of urea (ureolysis) by Bacillus pasteurii under simulated in situ aquifer conditions. Experiments were performed at 10, 15, and 20 degrees C over 7 days in microcosms inoculated with B. pasteurii ATCC 11859, containing an artificial groundwater and urea (AGW) or an AGW including a Sr contaminant treatment. During the experiments, the concentration of ammonium generated by bacterial ureolysis increased asymptotically, and derived rate constants (k(urea)) that were between 13 and 10 times greater at 20 degrees C than at 15 and 10 degrees C. Calcite precipitation was initiated after similar amounts of urea had been hydrolyzed (similar to 4.0 mmol L-1) and a similar critical saturation state (mean S-critical = 53, variation 20%) had been reached, independent of temperature and Sr treatment. Because of the positive relationship between the rate of ureolysis and temperature, precipitation began by the end of day 1 at 20 degrees C, and between days 1 and 2 at 15 and 10 degrees C. The rate of calcite precipitation increased with, and was fundamentally controlled by calcite saturation state (S), irrespective of temperature. The presence of Sr slightly slowed calcite precipitation rates at equivalent values of S, which may reflect the screening of active nucleation and crystal growth sites by Sr. Homogeneous partitioning coefficients (D-Sr) exhibited a positive association with calcite precipitation rates, but were greater at higher experimental temperatures at equivalent precipitation rates (20 degrees C mean = 0,46; 15 degrees C mean = 0.24; 10 degrees C mean = 0.29). Copyright (c) 2005 Elsevier Ltd.