The Effect of the CO32- to Ca2+ Ion activity ratio on calcite precipitation kinetics and Sr2+ partitioning
Engineering the precipitation of calcium carbonate, which can co-precipitate trace metal contaminants, is a proposed strategy for remediating toxic or radioactive metals in subsurface environments. Engineering precipitation of multi-component minerals will involve injection of chemical amendments that must be mixed at a molecular level to supersaturated conditions that are sufficient to promote rapid mineral precipitation relative to natural systems. In subsurface systems this often means reactant mixing zones will be formed that are characterized by gradients in solute concentrations, saturation state, and solute activity ratios. To better understand the effect of ion activity ratios on CaCO{sub 3} precipitation kinetics and Sr{sup 2+} co-precipitation we experiments were conducted under constant composition conditions where the supersaturation state ({Omega}) with respect to calcite was held constant at 9.4, but the ion activity ratio (r = a{sub co{sub 3}{sup 2-}}/a{sub Ca{sup 2+}}) ranged from 0.003 to 4.15. Results: Under the chosen experimental conditions the CaCO{sub 3} phase formed was calcite and initial precipitation rates varied from a maximum rate of 84.7 {mu}mol/ m{sup 2}/min for a carbonate to calcium activity ratio of (0.21). However, precipitation rates were found to vary with time which could be indicative of variations in precipitation mechanisms that are related to the ion activity ratio. The observed trends in the distribution coefficients for co-precipitated Sr2+ (D{sup P}{sub Sr}{sup 2+}) relative to the calcite precipitation rate (i.e. a positive correlation) indicate that increasing calcite precipitation rates increase the incorporation of Sr{sup 2+}. Conclusion: The observed variation between the rate maxima and minima based on the ion activity ratio could have great deal of implication for sequestering radionuclides (e.g. {sup 90}Sr) and other toxic metals in engineered systems at contaminated sites. Extending our data plot range allowed us to have clues about the differences in mechanism calcite precipitation, which would have significance in our understanding of mineral precipitation modes in subsurface remediation strategies. The positive correlation between D{sup P}{sub Sr}{sup 2+} and calcite precipitation rate could be indicative of the impact calcite precipitation would have on sequestering toxic metals in subsurface environment.
- Research Organization:
- Idaho National Lab. (INL), Idaho Falls, ID (United States)
- Sponsoring Organization:
- DOE - SC
- DOE Contract Number:
- DE-AC07-05ID14517
- OSTI ID:
- 1039342
- Report Number(s):
- INL/JOU-11-22513; TRN: US201209%%385
- Journal Information:
- Geochemical Transactions, Vol. 13, Issue 1; ISSN 1467-4866
- Country of Publication:
- United States
- Language:
- English
Similar Records
in situ Calcite Precipitation for Contaminant Immobilization
CaCO3 Precipitation, Transport and Sensing in Porous Media with In Situ Generation of Reactants