The high primary porosity and permeability of eogenetic karst aquifers permit water recharged through secondary dissolution features to be temporarily stored in aquifer matrix porosity. The recharged water contains elevated dissolved organic carbon (DOC) concentrations that, when oxidized, enhance limestone dissolution and impact carbon cycling. We evaluate the relationship between DOC oxidation and limestone dissolution using observations at a stream sink‐rise system and reversing spring in the Floridan aquifer, north‐central Florida, USA, where subsurface residence times of recharged water are days and months, respectively. We estimate water chemical compositions during surface water‐groundwater interactions at these two systems with mixing models of surface water and groundwater compositions and compare them with measured DOC, dissolved inorganic carbon (DIC), Ca2+and dissolved organic nitrogen (DON) concentrations. Differences between measured and modelled concentrations represent net changes that can be attributed to calcite dissolution and redox reactions, including DOC oxidation. DOC losses and Ca2+gains exhibit significant (p < 0.01) inverse linear correlations at both the reversing spring (slope = −0.9, r2 = 0.99) and the sink‐rise system (slope = −0.4, r2 = 0.72). DOC oxidation in both systems was associated with decreases in the molar C:N ratio (DOC:DON). Significant (p < 0.01) positive linear correlations between increases in Ca2+and DIC concentrations after correcting for DIC derived from calcite dissolution occurred at both the reversing spring (slope = 1.3, r2 = 0.99) and the sink‐rise system (slope = 1.61, r2 = 0.75). Greater deviations from the expected slope of −1 or +1 at the sink‐rise system than at the reversing spring indicate DOC oxidation contributes less dissolution at the sink‐rise system than at the reversing spring, likely from shorter storage in the subsurface. A portion of the deviation from expected slope values can be explained by the dissolution of Mg‐rich carbonate or dolomite rather than pure calcite dissolution. Despite this, slope values reflect kinetic effects controlling incomplete consumption of carbonic acid during dissolution reactions.
Groundwater aquifers are an essential source of drinking water, and must be protected against contamination. Phosphogypsum stacks originating from the processing of phosphate rock contain small amounts of radionuclides, such as226Ra. In September 2016, a sinkhole located beneath a phosphogypsum stack collapsed under central Florida’s carbonate karst terrain, where the aquifer is mostly confined, raising concern over water quality in the regions nearby. Monitoring and modeling the transport of the contaminated plume is vital to ensure drinking water criteria are met and to improve decision making regarding treatment. To achieve this, a geochemical modeling using PHREEQC software was employed to investigate the trajectory of the plume based on hydraulic and hydrologic conditions. Adsorption was simulated as a removal mechanism that could further reduce the intensity of the plume. The aquifer’s response to the release of contaminated water from the collapsed stack was quantified by simulating a number of scenarios, including variable radionuclide leakage quantities. Results suggest that it may take between 11–17 years and between 5.2 to 8.3 km from the sinkhole leak to reduce radionuclide concentrations to previous levels. Coupling the adsorption effect by minerals in Floridan aquifer (e.g. ferrihydrite, carbonate) can reduce radionuclide migration time to 9–16 years and distances between 4.3 to 7.8 km from the sinkhole leak. It can also reduce the distance needed to lower radionuclide concentrations, though not significantly. Additionally, due to the complexities of soil chemistry, the importance of groundwater remediation is emphasized.
more » « less- Award ID(s):
- 1665343
- NSF-PAR ID:
- 10154338
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Scientific Reports
- Volume:
- 8
- Issue:
- 1
- ISSN:
- 2045-2322
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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