Near-field high temperature transport: evidence from the genesis of the Osamu Utsumi uranium mine, Poços de Caldas alkaline complex, Brazil

Abstract

The chemical, isotopic and mineralogical alteration which occurred during primary uranium ore deposition at the breccia pipe-hosted Osamu Utsumi mine, Poços de Caldas, Brazil was studied as a natural analogue for near field radionuclide migration. Chemical and isotopic alteration models were combined with finite difference models of the convective cooling of caldera intrusives. The modeling indicates that the intense chemical, isotopic, and mineralogical alteration of the Osamu Utsumi breccia pipe requires the circulation of > 10 5 kg/cm 2 of boiling hydrothermal fluid > 200°C through each square centimeter cross-section of the pipe. This circulation could be driven by heat from a 6 km diameter intrusive extending to 10 km depth. Even with this large amount of circulation concentrated in the permeable breccia pipe, uranium solubilities must be 2 1 2 orders of magnitude greater than indicated in the most recent experiments (and more in line with previous estimates) to produce the primary uranium mineralization at the Osamu Utsumi mine. The same models applied to a hypothetical high temperature waste repository show that heat from radioactive decay will produce a hydrothermal circulation system remarkably similar to that studied at the natural analogue site at Poços de Caldas. The depth of fluid convection induced by the hypothetical repository would be 5 to 10 km, the maximum temperature would be ∼ 300°C, the lifetime of the high temperature phase would be a few thousand years, and boiling would occur and cause most of the alteration within the hypothetical waste repository. This physical analysis emphasizes the importance of permeability on a 10 × 10 × 10 km scale in controlling the potential amount of circulation through the hypothetical repository. Application of the chemical models successfully used to interpret mineralization and alteration at the Poços de Caldas Osamu Utsumi mine to the hypothetical waste repository shows that even in a worst case scenario (waste implaced in a permeable host rock with no measures taken to inhibit flow though the repository) the amount of hydrothermal alteration in the hypothetical repository will be ∼ 0.1% of that in the breccia pipe at Osamu Utsumi. Assuming no barriers to uranium mobility, uranium precipitation above the hypothetical repository would be 0.04 ppm (rather than 40 ppm), hydrothermal alteration 0.03 wt% (rather than 30 wt%), etc. Our analysis indicates that modeled mineralogical alteration is sensitive to the thermodynamic data base used. Prediction of mineralogical alteration (which may be necessary to predict the migration of radionuclides other than uranium, for example) probably cannot be based directly on even very carefully collected laboratory thermodynamic data. Mineralogical complexities of the system, as well as data base uncertainties will require calibration of the thermodynamic framework against mineralogical alteration observed in the laboratory or field.