Albitization related U and Th mobilization under reducing conditions

Abstract

Hydrothermally altered quartzofeldspathic gneisses, granites and pegmatites of the West Garo Hills, Shillong Plateau (eastern India) preserve alteration assemblages of monazite, xenotime and zircon comprising thorite and coffinite in the altered domains. Albitization of muscovite and K-feldspars, sericitization of K-feldspar and albite, alteration of biotite to hydrobiotite, and crystallization of tourmaline is suggestive of the involvement of acidic fluids. The microtextural relations and the mineral assemblages indicate prevalence of low-temperature (T < 300 °C) conditions during hydrothermal alteration. The light δ¹¹B values of tourmaline (–15.1 to –13.5 ‰) suggests derivation/interaction of the fluids from/with metapelitic rock and/or S-type granite. Low ‘inferred’ Fe³⁺/Fe²⁺ ratio in tourmaline (based on high Al content in Y-site, 0.16–0.56 apfu, avg. 0.36 apfu), estimated excess charge (0.22–0.47, avg. 0.35 apfu) and lack of any Fe–Al relation support a reduced nature of the hydrothermal fluid. Mass balance calculations reveal that Th and U required for the formation of thorite and coffinite, respectively were likely derived from monazite and xenotime, and zircon. Significantly lower Cl^─ contents in hydrobiotite (avg. 0.03 wt%) compared to the unaltered biotite (avg. 0.13 wt%) suggests release of Cl^─ to the hydrothermal fluid during alteration. Textural evidences of albitization together with Cl^─ release from biotite suggest increased Cl^─ concentrations in the fluid during hydrothermal alteration. Based on solubility calculations for various U and Th species, we propose that high Cl^─ content in the fluid aided mobilization of Th and U as ThCl₄⁰ and UCl₄⁰/UO₂Cl₂⁰ complexes from accessory radioactive phases under reducing conditions. These results suggest that significant mobility of U and Th can be achieved in acidic high salinity fluid even under reducing conditions. Thermodynamic calculations for the solubility of Th- and U-chloride complexes and stability of monazite/xenotime in a range of pH and temperature suggest that thorite and coffinite precipitation was the result of an increase in pH.