Uranium (U) contamination
in groundwater from geogenic sources
affects water quality globally. Here, we use a multifaceted isotopic
and geochemical approach to elucidate U sources and controls on geogenic
U release to groundwater and surface water at a prospective subarctic
gold deposit in Yukon, Canada, that is characterized by permafrost,
fractured bedrock, and cold (<2 °C) groundwater. X-ray absorption
spectroscopy, sequential extractions, and micro X-ray fluorescence
mapping show extensive subsurface oxidation and solid-phase U present
in its hexavalent and mobile form. Limited 238U/235U isotope fractionation and predominance of U(VI) in rocks suggest
U(VI) sorption–desorption is the main driver of U mobilization.
Groundwater U concentrations are appreciable (median 38 μg/L,
range 1.2–535 μg/L) and are explained by high-alkalinity,
Ca-rich groundwater produced from oxidative weathering of sulfide
and carbonate-mineralized structures around the deposit. Minor 238U/235U isotope fractionation in groundwater indicates
that limited U(VI) reduction occurs beneath permafrost despite groundwater
redox conditions below Fe(III) and S(VI) reduction, and groundwater
ages inferred from 3H and 14C to be on the order
of thousands of years. The complexation of U as uranyl–calcium–carbonate
complexes and the resilience of these complexes to U(VI) reduction
contributes to high U(VI) mobility under cold groundwater conditions.
This study provides insight into processes and time scales of U transport
in subarctic groundwater at a pivotal time when hydrogeochemical changes
may be anticipated in cold regions worldwide due to permafrost degradation.