Influence of Carbonate on Uranium Solubility in the WIPP

Abstract

ABSTRACTIn the performance assessment (PA) for the Waste Isolation Pilot Plant (WIPP), the solubility of uranium (VI) was conservatively set at 10-3 M for all expected WIPP conditions, including the potential and likely effects of carbonate complexation [1]. Under WIPP-relevant conditions, long-term experiments were performed to establish the uranium (VI) solubility limits in WIPP-simulated brine over a broad range of pCH+ values [7.5-12.5] and to evaluate the contribution of carbonate complexation and hydrolysis to uranium (VI) speciation. Data obtained in carbonate-free ERDA-6 brine, a simulated WIPP brine, were reported earlier [2]. In the absence of carbonate, uranium solubility approached 10-7 M at the expected pCH+ in the WIPP (~ 9.5). In the presence of a significant amount of carbonate (millimole levels), recent experimental results showed that uranium (VI) concentrations will not exceed 10-4M. This measured solubility limit is an order of magnitude lower than the uranium solubility value currently used in the WIPP PA [3]. A small effect of borate complexation was found in the pCH+ range [7.5-10]. At pCH+ ≥ 10, hydrolysis overwhelmed carbonate effects, and no amphoteric effect was observed.