Solution Chemistry for Actinide Borate Species to High Ionic Strengths: Equilibrium Constants for AmHB4O72+ And AmB9O13(OH)4(cr) and Their Importance to Nuclear Waste Management

Abstract

ABSTRACTBorate is present in natural groundwaters and borate is also released into groundwaters when borosilicate glass, waste form for high level nuclear waste, is corroded. Borate can form an aqueous complex, AmHB4O72+, with actinides in +III oxidation state. In this work, we present our evaluation of the equilibrium constant for formation of AmHB4O72+ and the associated Pitzer interaction parameters at 25°C.Using Nd(III) as an analog to Am(III), solubility data of Nd(OH)3(s) in NaCl solutions in the presence of borate ion from the literature, is used to determine Am(III) interactions with borate. The log10K for the formation reaction is 37.34. This evaluation is in accordance with the Waste Isolation Pilot Plant (WIPP) thermodynamic model in which the borate species include B(OH)3(aq), B(OH)4–, B3O3(OH)4–, B4O5(OH)42–, and NaB(OH)4(aq). The WIPP thermodynamic database uses the Pitzer model to calculate activity coefficients of aqueous species.In addition, the equilibrium constant for dissolution of AmB9O13(OH)4(cr) at 25oC is evaluated from the solubility data on NdB9O13(OH)4(cr) in NaCl solutions, again using Nd(III) as an analog to Am(III). The log10K for the dissolution reaction is –79.30. In the evaluation for log10K for the dissolution reaction, AmHB4O72+ is also considered.The equilibrium constant and Pitzer parameters evaluated by this study will be important to describe the chemical behavior of Am(III) in the presence of borate in geological repositories.