Aqueous Chemistry of Metals under Supercritical Water Reactor Coolant Conditions

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This proposal seeks funding for the second phase of a collaborative project that uses state-of-the-art instruments to determine ionization and association constants for simple acids, bases, dissolved metals, and metal complexes under near-critical and super-critical conditions that will be encountered in the proposed Generation IV Super-Critical-Water-cooled nuclear Reactor (SCWR). The instrumental methods include Raman and UV-visible spectroscopy; and visualization techniques; supported by ab initio computations. These are extremely specialized pieces of high-precision equipment, with capabilities shared by few other laboratories in North America, constructed for the specific purpose of making quantitative measurements under SCWR reactor operating conditions. The first phase of the project included the construction of high-pressure cells and instruments for operation in the supercritical region. Theoretical and Raman studies on copper, nickel and cobalt complexes, and conductivity studies on strontium ion pairing up to 350 oC were completed. The second phase will extend these studies to more species, and to temperatures above the critical point (T > 373 oC). Semi empirical equations will be developed to predict the behaviour of these and other aqueous species under the extreme conditions relevant to Gen IV steam generator chemistry. The metals to be studied include Co2+, Ni2+, Cu+, Fe3+, Fe2+, Pb2+ and ZrO2+, along with their reaction products with contaminant species and possible pH control agents.