Abstract
The anoxic corrosion of carbon steel liners to produce Fe 2+ and H 2 within copper nuclear waste containers could lead to the scavenging of the radiolytic oxidants (H 2O 2, O 2) required to drive nuclear fuel (UO 2) corrosion and the release of radionuclides. Steel corrosion has been studied in solutions containing various concentrations of Na 2CO 3/NaHCO 3, Na 2SO 4 and NaCl to simulate an anticipated change in environment from carbonate-dominated to chloride-dominated groundwater composition over time. A combination of electrochemical techniques, scanning electron microscopy, and in situ Raman spectroscopy has been used. In concentrated carbonate solutions, corrosion is maintained within pores in a siderite (FeCO 3·H 2O) deposit by the complexation of Fe 2+ by HCO 3 − and the reduction of protons supplied by HCO 3 − dissociation. In mixed-anion solutions at lower CO 3 2−/HCO 3 − concentrations, a compact green rust deposit covers the surface and the corrosion rate is suppressed. In concentrated NaCl solutions, the absence of CO 3 2−/HCO 3 − buffering leads to a rapid shut down of the corrosion process which may be aided by the formation of Fe III surface phases if traces of dissolved O 2 are available.
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