Several Fe-based amorphous metal formulations have been identified that appear to have corrosion resistance comparable to (or better than) that of Ni-based Alloy C-22 (UNS No. N06022), based on measurements of breakdown potential and corrosion rate in seawater. Both chromium (Cr) and molybdenum (Mo) provide corrosion resistance, boron (B) enables glass formation, and rare earths such as yttrium (Y) lower critical cooling rate (CCR). SAM2X5 (Fe{sub 49.7}Cr{sub 17.7}Mn{sub 1.9}Mo{sub 7.4}W{sub 1.6}B{sub 15.2}C{sub 3.8}Si{sub 2.4}) has no yttrium, and is characterized by relatively high critical cooling rates of approximately 600 Kelvin per second. Data for the SAM2X5 formulation is reported here. In contrast to yttrium-containing iron-based amorphous metals, SAM2X5 can be readily gas atomized to produce spherical powders which enable more facile thermal spray deposition. The reference material, nickel-based Alloy C-22, is an outstanding corrosion-resistant engineering material. Even so, crevice corrosion has been observed with C-22 in hot sodium chloride environments without buffer or inhibitor. SAM2X5 also experiences crevice corrosion under sufficiently harsh conditions. Both Alloy C-22 and Type 316L stainless lose their resistance to corrosion during thermal spraying, due to the formation of deleterious intermetallic phases which depletes the matrix of key alloy elements, whereas SAM2X5 can be applied as coatings with the same corrosion resistance as a fully-dense completely amorphous melt-spun ribbon, provided that its amorphous nature is preserved during thermal spraying. The hardness of Type 316L Stainless Steel is approximately 150 VHN, that of Alloy C-22 is approximately 250 VHN, and that of HVOF SAM2X5 ranges from 1100-1300 VHN [MRS12-13]. Such hardness makes these materials particularly attractive for applications where corrosion-erosion and wear are also issues. Since SAM2X5 has high boron content, it can absorb neutrons efficiently, and may therefore find useful applications as a criticality control material within the nuclear industry.

The passive film stability of several Fe-based amorphous metal formulations have been found to be comparable to that of stainless steels and Ni-based Alloy C-22 (UNS No. N06022), based on electrochemical measurements of the passive film breakdown potential and general corrosion rates. Electrochemical studies of the passive film stability of SAM1651 are reported here. Chromium (Cr), molybdenum (Mo) and tungsten (W) provide corrosion resistance; boron (B) enables glass formation; and rare earths such as yttrium (Y) lower critical cooling rate (CCR). Yttrium-containing SAM1651, also known as SAM7 (Fe{sub 48.0}Cr{sub 15.0}Mo{sub 14.0}B{sub 6.0}C{sub 15.0}Y{sub 2.0}), has a critical cooling rate (CCR) of approximately 80 Kelvin per second, while yttrium-free SAM2X5 (Fe{sub 49.7}Cr{sub 17.7}Mn{sub 1.9}Mo{sub 7.4}W{sub 1.6}B{sub 15.2}C{sub 3.8}Si{sub 2.4}) has a higher critical cooling rate of approximately 600 Kelvin per second. SAM1651's low CCR enables it to be rendered as a completely amorphous material in practical materials processes. While the yttrium enables a low CCR to be achieved, it makes the material relatively difficult to atomize, due to increases in melt viscosity. Consequently, the powders have irregular shape, which makes pneumatic conveyance during thermal spray deposition difficult. The reference material, nickel-based Alloy C-22, is an outstanding corrosion-resistant engineering material. Even so, crevice corrosion has been observed with C-22 in hot sodium chloride environments without buffer or inhibitor. SAM1651 may also experience crevice corrosion under sufficiently harsh conditions. Both Alloy C-22 and Type 316L stainless lose their resistance to corrosion during thermal spraying, due to the formation of deleterious intermetallic phases which depletes the matrix of key alloy elements, whereas SAM1651 can be applied as coatings with the same corrosion resistance as a fully-dense completely amorphous melt-spun ribbon, provided that its amorphous nature is preserved during thermal spraying. Materials synthesis and characterization is discussed. Data showing the corrosion resistance of SAM1651 in hot concentrated calcium chloride, as well as natural seawater are presented, and compared to a number of reference materials.

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In these experiments we studied the behavior of a synthetic concentrated J13 solution as it comes in contact with a Ni-Cr-Mo-alloy selected for waste canisters in the designated high-level nuclear-waste repository at Yucca Mountain, Nevada. Concentrated synthetic J13 solution was allowed to drip slowly onto heated test specimens (90 C, 60% relative humidity) where the water moved down the surface of the specimens, evaporated and minerals precipitated. Mineral separation or zoning along the evaporation path was not observed. We infer from solid analyses and geochemical modeling, that the most corrosive components (Ca, Mg, and F) are limited by mineral precipitation. Minerals identified by x-ray diffraction include thermonatrite, natrite, and trona, all sodium carbonate minerals, as well as kogarkoite (Na{sub 3}SO{sub 4}F), halite (NaCl), and niter (KNO{sub 3}). Calcite and a magnesium silicate precipitation are based on chemical analyses of the solids and geochemical modeling. The most significant finding of this study is that sulfate and fluoride concentrations are controlled by the solubility of kogarkoite. Kogarkoite thermodynamic data are needed in the Yucca Mountain Project database to predict the corrosiveness of carbonate brines and to establish the extent to which fluoride is removed from the brines as a solid.

Yttrium-containing SAM1651 (Fe{sub 48.0}Cr{sub 15.0}Mo{sub 14.0}B{sub 6.0}C{sub 15.0}Y{sub 2.0}), has a critical cooling rate (CCR) of approximately 80 Kelvin per second, while SAM2X5 (Fe{sub 49.7}Cr{sub 17.7}Mn{sub 1.9}Mo{sub 7.4}W{sub 1.6}B{sub 15.2}C{sub 3.8}Si{sub 2.4}) with no yttrium has a higher critical cooling rate of approximately 600 Kelvin per second. SAM1651's low CCR enables it to be rendered as a completely amorphous material in practical materials processes. Chromium (Cr), molybdenum (Mo) and tungsten (W) provide corrosion resistance; boron (B) enables glass formation; and rare earths such as yttrium (Y) lower critical cooling rate (CCR). The passive film stability of these Fe-based amorphous metal formulations have been found to be superior to that of conventional stainless steels, and comparable to that of Ni-based alloys, based on electrochemical measurements of the passive film breakdown potential and general corrosion rates.

We have conducted a series of deliquescence, boiling point, chemical transformation, and evaporation experiments to determine the composition of waters likely to contact waste package surfaces over the thermal history of the repository as it heats up and cools back down to ambient conditions. In the above-boiling period, brines will be characterized by high nitrate to chloride ratios that are stable to higher temperatures than previously predicted. This is clearly shown for the NaCl-KNO{sub 3} salt system in the deliquescence and boiling point experiments in this report. Our results show that additional thermodynamic data are needed in nitrate systems to accurately predict brine stability and composition due to salt deliquescence in dust deposited on waste package surfaces. Current YMP models capture dry-out conditions but not composition for NaCl-KNO{sub 3} brines, and they fail to predict dry-out conditions for NaCl-KNO{sub 3}-NaNO{sub 3} brines. Boiling point and deliquescence experiments are needed in NaCl-KNO{sub 3}-NaNO{sub 3} and NaCl-KNO{sub 3}-NaNO{sub 3}-Ca(NO{sub 3}){sub 2} systems to directly determine dry-out conditions and composition, because these salt mixtures are also predicted to control brine composition in the above-boiling period. Corrosion experiments are needed in high temperature and high NO{sub 3}:Cl brines to determine if nitrate inhibits corrosion in these concentrated brines at temperatures above 160 C. Chemical transformations appear to be important for pure calcium- and magnesium-chloride brines at temperatures greater than 120 C. This stems from a lack of acid gas volatility in NaCl/KNO{sub 3} based brines and by slow CO{sub 2}(g) diffusion in alkaline brines. This suggests that YMP corrosion models based on bulk solution experiments over the appropriate composition, temperature, and relative humidity range can be used to predict corrosion in thin brine films formed by salt deliquescence. In contrast to the above-boiling period, the below-boiling period is characterized predominately by NaCl based brines with minor amounts of K, NO{sub 3}, Ca, Mg, F, and Br at less than 70% relative humidity. These brines are identified as sulfate and bicarbonate brines by the chemical divide theory. Nitrate to chloride ratios are strongly tied to relative humidity and halite solubility. Once the relative humidity is low enough to produce brines saturated with respect to halite, then NO{sub 3}:Cl increases to levels and may inhibit corrosion. In addition to the more abundant NaCl-based brines some measured pore waters will evaporate towards acid NaCl-CaCl{sub 2} brines. Acid volatility also occurs with this brine type indicating that chemical transformations may be important in thin films. In contrast to the above-boiling period, comparison of our experimental data with calculated data suggest that current YMP geochemical models adequately predict in-drift chemistry in the below-boiling period.