Potential-pH diagrams considering complex oxide solution phases for understanding aqueous corrosion of multi-principal element alloys

Wang, Kang; Han, Junsoo; Gerard, Angela Yu; Scully, John R.; Zhou, Bi-Cheng

doi:10.1038/s41529-020-00141-6

Title: Potential-pH diagrams considering complex oxide solution phases for understanding aqueous corrosion of multi-principal element alloys

Journal Article · Thu Nov 12 00:00:00 EST 2020 · npj Materials Degradation

DOI:https://doi.org/10.1038/s41529-020-00141-6· OSTI ID:1852331

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; Gerard, Angela Yu;

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The potential-pH diagram, a graphical representation of the thermodynamically predominant reaction products in aqueous corrosion, is originally proposed for the corrosion of pure metals. The original approach only leads to stoichiometric oxides and hydroxides as the oxidation products. However, numerous experiments show that non-stoichiometric oxide scales are prevalent in the aqueous corrosion of alloys. In the present study, a room temperature potential-pH diagram considering oxide solid solutions, as a generalization of the traditional potential-pH diagram with stoichiometric oxides, is constructed for an FCC single-phase multi-principal element alloy (MPEA) based on the CALculation of PHAse Diagram method. The predominant reaction products, the ions in aqueous solution, and the cation distribution in oxides are predicted. The oxide solid solution is stabilized by the mixing free energy (or mixing entropy) and the stabilizing effect becomes more significant as the temperature increases. Consequently, solid solution oxides are stable in large regions of the potential-pH diagram and the mixing free energy mostly affects the equilibrium composition of the stable oxides, while the shape of stable regions for oxides is mostly determined by the structure of the stable oxides. Agreements are found for Ni²⁺, Fe²⁺, and Mn²⁺between the atomic emission spectroelectrochemistry measurements and thermodynamic calculations, while deviations exist for Cr³⁺and Co²⁺possibly due to surface complexation with species such as Cl^-and the oxide dissolution. By incorporating the solution models of oxides, the current work presents a general and more accurate way to analyze the reaction products during aqueous corrosion of MPEAs.

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Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: SC0016584

OSTI ID:: 1852331

Journal Information:: npj Materials Degradation, Vol. 4, Issue 1; ISSN 2397-2106

Publisher:: Springer

Country of Publication:: United States

Language:: English

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