Atomic-scale understanding of oxide growth and dissolution kinetics of Ni-Cr alloys

Xiao, Penghao; Orme, Christine A.; Qiu, S. Roger; Pham, Tuan Anh; Cho, Seongkoo; Bagge-Hansen, Michael; Wood, Brandon C.

doi:10.1038/s41467-024-54627-x

Title: Atomic-scale understanding of oxide growth and dissolution kinetics of Ni-Cr alloys

Journal Article · 02 January 2025 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-54627-x · OSTI ID:2516799

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Dalhousie Univ., Halifax, NS (Canada)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Aqueous corrosion of metals is governed by formation and dissolution of a passivating, multi-component surface oxide. Unfortunately, a detailed atomistic description is challenging due to the compositional complexity and the need to consider multiple kinetic factors simultaneously. To this end, we combine experiments with a first-principles-derived, multiscale computational framework that transcends thermodynamic descriptions to explicitly simulate the kinetic evolution of surface oxides of Ni-Cr alloys as a function of composition, temperature, pH, and applied voltage. In the absence of pitting, we identify three distinct voltage regimes, which are kinetically dominated by oxide growth, dissolution, and competitive dissolution and reprecipitation. Evolving compositional gradients and oxide thickness are revealed, including a transition between a metastable Ni-Cr mixed oxide and a thick, porous Ni-dominated oxide. Beyond elucidating the underlying physics, we highlight the need for competing kinetics in models to properly predict the transition from passivation to corrosion. Our results provide a key step towards co-design of alloy composition alongside environmental conditions for sustainable use across a variety of critical energy and infrastructure applications.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: Natural Sciences and Engineering Research Council of Canada (NSERC); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC52-07NA27344

OSTI ID:: 2516799

Report Number(s):: LLNL--JRNL-837303; 1056897

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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