High-throughput thermodynamic screening of oxide-scale adhesion across the CoCrFeMnNiAl high-entropy alloys
Abstract
One significant benefit of reactive element (RE) additions is the colossal improvement in oxide-scale retention during high-temperature oxidation. Selecting optimal RE dopants in high-entropy alloys remains empirical because the relevant thermodynamic landscape is inaccessible to first-principles at the required compositional resolution. Here we apply the macroscopic atom model, coupled with McLean isotherm and Guttmann models, to screen adhesion across nine CoCrFeMnNiAl sub-families at \ce{Cr2O3} and \ce{Al2O3} interfaces, ranking five REs (Hf, Y, Zr, La, Ti) for segregation, adhesion enhancement, and sulfur displacement. The screening reveals an oxide-dependent ranking inversion, with Hf dominating at \ce{Cr2O3} and La dominating at \ce{Al2O3}, driven by the interplay between RE--O and RE--matrix interaction enthalpies. Mn-containing alloys exhibit intrinsic sulfur resistance, consistent with their experimentally observed oxidation characteristics. A sulfur immunity phase diagram identifies compositions with Al~+~Mn~≳~25~at\% as thermodynamically immune to S-induced adhesion loss. All crossover concentrations collapse onto a universal exponential governed by the segregation enthalpy difference, providing a transferable design rule. Inverse design identifies \ce{Co16Cr16Fe16Ni16Al35} as the optimal S-immune composition with Wsep = 5.95~J/m2 without RE doping.
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BibTeX
@misc{boakye2026highthroughput,
title = {{High-throughput thermodynamic screening of oxide-scale adhesion across the CoCrFeMnNiAl high-entropy alloys}},
author = {Dennis Boakye and Chuang Deng},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.11640},
eprint = {2609.11640},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.11640},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - UNPB
TI - High-throughput thermodynamic screening of oxide-scale adhesion across the CoCrFeMnNiAl high-entropy alloys
AU - Dennis Boakye
AU - Chuang Deng
PY - 2026
DA - 2026/09/10
PB - arXiv
DO - 10.48550/arxiv.2609.11640
UR - https://arxiv.org/abs/2609.11640
AB - One significant benefit of reactive element (RE) additions is the colossal improvement in oxide-scale retention during high-temperature oxidation. Selecting optimal RE dopants in high-entropy alloys remains empirical because the relevant thermodynamic landscape is inaccessible to first-principles at the required compositional resolution. Here we apply the macroscopic atom model, coupled with McLean isotherm and Guttmann models, to screen adhesion across nine CoCrFeMnNiAl sub-families at \ce{Cr2O3} and \ce{Al2O3} interfaces, ranking five REs (Hf, Y, Zr, La, Ti) for segregation, adhesion enhancement, and sulfur displacement. The screening reveals an oxide-dependent ranking inversion, with Hf dominating at \ce{Cr2O3} and La dominating at \ce{Al2O3}, driven by the interplay between RE--O and RE--matrix interaction enthalpies. Mn-containing alloys exhibit intrinsic sulfur resistance, consistent with their experimentally observed oxidation characteristics. A sulfur immunity phase diagram identifies compositions with Al~+~Mn~≳~25~at\% as thermodynamically immune to S-induced adhesion loss. All crossover concentrations collapse onto a universal exponential governed by the segregation enthalpy difference, providing a transferable design rule. Inverse design identifies \ce{Co16Cr16Fe16Ni16Al35} as the optimal S-immune composition with W_sep = 5.95~J/m^2 without RE doping.
ER -