In Situ Oxidation Studies of High-Entropy Alloy Nanoparticles

Song, Boao; Yang, Yong; Rabbani, Muztoba; Yang, Timothy T.; He, Kun; Hu, Xiaobing; Yuan, Yifei; Ghildiyal, Pankaj; Dravid, Vinayak P.; Zachariah, Michael R.; Saidi, Wissam A.; Liu, Yuzi; Shahbazian-Yassar, Reza

doi:10.1021/acsnano.0c05250

In Situ Oxidation Studies of High-Entropy Alloy Nanoparticles

Journal Article · Tue Oct 20 00:00:00 EDT 2020 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.0c05250· OSTI ID:1840536

^[1]; ^[2]; Rabbani, Muztoba ^[3]; ^[3]; He, Kun ^[4]; ^[4]; ^[1]; Ghildiyal, Pankaj ^[5]; ^[4]; ^[5]; ^[3]; ^[6]; ^[1]

Univ. of Illinois, Chicago, IL (United States)
Univ. of Maryland, College Park, MD (United States); Univ. of California, Riverside, CA (United States)
Univ. of Pittsburgh, PA (United States)
Northwestern Univ., Evanston, IL (United States). International Institute for Nanotechnology (IIN), Northwestern University Atomic and Nanoscale Characterization Experimental (NUANCE) Center
Univ. of California, Riverside, CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Although high-entropy alloys (HEAs) have shown tremendous potential for elevated temperature, anticorrosion, and catalysis applications, little is known on how HEA materials behave under complex service environments. Herein, we studied the high-temperature oxidation behavior of Fe_0.28Co_0.21Ni_0.20Cu_0.08Pt_0.23HEA nanoparticles (NPs) in an atmospheric pressure dry air environment by in situ gas-cell transmission electron microscopy. It is found that the oxidation of HEA NPs is governed by Kirkendall effects with logarithmic oxidation rates rather than parabolic as predicted by Wagner's theory. Further, the HEA NPs are found to oxidize at a significantly slower rate compared to monometallic NPs. The outward diffusion of transition metals and formation of disordered oxide layer are observed in real time and confirmed through analytical energy dispersive spectroscopy, and electron energy loss spectroscopy characterizations. Localized ordered lattices are identified in the oxide, suggesting the formation of Fe₂O₃, CoO, NiO, and CuO crystallites in an overall disordered matrix. Hybrid Monte Carlo and molecular dynamics simulations based on first-principles energies and forces support these findings and show that the oxidation drives surface segregation of Fe, Co, Ni, and Cu, while Pt stays in the core region. The present work offers key insights into how HEA NPs behave under high-temperature oxidizing environment and sheds light on future design of highly stable alloys under complex service conditions.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1840536

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 11 Vol. 14; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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