Passive Oxide Film Growth Observed On the Atomic Scale

Chen, Xiaobo; Liu, Zhenyu; Wu, Dongxiang; Cai, Na; Sun, Xianhu; Zakharov, Dmitri N.; Hwang, Sooyeon; Su, Dong; Wang, Guofeng; Zhou, Guangwen

doi:10.1002/admi.202102487

Title: Passive Oxide Film Growth Observed On the Atomic Scale

Journal Article · 25 February 2022 · Advanced Materials Interfaces

DOI: https://doi.org/10.1002/admi.202102487 · OSTI ID:1856775

Chen, Xiaobo ^[1]; Liu, Zhenyu ^[2]; Wu, Dongxiang ^[1]; Cai, Na ^[1]; Sun, Xianhu ^[1];

^[3]; Hwang, Sooyeon ^[3]; Su, Dong ^[3]; Wang, Guofeng ^[2];

^[1]

State Univ. of New York (SUNY), Binghamton, NY (United States)
Univ. of Pittsburgh, PA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Despite of the ubiquitous presence of passivation on most metal surfaces, the microscopic-level picture of how surface passivation occurs has been hitherto unclear. Using the canonical example of the surface passivation of aluminum, here we employ in situ atomistic transmission electron microscopy observations and computational modeling to disentangle entangled microscopic processes and identify the atomic processes leading to the surface passivation. Based on atomic-scale observations of the layer-by-layer expansion of the metal lattice and its subsequent transformation into the amorphous oxide, it is shown that the surface passivation occurs via a two-stage oxidation process, in which the first stage is dominated by intralayer atomic shuffling whereas the second stage is governed by interlayer atomic disordering upon the progressive oxygen uptake. The first stage can be bypassed by increasing surface defects to promote the interlayer atomic migration that results in direct amorphization of multiple atomic layers of the metal lattice. The identified two-stage reaction mechanism and the effect of surface defects in promoting interlayer atomic shuffling can find broader applicability in utilizing surface defects to tune the mass transport and passivation kinetics, as well as the composition, structure and transport properties of the passivation films.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; SC0001135

OSTI ID:: 1856775

Report Number(s):: BNL-222886-2022-JAAM

Journal Information:: Advanced Materials Interfaces, Journal Name: Advanced Materials Interfaces Journal Issue: 11 Vol. 9; ISSN 2196-7350

Publisher:: Wiley-VCHCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
36 MATERIALS SCIENCE
aluminum
in situ transmission microscopy
oxidation
surface passivation

Title: Passive Oxide Film Growth Observed On the Atomic Scale

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