Atomistic mechanisms of water vapor–induced surface passivation

Chen, Xiaobo; Shan, Weitao; Wu, Dongxiang; Patel, Shyam Bharatkumar; Cai, Na; Li, Chaoran; Ye, Shuonan; Liu, Zhao; Hwang, Sooyeon; Zakharov, Dmitri N.; Boscoboinik, Jorge Anibal; Wang, Guofeng; Zhou, Guangwen

doi:10.1126/sciadv.adh5565

Title: Atomistic mechanisms of water vapor–induced surface passivation

Journal Article · 31 October 2023 · Science Advances

DOI: https://doi.org/10.1126/sciadv.adh5565 · OSTI ID:2267563

^[1];

^[2]; Wu, Dongxiang ^[1];

^[1]; Cai, Na ^[1]; Li, Chaoran ^[1]; Ye, Shuonan ^[1]; Liu, Zhao ^[1];

^[3];

^[2];

^[1]

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

The microscopic mechanisms underpinning the spontaneous surface passivation of metals from ubiquitous water have remained largely elusive. Here, using in situ environmental electron microscopy to atomically monitor the reaction dynamics between aluminum surfaces and water vapor, we provide direct experimental evidence that the surface passivation results in a bilayer oxide film consisting of a crystalline-like Al(OH)₃ top layer and an inner layer of amorphous Al₂O₃. The Al(OH)₃ layer maintains a constant thickness of ~5.0 Å, while the inner Al₂O₃ layer grows at the Al₂O₃/Al interface to a limiting thickness. On the basis of experimental data and atomistic modeling, we show the tunability of the dissociation pathways of H₂O molecules with the Al, Al₂O₃, and Al(OH)₃ surface terminations. The fundamental insights may have practical significance for the design of materials and reactions for two seemingly disparate but fundamentally related disciplines of surface passivation and catalytic H₂ production from water.

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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). Scientific User Facilities (SUF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; SC0001135

OSTI ID:: 2267563

Report Number(s):: BNL--225123-2023-JAAM

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 44 Vol. 9; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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