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Title: In situ atomic-scale imaging of the metal/oxide interfacial transformation

Directly probing structure dynamics at metal/oxide interfaces has been a major challenge due to their buried nature.Using environmental transmission electron microscopy,here we report observations of the in-place formation of Cu 2O/Cu interfaces via the oxidation of Cu, and subsequently probe the atomic mechanisms by which interfacial transformation and grain rotation occur at the interfaces during reduction in an H 2 gas environment. The Cu 2O→Cu transformation is observed to occur initially along the Cu 2O/Cu interface in a layer-by-layer manner.The accumulation of oxygen vacancies at the Cu 2O/Cu interface drives the collapse of the Cu 2O lattice near the interface region, which results in a tilted Cu 2O/Cu interface with concomitant Cu 2O island rotation. Lastly, these results provide unprecedented microscopic detail regarding the redox reactions of supported oxides,which differs fundamentally from the reduction of bulk or isolated oxides that requires the formation of new interfaces between the parent oxide and the reduced phase.
Authors:
 [1] ;  [1] ; ORCiD logo [2] ; ORCiD logo [2] ;  [1]
  1. State Univ. of New York at Binghamton, Binghamton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-205663-2018-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; metal oxide interfaces; environmental transmission electron microscopy; Cu oxidation; Cu reduction; DFT calculations
OSTI Identifier:
1438307

Zou, Lianfeng, Li, Jonathan, Zakharov, Dmitri, Stach, Eric A., and Zhou, Guangwen. In situ atomic-scale imaging of the metal/oxide interfacial transformation. United States: N. p., Web. doi:10.1038/s41467-017-00371-4.
Zou, Lianfeng, Li, Jonathan, Zakharov, Dmitri, Stach, Eric A., & Zhou, Guangwen. In situ atomic-scale imaging of the metal/oxide interfacial transformation. United States. doi:10.1038/s41467-017-00371-4.
Zou, Lianfeng, Li, Jonathan, Zakharov, Dmitri, Stach, Eric A., and Zhou, Guangwen. 2017. "In situ atomic-scale imaging of the metal/oxide interfacial transformation". United States. doi:10.1038/s41467-017-00371-4. https://www.osti.gov/servlets/purl/1438307.
@article{osti_1438307,
title = {In situ atomic-scale imaging of the metal/oxide interfacial transformation},
author = {Zou, Lianfeng and Li, Jonathan and Zakharov, Dmitri and Stach, Eric A. and Zhou, Guangwen},
abstractNote = {Directly probing structure dynamics at metal/oxide interfaces has been a major challenge due to their buried nature.Using environmental transmission electron microscopy,here we report observations of the in-place formation of Cu2O/Cu interfaces via the oxidation of Cu, and subsequently probe the atomic mechanisms by which interfacial transformation and grain rotation occur at the interfaces during reduction in an H2 gas environment. The Cu2O→Cu transformation is observed to occur initially along the Cu2O/Cu interface in a layer-by-layer manner.The accumulation of oxygen vacancies at the Cu2O/Cu interface drives the collapse of the Cu2O lattice near the interface region, which results in a tilted Cu2O/Cu interface with concomitant Cu2O island rotation. Lastly, these results provide unprecedented microscopic detail regarding the redox reactions of supported oxides,which differs fundamentally from the reduction of bulk or isolated oxides that requires the formation of new interfaces between the parent oxide and the reduced phase.},
doi = {10.1038/s41467-017-00371-4},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {8}
}

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