Evidence for redispersion of Ni on LaMnO3 films following high-temperature oxidation
Abstract
LaMnO3 films, 0.5-nm thick, were deposited by atomic layer deposition (ALD) onto γ-Al2O3 that had been modified with 15-wt% CaO. The CaO was shown to be effective in preventing formation of LaAlO3 that formed when La2O3 was deposited directly onto γ-Al2O3. Lattice fringes on the resulting CaAl2O4/γ-Al2O3 substrate were weakly resolved, allowing a detailed characterization of the LaMnO3 films. High-resolution transmission electron microscopy (HR-TEM) images showed that the LaMnO3 formed two-dimensional crystallites, ~10 to 15 nm wide, that covered most of the surface. Crystallites with (001) and (111) orientation were clearly identified. High-temperature oxidation caused Ni to spread over the LaMnO3 film, suggesting there is a reaction of the Ni2+ cations with the perovskite lattice. Ni formed by high-temperature reduction on these films remained well dispersed and significantly more active for CO2 reforming of CH4 compared to Ni on MgAl2O4, even after repeated oxidation and reduction cycles at 1073 K. Finally, the implications of these results for understanding metal-support interactions between Ni and LaMnO3 are discussed.
- Publication Date:
- Research Org.:
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); University of Pennsylvania Materials Research Science and Engineering Center (MRSEC)
- OSTI Identifier:
- 1842776
- Grant/Contract Number:
- FG02-13ER16380; SC0009440
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 407; Journal ID: ISSN 0021-9517
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ni catalyst; Perovskite thin film; Atomic layer deposition; Transmission electron microscopy; Dry reforming of methane
Citation Formats
Kwon, Ohhun, Foucher, Alexandre C., Huang, Renjing, Stach, Eric A., Vohs, John M., and Gorte, Raymond J. Evidence for redispersion of Ni on LaMnO3 films following high-temperature oxidation. United States: N. p., 2022.
Web. doi:10.1016/j.jcat.2022.01.036.
Kwon, Ohhun, Foucher, Alexandre C., Huang, Renjing, Stach, Eric A., Vohs, John M., & Gorte, Raymond J. Evidence for redispersion of Ni on LaMnO3 films following high-temperature oxidation. United States. https://doi.org/10.1016/j.jcat.2022.01.036
Kwon, Ohhun, Foucher, Alexandre C., Huang, Renjing, Stach, Eric A., Vohs, John M., and Gorte, Raymond J. Mon .
"Evidence for redispersion of Ni on LaMnO3 films following high-temperature oxidation". United States. https://doi.org/10.1016/j.jcat.2022.01.036. https://www.osti.gov/servlets/purl/1842776.
@article{osti_1842776,
title = {Evidence for redispersion of Ni on LaMnO3 films following high-temperature oxidation},
author = {Kwon, Ohhun and Foucher, Alexandre C. and Huang, Renjing and Stach, Eric A. and Vohs, John M. and Gorte, Raymond J.},
abstractNote = {LaMnO3 films, 0.5-nm thick, were deposited by atomic layer deposition (ALD) onto γ-Al2O3 that had been modified with 15-wt% CaO. The CaO was shown to be effective in preventing formation of LaAlO3 that formed when La2O3 was deposited directly onto γ-Al2O3. Lattice fringes on the resulting CaAl2O4/γ-Al2O3 substrate were weakly resolved, allowing a detailed characterization of the LaMnO3 films. High-resolution transmission electron microscopy (HR-TEM) images showed that the LaMnO3 formed two-dimensional crystallites, ~10 to 15 nm wide, that covered most of the surface. Crystallites with (001) and (111) orientation were clearly identified. High-temperature oxidation caused Ni to spread over the LaMnO3 film, suggesting there is a reaction of the Ni2+ cations with the perovskite lattice. Ni formed by high-temperature reduction on these films remained well dispersed and significantly more active for CO2 reforming of CH4 compared to Ni on MgAl2O4, even after repeated oxidation and reduction cycles at 1073 K. Finally, the implications of these results for understanding metal-support interactions between Ni and LaMnO3 are discussed.},
doi = {10.1016/j.jcat.2022.01.036},
journal = {Journal of Catalysis},
number = ,
volume = 407,
place = {United States},
year = {Mon Feb 07 00:00:00 EST 2022},
month = {Mon Feb 07 00:00:00 EST 2022}
}
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