A Thermodynamic Investigation of Ni on Thin-Film Titanates (ATiO3)
Abstract
Thin, ~1-nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and then studied as catalyst supports for ~5 wt % of Ni that was added to the perovskite thin films by Atomic Layer Deposition. Scanning Transmission Electron Microscopy demonstrated that both the Ni and the perovskites uniformly covered the surface of the support following oxidation at 1073 K, even after redox cycling, but large Ni particles formed following a reduction at 1073 K. When compared to Ni/MgAl2O4, the perovskite-containing catalysts required significantly higher temperatures for Ni reduction. Equilibrium constants for Ni oxidation, as determined from Coulometric Titration, indicated that the oxidation of Ni shifted to lower PO2 on the perovskite-containing materials. Based on Ni equilibrium constants, Ni interactions are strongest with CaTiO3, followed by SrTiO3 and BaTiO3. The shift in the equilibrium constant was shown to cause reversible deactivation of the Ni/CaTiO3/MgAl2O4 catalyst for CO2 reforming of CH4 at high CO2 pressures, due to the oxidation of the Ni.
- 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)
- OSTI Identifier:
- 1734646
- Grant/Contract Number:
- FG02-13ER16380; SC0009440
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganics
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 12; Journal ID: ISSN 2304-6740
- Publisher:
- MDPI
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Atomic Layer Deposition; Ni catalyst; reforming catalyst; thermodynamics
Citation Formats
Lin, Chao, Foucher, Alexandre C., Stach, Eric A., and Gorte, Raymond J. A Thermodynamic Investigation of Ni on Thin-Film Titanates (ATiO3). United States: N. p., 2020.
Web. doi:10.3390/inorganics8120069.
Lin, Chao, Foucher, Alexandre C., Stach, Eric A., & Gorte, Raymond J. A Thermodynamic Investigation of Ni on Thin-Film Titanates (ATiO3). United States. https://doi.org/10.3390/inorganics8120069
Lin, Chao, Foucher, Alexandre C., Stach, Eric A., and Gorte, Raymond J. Fri .
"A Thermodynamic Investigation of Ni on Thin-Film Titanates (ATiO3)". United States. https://doi.org/10.3390/inorganics8120069. https://www.osti.gov/servlets/purl/1734646.
@article{osti_1734646,
title = {A Thermodynamic Investigation of Ni on Thin-Film Titanates (ATiO3)},
author = {Lin, Chao and Foucher, Alexandre C. and Stach, Eric A. and Gorte, Raymond J.},
abstractNote = {Thin, ~1-nm films of CaTiO3, SrTiO3, and BaTiO3 were deposited onto MgAl2O4 by Atomic Layer Deposition (ALD) and then studied as catalyst supports for ~5 wt % of Ni that was added to the perovskite thin films by Atomic Layer Deposition. Scanning Transmission Electron Microscopy demonstrated that both the Ni and the perovskites uniformly covered the surface of the support following oxidation at 1073 K, even after redox cycling, but large Ni particles formed following a reduction at 1073 K. When compared to Ni/MgAl2O4, the perovskite-containing catalysts required significantly higher temperatures for Ni reduction. Equilibrium constants for Ni oxidation, as determined from Coulometric Titration, indicated that the oxidation of Ni shifted to lower PO2 on the perovskite-containing materials. Based on Ni equilibrium constants, Ni interactions are strongest with CaTiO3, followed by SrTiO3 and BaTiO3. The shift in the equilibrium constant was shown to cause reversible deactivation of the Ni/CaTiO3/MgAl2O4 catalyst for CO2 reforming of CH4 at high CO2 pressures, due to the oxidation of the Ni.},
doi = {10.3390/inorganics8120069},
journal = {Inorganics},
number = 12,
volume = 8,
place = {United States},
year = {Fri Dec 11 00:00:00 EST 2020},
month = {Fri Dec 11 00:00:00 EST 2020}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Perovskite-Pd Three-Way Catalysts for Automotive Applications
conference, March 1993
- Tanaka, Hirohisa; Fujikawa, Hirotoshi; Takahashi, lchiro
- International Congress & Exposition, SAE Technical Paper Series
Improved Thermal Stability and Methane-Oxidation Activity of Pd/Al 2 O 3 Catalysts by Atomic Layer Deposition of ZrO 2
journal, August 2015
- Onn, Tzia Ming; Zhang, Shuyi; Arroyo-Ramirez, Lisandra
- ACS Catalysis, Vol. 5, Issue 10
Investigation of Rh–titanate (ATiO 3 ) interactions on high-surface-area perovskite thin films prepared by atomic layer deposition
journal, January 2020
- Lin, Chao; Foucher, Alexandre C.; Ji, Yichen
- Journal of Materials Chemistry A, Vol. 8, Issue 33
Approaches for Understanding and Controlling Interfacial Effects in Oxide-Supported Metal Catalysts
journal, July 2018
- Ro, Insoo; Resasco, Joaquin; Christopher, Phillip
- ACS Catalysis, Vol. 8, Issue 8
A Perspective on Thin-Film Perovskites as Supports for Metal Catalysts
journal, July 2020
- Mao, Xinyu; Lin, Chao; Graham, George W.
- ACS Catalysis, Vol. 10, Issue 15
Perovskite LaxM1−xNi0.8Fe0.2O3 catalyst for steam reforming of toluene: Crucial role of alkaline earth metal at low steam condition
journal, April 2014
- Oemar, U.; Ang, M. L.; Hee, W. F.
- Applied Catalysis B: Environmental, Vol. 148-149
Changes in Ni-NiO equilibrium due to LaFeO3 and the effect on dry reforming of CH4
journal, January 2020
- Mao, Xinyu; Foucher, Alexandre C.; Stach, Eric A.
- Journal of Catalysis, Vol. 381
Regeneration of Palladium Subsequent to Solid Solution and Segregation in a Perovskite Catalyst: An Intelligent Catalyst
journal, January 2001
- Tanaka, Hirohisa; Tan, Isao; Uenishi, Mari
- Topics in Catalysis, Vol. 16/17, Issue 1/4, p. 63-70
Improved Coking Resistance of “Intelligent” Ni Catalysts Prepared by Atomic Layer Deposition
journal, July 2018
- Lin, Chao; Jang, Joon Baek; Zhang, Lihua
- ACS Catalysis, Vol. 8, Issue 8
Regeneration of NiAl2O4 spinel type catalysts used in the reforming of raw bio-oil
journal, December 2018
- Remiro, Aingeru; Arandia, Aitor; Oar-Arteta, Lide
- Applied Catalysis B: Environmental, Vol. 237
Smart Pd Catalyst with Improved Thermal Stability Supported on High-Surface-Area LaFeO 3 Prepared by Atomic Layer Deposition
journal, January 2018
- Onn, Tzia Ming; Monai, Matteo; Dai, Sheng
- Journal of the American Chemical Society, Vol. 140, Issue 14
The intelligent catalyst having the self-regenerative function of Pd, Rh and Pt for automotive emissions control
journal, September 2006
- Tanaka, H.; Uenishi, M.; Taniguchi, M.
- Catalysis Today, Vol. 117, Issue 1-3
Design of the Intelligent Catalyst for Japan ULEV Standard
journal, July 2004
- Tanaka, Hirohisa; Taniguchi, Masashi; Kajita, Nobuhiko
- Topics in Catalysis, Vol. 30/31
A Nickel-Based Perovskite Catalyst with a Bimodal Size Distribution of Nickel Particles for Dry Reforming of Methane
journal, March 2018
- Chai, Yingjie; Fu, Yu; Feng, He
- ChemCatChem, Vol. 10, Issue 9
Evidence and Model for Strain-Driven Release of Metal Nanocatalysts from Perovskites during Exsolution
journal, December 2015
- Oh, Tae-Sik; Rahani, Ehsan K.; Neagu, Dragos
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 24
A redox stable Pd-doped perovskite for SOFC applications
journal, January 2019
- Marcucci, Andrea; Zurlo, Francesca; Sora, Isabella Natali
- Journal of Materials Chemistry A, Vol. 7, Issue 10
Ni-Substituted Sr(Ti,Fe)O3 SOFC Anodes: Achieving High Performance via Metal Alloy Nanoparticle Exsolution
journal, March 2018
- Zhu, Tenglong; Troiani, Horacio E.; Mogni, Liliana V.
- Joule, Vol. 2, Issue 3
Stabilization of ZrO2 Powders via ALD of CeO2 and ZrO2
journal, October 2017
- Lin, Chao; Mao, Xinyu; Onn, Tzia
- Inorganics, Vol. 5, Issue 4
Self-Regenerating Rh- and Pt-Based Perovskite Catalysts for Automotive-Emissions Control
journal, September 2006
- Tanaka, Hirohisa; Taniguchi, Masashi; Uenishi, Mari
- Angewandte Chemie International Edition, Vol. 45, Issue 36
Self-regeneration of a Pd-perovskite catalyst for automotive emissions control
journal, July 2002
- Nishihata, Y.; Mizuki, J.; Akao, T.
- Nature, Vol. 418, Issue 6894
Redox behavior of palladium at start-up in the Perovskite-type LaFePdOx automotive catalysts showing a self-regenerative function
journal, May 2005
- Uenishi, Mari; Taniguchi, Masashi; Tanaka, Hirohisa
- Applied Catalysis B: Environmental, Vol. 57, Issue 4
Nano-socketed nickel particles with enhanced coking resistance grown in situ by redox exsolution
journal, September 2015
- Neagu, Dragos; Oh, Tae-Sik; Miller, David N.
- Nature Communications, Vol. 6, Issue 1
Oxidative Methane Reforming with an Intelligent Catalyst: Sintering-Tolerant Supported Nickel Nanoparticles
journal, October 2013
- Deng, Jie; Cai, Mengdie; Sun, Wenjing
- ChemSusChem, Vol. 6, Issue 11
“Intelligent” Pt Catalysts Studied on High-Surface-Area CaTiO 3 Films
journal, June 2019
- Lin, Chao; Foucher, Alexandre C.; Ji, Yichen
- ACS Catalysis, Vol. 9, Issue 8