skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Catalytic partial oxidation of CH 4 over Ni-substituted barium hexaaluminate catalysts

Abstract

Ba 0.75Ni yAl 12-yO 19-δ (y = 0.2, 0.4, 0.6, 0.8 and 1.0) catalysts were tested for the partial oxidation of CH 4 at temperatures between 200 and 900 °C. Temperature programmed reaction results indicate that light-off for the partial oxidation reaction occurred between 665 and 687 °C for all catalysts. Isothermal runs performed at 900 °C on the catalysts showed stable reaction product concentrations, consistent with equilibrium. Post-reaction analysis of the used catalysts showed that there are two distinct zones in the catalyst bed. In a short leading edge of the bed, the apparently complete consumption of oxygen leads to a catalyst which XANES analysis shows is primarily Ni-substituted into the hexaaluminate phase. In the downstream portion of the bed, Ni is shown to be present as metallic Ni. This corresponds to a reaction sequence in which the oxidation of CH 4 proceeds at the inlet until all oxygen is reacted, followed by the reaction of CO 2 and H 2O with unreacted CH 4, and its derivatives, to produce the final syngas mixture. Finally, from the change in the unit-cell dimensions with Ni substitution, there is a clear indication that Ni 2+, which has a larger ionic radiusmore » than aluminum, substitutes for Al 3+ in the hexaaluminate lattice in the synthesis process, and there is no restructuring of the bulk hexaaluminate phase after the Ni is removed from the lattice.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
National Energy Technology Lab. (NETL), Pittsburgh, PA, and Morgantown, WV (United States). In-house Research; National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1151815
Report Number(s):
TPR-2953
Journal ID: ISSN 0920-5861
Resource Type:
Journal Article
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 157; Journal Issue: 1-4; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Hexaaluminate; Partial oxidation; Nickel; Methane

Citation Formats

Gardner, Todd H., Spivey, James J., Campos, Andrew, Hissam, Jason C., Kugler, Edwin L., and Roy, Amitava D. Catalytic partial oxidation of CH4 over Ni-substituted barium hexaaluminate catalysts. United States: N. p., 2010. Web. doi:10.1016/j.cattod.2010.05.033.
Gardner, Todd H., Spivey, James J., Campos, Andrew, Hissam, Jason C., Kugler, Edwin L., & Roy, Amitava D. Catalytic partial oxidation of CH4 over Ni-substituted barium hexaaluminate catalysts. United States. doi:10.1016/j.cattod.2010.05.033.
Gardner, Todd H., Spivey, James J., Campos, Andrew, Hissam, Jason C., Kugler, Edwin L., and Roy, Amitava D. Wed . "Catalytic partial oxidation of CH4 over Ni-substituted barium hexaaluminate catalysts". United States. doi:10.1016/j.cattod.2010.05.033.
@article{osti_1151815,
title = {Catalytic partial oxidation of CH4 over Ni-substituted barium hexaaluminate catalysts},
author = {Gardner, Todd H. and Spivey, James J. and Campos, Andrew and Hissam, Jason C. and Kugler, Edwin L. and Roy, Amitava D.},
abstractNote = {Ba0.75NiyAl12-yO19-δ (y = 0.2, 0.4, 0.6, 0.8 and 1.0) catalysts were tested for the partial oxidation of CH4 at temperatures between 200 and 900 °C. Temperature programmed reaction results indicate that light-off for the partial oxidation reaction occurred between 665 and 687 °C for all catalysts. Isothermal runs performed at 900 °C on the catalysts showed stable reaction product concentrations, consistent with equilibrium. Post-reaction analysis of the used catalysts showed that there are two distinct zones in the catalyst bed. In a short leading edge of the bed, the apparently complete consumption of oxygen leads to a catalyst which XANES analysis shows is primarily Ni-substituted into the hexaaluminate phase. In the downstream portion of the bed, Ni is shown to be present as metallic Ni. This corresponds to a reaction sequence in which the oxidation of CH4 proceeds at the inlet until all oxygen is reacted, followed by the reaction of CO2 and H2O with unreacted CH4, and its derivatives, to produce the final syngas mixture. Finally, from the change in the unit-cell dimensions with Ni substitution, there is a clear indication that Ni2+, which has a larger ionic radius than aluminum, substitutes for Al3+ in the hexaaluminate lattice in the synthesis process, and there is no restructuring of the bulk hexaaluminate phase after the Ni is removed from the lattice.},
doi = {10.1016/j.cattod.2010.05.033},
journal = {Catalysis Today},
issn = {0920-5861},
number = 1-4,
volume = 157,
place = {United States},
year = {2010},
month = {11}
}