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HERO ID
1739257
Reference Type
Journal Article
Title
Reducing the deactivation of Ni-metal during the catalytic partial oxidation of a surrogate diesel fuel mixture
Author(s)
Haynes, DJ; Campos, A; Smith, MW; Berry, DA; Shekhawat, D; Spivey, JJ
Year
2010
Is Peer Reviewed?
Yes
Journal
Catalysis Today
ISSN:
0920-5861
Volume
154
Issue
3-4
Page Numbers
210-216
DOI
10.1016/j.cattod.2010.03.072
Web of Science Id
WOS:000281607400006
Abstract
Ni catalysts are active and selective for the conversion of hydrocarbon into synthesis gas. However, conventional supported Ni catalysts rapidly deactivate at the high temperatures required for partial oxidation of diesel fuel by sintering and metal vaporization, as well as by carbon deposition and sulfur poisoning. Thus, to reduce deactivation Ni (3 wt%) was substituted into the structures of Ba-hexaaluminate (BNHA) and La-Sr-Zr pyrochlore (LSZN), and their activity was compared to a supported Ni/Al(2)O(3) for the catalytic partial oxidation (CPOX) of a surrogate diesel fuel. Characterization by XRD showed a single phase beta-alumina for the hexaaluminate, while LSZN had a pyrochlore structure with a defect SrZrO(3) perovskite phase. Temperature programmed reduction experiments confirmed Ni was reducible in all catalysts. XANES results confirmed that Ni atoms were substituted into the hexaaluminate and pyrochlore structures, as spectra for each catalyst showed different coordination environments for Ni compared to a NiO standard. During CPOX activity tests (T = 900 degrees C and WHSV= 50,000 scc/g(cat)/h), the LSZN pyrochlore produced stable H(2) and CO yields in the presence of 5 wt% 1-methylnaphthalene and 50ppmw dibenzothiophene/n-tetradecane for 2 h, while both Ni/Al(2)O(3) and BNHA catalysts were irreversibly deactivated by this mixture over the same time. Activity loss was strongly linked to carbon formation. (C) 2010 Elsevier B.V. All rights reserved.
Keywords
Pyrochlore; Hexaaluminate; Nickel; Logistic fuel reforming; Partial oxidation catalyst
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