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Title: Effect of nickel hexaaluminate mirror cation on structure-sensitive reactions during n-tetradecane partial oxidation

Abstract

Reforming studies were conducted on nickel-substituted hexaaluminate catalysts, ANi0.4Al11.6O19-δ (A = La, Sr and Ba), to reform liquid hydrocarbon fuels into H2-rich synthesis gas for fuel cell applications. The reaction conditions studied were the partial oxidation of n-tetradecane (I) and n-tetradecane with 50 ppmw sulfur as dibenzothiophene (II). Hexaaluminate catalyst activity toward reaction conditions (I) and (II) as well as the surface Ni concentration and dispersion was shown to correlate with the type of mirror cation substituted into the lattice. The Ni surface concentration was determined by XPS to be 5.3, <0.1 and 0.7 wt.% for LaNi0.4Al11.6O19-δ, BaNi0.4Al11.6O19-δ and SrNi0.4Al11.6O19-δ, respectively. SrNi0.4Al11.6O19-δ and BaNi0.4Al11.6O19-δ catalysts exhibited stable performance for reaction condition (I), while the loss in activity exhibited over time by LaNi0.4Al11.6O19-δ suggested site blocking by carbon deposition. Under reaction condition (II), additional activity loss was experienced by both LaNi0.4Al11.6O19-δ and Al11.6O19-δ catalysts due to the presence of dibenzothiophene. However, LaNi0.4Al11.6O19-δ experienced more severe and partially reversible site blocking where SrNi0.4Al11.6O19-δ experienced a less severe loss of activity, selectivity and irreversible site blocking. The behavior observed in nickel-substituted hexaaluminate catalysts suggests that the different mirror cations influenced the coordination of Ni sites within the lattice and adsorption of hydrocarbons tomore » the surface of the catalysts.« less

Authors:
; ; ; ; ;  [1]
  1. West Virginia University, Morgantown, WV
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, and Morgantown, WV
Sponsoring Org.:
USDOE - Office of Fossil Energy (FE)
OSTI Identifier:
913355
Report Number(s):
DOE/NETL-IR-2007-109
Journal ID: ISSN 0926-860X
DOE Contract Number:
None cited
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Catalysis. A, General; Journal Volume: 323
Country of Publication:
United States
Language:
English
Subject:
Nickel; Hexaaluminate; Partial oxidation; Sulfur; Diesel; Fuel cell

Citation Formats

Gardner, T H, Shekhawat, D, Berry, D A, Smith, M W, Salazar, M, and Kugler, E L. Effect of nickel hexaaluminate mirror cation on structure-sensitive reactions during n-tetradecane partial oxidation. United States: N. p., 2007. Web. doi:10.1016/j.apcata.2007.01.051.
Gardner, T H, Shekhawat, D, Berry, D A, Smith, M W, Salazar, M, & Kugler, E L. Effect of nickel hexaaluminate mirror cation on structure-sensitive reactions during n-tetradecane partial oxidation. United States. doi:10.1016/j.apcata.2007.01.051.
Gardner, T H, Shekhawat, D, Berry, D A, Smith, M W, Salazar, M, and Kugler, E L. Mon . "Effect of nickel hexaaluminate mirror cation on structure-sensitive reactions during n-tetradecane partial oxidation". United States. doi:10.1016/j.apcata.2007.01.051.
@article{osti_913355,
title = {Effect of nickel hexaaluminate mirror cation on structure-sensitive reactions during n-tetradecane partial oxidation},
author = {Gardner, T H and Shekhawat, D and Berry, D A and Smith, M W and Salazar, M and Kugler, E L},
abstractNote = {Reforming studies were conducted on nickel-substituted hexaaluminate catalysts, ANi0.4Al11.6O19-δ (A = La, Sr and Ba), to reform liquid hydrocarbon fuels into H2-rich synthesis gas for fuel cell applications. The reaction conditions studied were the partial oxidation of n-tetradecane (I) and n-tetradecane with 50 ppmw sulfur as dibenzothiophene (II). Hexaaluminate catalyst activity toward reaction conditions (I) and (II) as well as the surface Ni concentration and dispersion was shown to correlate with the type of mirror cation substituted into the lattice. The Ni surface concentration was determined by XPS to be 5.3, <0.1 and 0.7 wt.% for LaNi0.4Al11.6O19-δ, BaNi0.4Al11.6O19-δ and SrNi0.4Al11.6O19-δ, respectively. SrNi0.4Al11.6O19-δ and BaNi0.4Al11.6O19-δ catalysts exhibited stable performance for reaction condition (I), while the loss in activity exhibited over time by LaNi0.4Al11.6O19-δ suggested site blocking by carbon deposition. Under reaction condition (II), additional activity loss was experienced by both LaNi0.4Al11.6O19-δ and Al11.6O19-δ catalysts due to the presence of dibenzothiophene. However, LaNi0.4Al11.6O19-δ experienced more severe and partially reversible site blocking where SrNi0.4Al11.6O19-δ experienced a less severe loss of activity, selectivity and irreversible site blocking. The behavior observed in nickel-substituted hexaaluminate catalysts suggests that the different mirror cations influenced the coordination of Ni sites within the lattice and adsorption of hydrocarbons to the surface of the catalysts.},
doi = {10.1016/j.apcata.2007.01.051},
journal = {Applied Catalysis. A, General},
number = ,
volume = 323,
place = {United States},
year = {Mon Apr 30 00:00:00 EDT 2007},
month = {Mon Apr 30 00:00:00 EDT 2007}
}