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Title: Low Temperature Propane Oxidation over Co3O4 based Nano-array Catalysts. Ni Dopant Effect, Reaction Mechanism and Structural Stability

Low temperature propane oxidation has been achieved by Co3O4-based nano-array catalysts featuring low catalytic materials loading. The Ni doping into the Co3O4 lattice has led to enhanced reaction kinetics at low temperature by promoting the surface lattice oxygen activity. In situ DRIFTS investigation in tandem with isotopic oxygen exchange reveals that the propane oxidation proceeds via Mars-van Krevelen mechanism where surface lattice oxygen acts as the active site whereas O2 in the reaction feed does not directly participate in CO2 formation. The Ni doping promotes the formation of less stable carbonates on the surface to facilitate the CO2 desorption. The thermal stability of Ni doped Co3O4 decreases with increased Ni concentration while catalytic activity increases. A balance between enhanced activity and compromised thermal stability shall be considered in the Ni doped Co3O4 nano-array catalysts for low temperature hydrocarbon oxidation. This study provides useful and timely guidance for rational catalyst design toward low temperature catalytic oxidation.
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [1] ;  [3] ;  [1] ;  [1]
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. National Univ. of Singapore (Singapore)
Publication Date:
OSTI Identifier:
1213987
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 180; Journal Issue: 1; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY