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This content will become publicly available on December 29, 2018

Title: LaFe 0.9Ni 0.1O 3 perovskite catalyst with enhanced activity and coke-resistance for dry reforming of ethane

In this work, a LaFe 0.9Ni 0.1O 3 perovskite catalyst was evaluated for dry reforming of ethane (DRE), with two conventional oxide supported Ni catalysts (Ni/La 2O 3 and NiFe/La 2O 3) being used as references. LaFe 0.9Ni 0.1O 3 showed the best activity and high coke-/sintering-resistance. TEM, TGA, and Raman characterizations confirmed that the deactivation of Ni/La 2O 3 was owing to the growth of Ni particles and the accumulation of coke, although the formation of La 2O 2CO 3 was able to remove part of the coke during the reaction. The introduction of Fe-related species inhibited the coke formation while decreased the activity due to the loss of active sites. A portion of Ni ions in the perovskite lattice could be reduced to form highly dispersed and stable Ni nanoparticles on the surface during the reaction and oxygen vacancies were left in the perovskite lattice. Pulse reactor studies revealed that the oxygen vacancies in the perovskite could facilitate the activation and dissociation of CO 2 to form CO and reactive oxygen species. Additionally, C 2H 6 was activated with the assistance of oxygen from the surface or subsurface of LaFe 0.9Ni 0.1O 3 to form CO, rather thanmore » directly dissociated to surface carbon species as observed over Ni/La 2O 3.« less
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [4] ;  [5] ;  [5] ;  [6] ; ORCiD logo [7]
  1. Tsinghua Univ., Beijing (China). School of Materials Science and Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department; Tsinghua Univ., Beijing (China). Department of Chemical Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
  4. Stony Brook Univ., NY (United States). Material Science and Engineering
  5. Tsinghua Univ., Beijing (China). School of Materials Science and Engineering
  6. Long Island University (Post), Greenvale, NY (United States). Chemistry Department
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department; Columbia Univ., New York, NY (United States). Department of Chemical Engineering
Publication Date:
Report Number(s):
BNL-203437-2018-JAAM
Journal ID: ISSN 0021-9517
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 358; Journal Issue: C; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Perovskite; Dry reforming; Coke-resistance; Oxygen vacancy; CO2
OSTI Identifier:
1430878