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Title: LaFe0.9Ni0.1O3 perovskite catalyst with enhanced activity and coke-resistance for dry reforming of ethane

Journal Article · · Journal of Catalysis
 [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
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In this work, a LaFe0.9Ni0.1O3 perovskite catalyst was evaluated for dry reforming of ethane (DRE), with two conventional oxide supported Ni catalysts (Ni/La2O3 and NiFe/La2O3) being used as references. LaFe0.9Ni0.1O3 showed the best activity and high coke-/sintering-resistance. TEM, TGA, and Raman characterizations confirmed that the deactivation of Ni/La2O3 was owing to the growth of Ni particles and the accumulation of coke, although the formation of La2O2CO3 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 CO2 to form CO and reactive oxygen species. Additionally, C2H6 was activated with the assistance of oxygen from the surface or subsurface of LaFe0.9Ni0.1O3 to form CO, rather than directly dissociated to surface carbon species as observed over Ni/La2O3.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1430878
Alternate ID(s):
OSTI ID: 1566232
Report Number(s):
BNL-203437-2018-JAAM
Journal Information:
Journal of Catalysis, Vol. 358, Issue C; ISSN 0021-9517
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 53 works
Citation information provided by
Web of Science

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Cited By (6)

Effect of Oxide Support on Catalytic Performance of FeNi‐based Catalysts for CO 2 ‐assisted Oxidative Dehydrogenation of Ethane journal November 2019
Cooperative Co 0 /Co II Sites Stabilized by a Perovskite Matrix Enable Selective C−O and C−C bond Hydrogenolysis of Oxygenated Arenes journal April 2019
Large Specific Surface Area Macroporous Nanocast LaFe 1− x Ni x O 3 : A Stable Catalyst for Catalytic Methane Dry Reforming journal December 2019
Reversible Segregation of Ni in LaFe 0.8 Ni 0.2 O 3± δ During Coke Removal journal August 2018
Effect of Fe and Mn Substitution in LaNiO3 on Exsolution, Activity, and Stability for Methane Dry Reforming journal December 2019
Improved Catalytic Performance of Ethane Dehydrogenation in the Presence of CO 2 over Zr-Promoted Cr/SiO 2 journal December 2019

Figures / Tables (13)

Fig. 1.(p. 12)figure Fig. 1.
Table 1.(p. 12)table Table 1.
Fig. 2.(p. 13)figure Fig. 2.
Fig. 3.(p. 15)figure Fig. 3.
Fig. 4.(p. 16)figure Fig. 4.
Fig. 5.(p. 16)figure Fig. 5.
Fig. 6.(p. 19)figure Fig. 6.
Fig. 7.(p. 20)figure Fig. 7.
Fig. 8.(p. 21)figure Fig. 8.
Fig. 9.(p. 23)figure Fig. 9.
Table 2.(p. 23)table Table 2.
Fig. 10.(p. 25)figure Fig. 10.
Table 3.(p. 25)table Table 3.

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Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
Perovskite
Dry reforming
Coke-resistance
Oxygen vacancy
CO2