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

Zhao, Baohuai; Yan, Binhang; Yao, Siyu; Xie, Zhenhua; Wu, Qiyuan; Ran, Rui; Weng, Duan; Zhang, Cheng; Chen, Jingguang G.

doi:10.1016/j.jcat.2017.12.012

LaFe_0.9Ni_0.1O₃ perovskite catalyst with enhanced activity and coke-resistance for dry reforming of ethane

Journal Article · Fri Dec 29 00:00:00 EST 2017 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2017.12.012· OSTI ID:1430878

Zhao, Baohuai ^[1]; Yan, Binhang ^[2]; Yao, Siyu ^[3]; Xie, Zhenhua ^[3]; Wu, Qiyuan ^[4]; Ran, Rui ^[5]; Weng, Duan ^[5]; Zhang, Cheng ^[6]; ^[7]

Tsinghua Univ., Beijing (China). School of Materials Science and Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department; Tsinghua Univ., Beijing (China). Department of Chemical Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department
Stony Brook Univ., NY (United States). Material Science and Engineering
Tsinghua Univ., Beijing (China). School of Materials Science and Engineering
Long Island University (Post), Greenvale, NY (United States). Chemistry Department
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Department; Columbia Univ., New York, NY (United States). Department of Chemical Engineering

In this work, a LaFe_0.9Ni_0.1O₃ 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. LaFe_0.9Ni_0.1O₃ 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 LaFe_0.9Ni_0.1O₃ to form CO, rather than directly dissociated to surface carbon species as observed over Ni/La₂O₃.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704

OSTI ID:: 1430878

Alternate ID(s):: OSTI ID: 1430276
OSTI ID: 1566232

Report Number(s):: BNL--203437-2018-JAAM

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 358; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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