Influence of terbium doping on oxygen storage capacity of Ceria-zirconia supports: Enhanced durability of ni catalysts for propane steam reforming

D. Harshini, Yongmin Kim, SukWoo Nam, Tae Hoon Lim, Sung An Hong, Chang Won Yoon

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

Systematic studies were conducted to understand the influence of Tb doping on durability of Ni-based catalysts supported onto Ce0.75-xZr 0.25TbxO2 (CZT x, x = 0.0-0.2), prepared by glycine-nitrate process. Ni metals were deposited onto the as-synthesized supports using a solvothermal method. The prepared supports and catalysts were characterized by a number of ex-situ techniques including X-ray powder diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, H 2-temperature-programmed reduction and Brunauer-Emmett-Teller analyses. These studies along with soot oxidation experiments confirmed that the existence of Tb3+ and/or Ce3+ ions made significant contribution to enhancing oxygen storage capacity (OSC) of the Tb doped CeO 2-ZrO2 based materials, and among all the supports studied, Ce0.65Zr0.25Tb0.1O2 (x = 0.1, CZT 0.1 ) showed the highest OSC. To assess the performance of these catalysts, steam reforming reactions of propane were further carried out on the Ni supported catalysts (Ni/CZT x ) at a steam-to-carbon ratio of 1.5, a gas hourly spaced velocity of 45,000 h-1, and a reaction temperature of 700 C. Consistent with the determined OSC of the catalysts, the durabilities of the Ni/CZT x catalysts were found to be increased in the order of Ni/CZT 0.1 > Ni/CZT 0.15 > Ni/CZT 0.2 > Ni/CZT 0.05 > Ni/CZ. In particular, the activity of Ni/CZT 0.1 was maintained to be >99 % of propane conversion at least for 200 h without significant deactivation. Graphical Abstract: [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)49-57
Number of pages9
JournalCatalysis Letters
Volume143
Issue number1
DOIs
Publication statusPublished - 2013 Jan 1
Externally publishedYes

Fingerprint

Terbium
Propane
Steam reforming
Cerium compounds
Catalyst supports
Zirconia
Durability
Doping (additives)
Oxygen
Catalysts
Soot
Steam
Reforming reactions
Nitrates
X ray powder diffraction
Glycine
Raman spectroscopy
Amino acids
Carbon
X ray photoelectron spectroscopy

Keywords

  • Catalysts
  • Ceria-zirconia
  • Doping
  • Oxygen storage capacity
  • Steam reforming of propane
  • Terbium

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

Cite this

Influence of terbium doping on oxygen storage capacity of Ceria-zirconia supports : Enhanced durability of ni catalysts for propane steam reforming. / Harshini, D.; Kim, Yongmin; Nam, SukWoo; Lim, Tae Hoon; Hong, Sung An; Yoon, Chang Won.

In: Catalysis Letters, Vol. 143, No. 1, 01.01.2013, p. 49-57.

Research output: Contribution to journalArticle

Harshini, D. ; Kim, Yongmin ; Nam, SukWoo ; Lim, Tae Hoon ; Hong, Sung An ; Yoon, Chang Won. / Influence of terbium doping on oxygen storage capacity of Ceria-zirconia supports : Enhanced durability of ni catalysts for propane steam reforming. In: Catalysis Letters. 2013 ; Vol. 143, No. 1. pp. 49-57.
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AU - Hong, Sung An

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AB - Systematic studies were conducted to understand the influence of Tb doping on durability of Ni-based catalysts supported onto Ce0.75-xZr 0.25TbxO2 (CZT x, x = 0.0-0.2), prepared by glycine-nitrate process. Ni metals were deposited onto the as-synthesized supports using a solvothermal method. The prepared supports and catalysts were characterized by a number of ex-situ techniques including X-ray powder diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, H 2-temperature-programmed reduction and Brunauer-Emmett-Teller analyses. These studies along with soot oxidation experiments confirmed that the existence of Tb3+ and/or Ce3+ ions made significant contribution to enhancing oxygen storage capacity (OSC) of the Tb doped CeO 2-ZrO2 based materials, and among all the supports studied, Ce0.65Zr0.25Tb0.1O2 (x = 0.1, CZT 0.1 ) showed the highest OSC. To assess the performance of these catalysts, steam reforming reactions of propane were further carried out on the Ni supported catalysts (Ni/CZT x ) at a steam-to-carbon ratio of 1.5, a gas hourly spaced velocity of 45,000 h-1, and a reaction temperature of 700 C. Consistent with the determined OSC of the catalysts, the durabilities of the Ni/CZT x catalysts were found to be increased in the order of Ni/CZT 0.1 > Ni/CZT 0.15 > Ni/CZT 0.2 > Ni/CZT 0.05 > Ni/CZ. In particular, the activity of Ni/CZT 0.1 was maintained to be >99 % of propane conversion at least for 200 h without significant deactivation. Graphical Abstract: [Figure not available: see fulltext.]

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