Sulfur poisoning mechanism of steam reforming catalysts

An X-ray absorption near edge structure (XANES) spectroscopic study

Yongsheng Chen, Chao Xie, Yan Li, Chunshan Song, Trudy B. Bolin

Research output: Contribution to journalArticle

48 Citations (Scopus)

Abstract

The present XANES study aims at elucidating the roles of carbon deposits and metal sulfides in the catalyst deactivation in steam reforming reactions with the presence of sulfur. CeO2-Al2O3- supported Ni and Rh-based catalysts were tested in steam reforming of liquid hydrocarbon fuel containing 350 ppm sulfur for H2 production at 800 °C. The Rh catalyst demonstrated much better sulfur tolerance than the Ni catalyst. XANES revealed that there are various sulfur species (metal sulfide, sulfonate, sulfate and organic sulfide) on the used Ni and Rh catalysts. Metal sulfide and organic sulfide are the dominant sulfur species on the Ni catalyst whereas sulfonate and sulfate predominate on the Rh catalyst. Meanwhile organic sulfide and sulfate are also observed on the support alone. Furthermore, there are more carbon deposits formed in the presence of sulfur on both catalysts. More carboxyl groups occur on the carbon deposits formed on the same catalyst when there is no sulfur in the fuel. From correlation analysis of the amounts of nickel sulfide and carbon deposits along with the relative catalytic activity loss, we conclude that sulfur causes the initial deactivation of the Ni catalyst by metal sulfide formation in the first few hours while build-up of carbon deposits contributes mainly to the subsequent deactivation.

Original languageEnglish (US)
Pages (from-to)5707-5711
Number of pages5
JournalPhysical Chemistry Chemical Physics
Volume12
Issue number21
DOIs
StatePublished - Jun 7 2010

Fingerprint

Catalyst poisoning
poisoning
Steam reforming
X ray absorption
Sulfur
steam
Sulfides
sulfur
sulfides
catalysts
Catalysts
Carbon
Deposits
x rays
deposits
Metals
carbon
deactivation
sulfates
sulfonates

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

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abstract = "The present XANES study aims at elucidating the roles of carbon deposits and metal sulfides in the catalyst deactivation in steam reforming reactions with the presence of sulfur. CeO2-Al2O3- supported Ni and Rh-based catalysts were tested in steam reforming of liquid hydrocarbon fuel containing 350 ppm sulfur for H2 production at 800 °C. The Rh catalyst demonstrated much better sulfur tolerance than the Ni catalyst. XANES revealed that there are various sulfur species (metal sulfide, sulfonate, sulfate and organic sulfide) on the used Ni and Rh catalysts. Metal sulfide and organic sulfide are the dominant sulfur species on the Ni catalyst whereas sulfonate and sulfate predominate on the Rh catalyst. Meanwhile organic sulfide and sulfate are also observed on the support alone. Furthermore, there are more carbon deposits formed in the presence of sulfur on both catalysts. More carboxyl groups occur on the carbon deposits formed on the same catalyst when there is no sulfur in the fuel. From correlation analysis of the amounts of nickel sulfide and carbon deposits along with the relative catalytic activity loss, we conclude that sulfur causes the initial deactivation of the Ni catalyst by metal sulfide formation in the first few hours while build-up of carbon deposits contributes mainly to the subsequent deactivation.",
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Sulfur poisoning mechanism of steam reforming catalysts : An X-ray absorption near edge structure (XANES) spectroscopic study. / Chen, Yongsheng; Xie, Chao; Li, Yan; Song, Chunshan; Bolin, Trudy B.

In: Physical Chemistry Chemical Physics, Vol. 12, No. 21, 07.06.2010, p. 5707-5711.

Research output: Contribution to journalArticle

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