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Title: Sulfur poisoning mechanism of steam reforming catalysts : an X-ray absorption near edge structure (XANES) spectroscopic study.

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. CeO{sub 2}-Al{sub 2}O{sub 3}-supported Ni and Rh-based catalysts were tested in steam reforming of liquid hydrocarbon fuel containing 350 ppm sulfur for H{sub 2} 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 fewmore » hours while build-up of carbon deposits contributes mainly to the subsequent deactivation.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
ONR; USDOE Office of Science (SC); National Science Foundation (NSF)
OSTI Identifier:
993396
Report Number(s):
ANL/XSD/JA-68409
Journal ID: ISSN 1463-9076; TRN: US201023%%326
DOE Contract Number:  
DE-AC02-06CH11357
Resource Type:
Journal Article
Journal Name:
Phys. Chem. Chem. Phys.
Additional Journal Information:
Journal Volume: 12; Journal Issue: Apr. 29, 2010; Journal ID: ISSN 1463-9076
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION; CARBON; CATALYSTS; DEACTIVATION; HYDROCARBONS; NICKEL SULFIDES; POISONING; PRODUCTION; STEAM; SULFATES; SULFIDES; SULFONATES; SULFUR; TOLERANCE

Citation Formats

Chen, Y, Xie, C, Li, Y, Song, C, Bolin, T, X-Ray Science Division, and Pennsylvania State Univ. Sulfur poisoning mechanism of steam reforming catalysts : an X-ray absorption near edge structure (XANES) spectroscopic study.. United States: N. p., 2010. Web. doi:10.1039/b925910b.
Chen, Y, Xie, C, Li, Y, Song, C, Bolin, T, X-Ray Science Division, & Pennsylvania State Univ. Sulfur poisoning mechanism of steam reforming catalysts : an X-ray absorption near edge structure (XANES) spectroscopic study.. United States. doi:10.1039/b925910b.
Chen, Y, Xie, C, Li, Y, Song, C, Bolin, T, X-Ray Science Division, and Pennsylvania State Univ. Thu . "Sulfur poisoning mechanism of steam reforming catalysts : an X-ray absorption near edge structure (XANES) spectroscopic study.". United States. doi:10.1039/b925910b.
@article{osti_993396,
title = {Sulfur poisoning mechanism of steam reforming catalysts : an X-ray absorption near edge structure (XANES) spectroscopic study.},
author = {Chen, Y and Xie, C and Li, Y and Song, C and Bolin, T and X-Ray Science Division and Pennsylvania State Univ.},
abstractNote = {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. CeO{sub 2}-Al{sub 2}O{sub 3}-supported Ni and Rh-based catalysts were tested in steam reforming of liquid hydrocarbon fuel containing 350 ppm sulfur for H{sub 2} 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.},
doi = {10.1039/b925910b},
journal = {Phys. Chem. Chem. Phys.},
issn = {1463-9076},
number = Apr. 29, 2010,
volume = 12,
place = {United States},
year = {2010},
month = {4}
}