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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 Rhcatalyst demonstrated much better sulfur tolerance than the Nicatalyst. XANES revealed that there are various sulfur species (metal sulfide, sulfonate, sulfate and organic sulfide) on the used Ni and Rhcatalysts. Metal sulfide and organic sulfide are the dominant sulfur species on the Nicatalyst whereas sulfonate and sulfate predominate on the Rhcatalyst. 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 carboxylgroups 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 Nicatalyst by metal sulfide formation in the first few hours while build-up of carbon deposits contributesmore » mainly to the subsequent deactivation.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL) National Synchrotron Light Source
Sponsoring Org.:
DOE - OFFICE OF SCIENCE
OSTI Identifier:
1020021
Report Number(s):
BNL-95867-2011-JA
Journal ID: ISSN 1463-9076; TRN: US201116%%5
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Physical Chemistry Chemical Physics
Additional Journal Information:
Journal Volume: 12; Journal Issue: 21; 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; national synchrotron light source

Citation Formats

Chen, Y, Xie, C, Li, Y, Song, C, and Bolin, T. 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. 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, and Bolin, T. Fri . "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_1020021,
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},
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 Rhcatalyst demonstrated much better sulfur tolerance than the Nicatalyst. XANES revealed that there are various sulfur species (metal sulfide, sulfonate, sulfate and organic sulfide) on the used Ni and Rhcatalysts. Metal sulfide and organic sulfide are the dominant sulfur species on the Nicatalyst whereas sulfonate and sulfate predominate on the Rhcatalyst. 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 carboxylgroups 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 Nicatalyst 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 = {Physical Chemistry Chemical Physics},
issn = {1463-9076},
number = 21,
volume = 12,
place = {United States},
year = {2010},
month = {1}
}