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Title: Influence of Sulfur on the Carbon Deposition in Liquid Hydrocarbon Steam Reforming over CeO2-Al2O3 supported Ni and Rh Catalysts

Abstract

This study was performed to elucidate the influence of sulfur on the carbon deposition in steam reforming of liquid hydrocarbons over CeO{sub 2}-Al{sub 2}O{sub 3} supported Ni and Rh catalysts at 800 C. The characteristics of the carbon deposits on the used catalysts after the reactions without and with sulfur were investigated by temperature-programmed oxidation (TPO), transmission electron microscopy (TEM), scanning transmission X-ray microscopy (STXM), temperature-programmed hydrogenation (TPH), X-ray absorption near edge structure (XANES), and scanning electron microscopy (SEM). Though abundant carbon deposits can accumulate on the pure CeO{sub 2}-Al{sub 2}O{sub 3} support due to fuel thermal cracking, the addition of Ni or Rh metal greatly reduced the carbon deposition in the sulfur-free reaction. The presence of sulfur increased the carbon deposition on both catalysts, which has a much more significant impact for the Ni catalyst. Carbon XANES study on the used catalysts revealed that graphitic carbon was dominant in the presence of sulfur, while oxidized carbon species (quinone-like carbon, carboxyl and carbonate) prevailed without sulfur. Meanwhile, the formation of carboxyl and carbonate more dramatically dropped on the Ni catalyst than that on the Rh catalyst. Our results strongly suggest that (I) the presence of sulfur can suppress carbon gasificationmore » and promote the formation of graphitic carbon on reforming catalysts due mainly to its poisoning effect on metals, and (II) Rh catalyst possesses stronger capability to maintain carbon gasification activity than Ni catalyst in the presence of sulfur.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE SC OFFICE OF SCIENCE (SC)
OSTI Identifier:
1041804
Report Number(s):
BNL-97482-2012-JA
Journal ID: ISSN 0926-860X; TRN: US201212%%216
DOE Contract Number:  
DE-AC02-98CH10886
Resource Type:
Journal Article
Journal Name:
Applied Catalysis A: General
Additional Journal Information:
Journal Volume: 394; Journal Issue: 1/2; Journal ID: ISSN 0926-860X
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ALUMINIUM OXIDES; CARBON; CARBON OXIDES; CARBONATES; CATALYSTS; DEPOSITION; DEPOSITS; FUELS; GASIFICATION; HYDROCARBONS; HYDROGENATION; LIQUIDS; METALS; MICROSCOPY; NICKEL; OXIDATION; POISONING; RHODIUM; SCANNING ELECTRON MICROSCOPY; STEAM REFORMER PROCESSES; SULFUR; TEMPERATURE DEPENDENCE; THERMAL CRACKING; TRANSMISSION ELECTRON MICROSCOPY

Citation Formats

Xie, C, Chen, Y, Li, Y, Wang, X, and Song, C. Influence of Sulfur on the Carbon Deposition in Liquid Hydrocarbon Steam Reforming over CeO2-Al2O3 supported Ni and Rh Catalysts. United States: N. p., 2011. Web. doi:10.1016/j.apcata.2010.12.019.
Xie, C, Chen, Y, Li, Y, Wang, X, & Song, C. Influence of Sulfur on the Carbon Deposition in Liquid Hydrocarbon Steam Reforming over CeO2-Al2O3 supported Ni and Rh Catalysts. United States. doi:10.1016/j.apcata.2010.12.019.
Xie, C, Chen, Y, Li, Y, Wang, X, and Song, C. Sat . "Influence of Sulfur on the Carbon Deposition in Liquid Hydrocarbon Steam Reforming over CeO2-Al2O3 supported Ni and Rh Catalysts". United States. doi:10.1016/j.apcata.2010.12.019.
@article{osti_1041804,
title = {Influence of Sulfur on the Carbon Deposition in Liquid Hydrocarbon Steam Reforming over CeO2-Al2O3 supported Ni and Rh Catalysts},
author = {Xie, C and Chen, Y and Li, Y and Wang, X and Song, C},
abstractNote = {This study was performed to elucidate the influence of sulfur on the carbon deposition in steam reforming of liquid hydrocarbons over CeO{sub 2}-Al{sub 2}O{sub 3} supported Ni and Rh catalysts at 800 C. The characteristics of the carbon deposits on the used catalysts after the reactions without and with sulfur were investigated by temperature-programmed oxidation (TPO), transmission electron microscopy (TEM), scanning transmission X-ray microscopy (STXM), temperature-programmed hydrogenation (TPH), X-ray absorption near edge structure (XANES), and scanning electron microscopy (SEM). Though abundant carbon deposits can accumulate on the pure CeO{sub 2}-Al{sub 2}O{sub 3} support due to fuel thermal cracking, the addition of Ni or Rh metal greatly reduced the carbon deposition in the sulfur-free reaction. The presence of sulfur increased the carbon deposition on both catalysts, which has a much more significant impact for the Ni catalyst. Carbon XANES study on the used catalysts revealed that graphitic carbon was dominant in the presence of sulfur, while oxidized carbon species (quinone-like carbon, carboxyl and carbonate) prevailed without sulfur. Meanwhile, the formation of carboxyl and carbonate more dramatically dropped on the Ni catalyst than that on the Rh catalyst. Our results strongly suggest that (I) the presence of sulfur can suppress carbon gasification and promote the formation of graphitic carbon on reforming catalysts due mainly to its poisoning effect on metals, and (II) Rh catalyst possesses stronger capability to maintain carbon gasification activity than Ni catalyst in the presence of sulfur.},
doi = {10.1016/j.apcata.2010.12.019},
journal = {Applied Catalysis A: General},
issn = {0926-860X},
number = 1/2,
volume = 394,
place = {United States},
year = {2011},
month = {12}
}