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Title: Comparative Study on the Sulfur Tolerance and Carbon Resistance of Supported Noble Metal Catalysts in Steam Reforming of Liquid Hydrocarbon Fuel

Abstract

This work was conducted to clarify the influence of the type of metal and support on the sulfur tolerance and carbon resistance of supported noble metal catalysts in steam reforming of liquid hydrocarbons. Al2O3-supported noble metal catalysts (Rh, Ru, Pt, and Pd), Rh catalysts on different supports (Al2O3, CeO2, SiO2, and MgO), and Pt catalyst supported on CeO2 and Al2O3, were examined for steam reforming of a liquid hydrocarbon fuel (Norpar13 from Exxon Mobil) at 800 C for 55 h. The results indicate that (1) Rh/Al2O3 shows higher sulfur tolerance than the Ru, Pt, and Pd catalysts on the same support; (2) both Al2O3 and CeO2 are promising supports for Rh catalyst to process sulfur-containing hydrocarbons; and (3) Pt/CeO2 exhibits better catalytic performance than Pt/Al2O3 in the reaction with sulfur. TEM results demonstrate that the metal particles in Rh/Al2O3 were better dispersed (mostly in 1-3 nm) compared with the other catalysts after reforming the sulfur-containing feed. As revealed by XPS, the binding energy of Rh 3d for Rh/Al2O3 is notably higher than that for Rh/CeO2, implying the formation of electron-deficient Rh particles in the former. The strong sulfur tolerance of Rh/Al2O3 may be related to the formation of well-dispersed electron-deficientmore » Rh particles on the Al2O3 support. Sulfur K-edge XANES illustrates the preferential formation of sulfonate and sulfate on Rh/Al2O3, which is believed to be beneficial for improving its sulfur tolerance as their oxygen-shielded sulfur structure may hinder direct Rh-S interaction. Due to its strong sulfur tolerance, the carbon deposition on Rh/Al2O3 was significantly lower than that on the Al2O3-supported Ru, Pt, and Pd catalysts after the reaction with sulfur. The superior catalytic performance of CeO2-supported Rh and Pt catalysts in the presence of sulfur can be ascribed mainly to the promotion effect of CeO2 on carbon gasification, leading to much lower carbon deposition compared with the Rh/Al2O3, Rh/MgO, Rh/SiO2 and Pt/Al2O3 catalysts.« less

Authors:
; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1047404
Report Number(s):
PNNL-SA-84935
37791; KP1704020; TRN: US201216%%263
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 2; Journal Issue: 6
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; BINDING ENERGY; CARBON; CATALYSTS; DEPOSITION; FUELS; GASIFICATION; HYDROCARBONS; LIQUIDS; METALS; PARTICLES; PERFORMANCE; STEAM REFORMER PROCESSES; SULFATES; SULFONATES; SULFUR; TOLERANCE; X-RAY PHOTOELECTRON SPECTROSCOPY; Environmental Molecular Sciences Laboratory

Citation Formats

Xie, Chao, Chen, Yongsheng, Engelhard, Mark H, and Song, Chunshan. Comparative Study on the Sulfur Tolerance and Carbon Resistance of Supported Noble Metal Catalysts in Steam Reforming of Liquid Hydrocarbon Fuel. United States: N. p., 2012. Web. doi:10.1021/cs200695t.
Xie, Chao, Chen, Yongsheng, Engelhard, Mark H, & Song, Chunshan. Comparative Study on the Sulfur Tolerance and Carbon Resistance of Supported Noble Metal Catalysts in Steam Reforming of Liquid Hydrocarbon Fuel. United States. doi:10.1021/cs200695t.
Xie, Chao, Chen, Yongsheng, Engelhard, Mark H, and Song, Chunshan. Wed . "Comparative Study on the Sulfur Tolerance and Carbon Resistance of Supported Noble Metal Catalysts in Steam Reforming of Liquid Hydrocarbon Fuel". United States. doi:10.1021/cs200695t.
@article{osti_1047404,
title = {Comparative Study on the Sulfur Tolerance and Carbon Resistance of Supported Noble Metal Catalysts in Steam Reforming of Liquid Hydrocarbon Fuel},
author = {Xie, Chao and Chen, Yongsheng and Engelhard, Mark H and Song, Chunshan},
abstractNote = {This work was conducted to clarify the influence of the type of metal and support on the sulfur tolerance and carbon resistance of supported noble metal catalysts in steam reforming of liquid hydrocarbons. Al2O3-supported noble metal catalysts (Rh, Ru, Pt, and Pd), Rh catalysts on different supports (Al2O3, CeO2, SiO2, and MgO), and Pt catalyst supported on CeO2 and Al2O3, were examined for steam reforming of a liquid hydrocarbon fuel (Norpar13 from Exxon Mobil) at 800 C for 55 h. The results indicate that (1) Rh/Al2O3 shows higher sulfur tolerance than the Ru, Pt, and Pd catalysts on the same support; (2) both Al2O3 and CeO2 are promising supports for Rh catalyst to process sulfur-containing hydrocarbons; and (3) Pt/CeO2 exhibits better catalytic performance than Pt/Al2O3 in the reaction with sulfur. TEM results demonstrate that the metal particles in Rh/Al2O3 were better dispersed (mostly in 1-3 nm) compared with the other catalysts after reforming the sulfur-containing feed. As revealed by XPS, the binding energy of Rh 3d for Rh/Al2O3 is notably higher than that for Rh/CeO2, implying the formation of electron-deficient Rh particles in the former. The strong sulfur tolerance of Rh/Al2O3 may be related to the formation of well-dispersed electron-deficient Rh particles on the Al2O3 support. Sulfur K-edge XANES illustrates the preferential formation of sulfonate and sulfate on Rh/Al2O3, which is believed to be beneficial for improving its sulfur tolerance as their oxygen-shielded sulfur structure may hinder direct Rh-S interaction. Due to its strong sulfur tolerance, the carbon deposition on Rh/Al2O3 was significantly lower than that on the Al2O3-supported Ru, Pt, and Pd catalysts after the reaction with sulfur. The superior catalytic performance of CeO2-supported Rh and Pt catalysts in the presence of sulfur can be ascribed mainly to the promotion effect of CeO2 on carbon gasification, leading to much lower carbon deposition compared with the Rh/Al2O3, Rh/MgO, Rh/SiO2 and Pt/Al2O3 catalysts.},
doi = {10.1021/cs200695t},
journal = {ACS Catalysis},
number = 6,
volume = 2,
place = {United States},
year = {2012},
month = {4}
}