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Title: Experimental and computational investigations of sulfur-resistant bimetallic catalysts for reforming of biomass gasification products

Abstract

A combination of density functional theory (DFT) calculations and experimental studies of supported catalysts was used to identify H{sub 2}S-resistant biomass gasification product reforming catalysts. DFT calculations were used to search for bimetallic, nickel-based (1 1 1) surfaces with lower sulfur adsorption energies and enhanced ethylene adsorption energies. These metrics were used as predictors for H{sub 2}S resistance and activity toward steam reforming of ethylene, respectively. Relative to Ni, DFT studies found that the Ni/Sn surface alloy exhibited enhanced sulfur resistance and the Ni/Ru system exhibited an improved ethylene binding energy with a small increase in sulfur binding energy. A series of supported bimetallic nickel catalysts was prepared and screened under model ethylene reforming conditions and simulated biomass tar reforming conditions. The observed experimental trends in activity were consistent with theoretical predictions, with observed reforming activities in the order Ni/Ru > Ni > Ni/Sn. Interestingly, Ni/Ru showed a high level of resistance to sulfur poisoning compared with Ni. This sulfur resistance can be partly explained by trends in sulfur versus ethylene binding energy at different types of sites across the bimetallic surface.

Authors:
; ;  [1]
  1. NREL
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
OTHERDOE - OTHER
OSTI Identifier:
1024495
Resource Type:
Journal Article
Journal Name:
J. Catal.
Additional Journal Information:
Journal Volume: 282; Journal Issue: (2) ; 09, 2011; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
ENGLISH
Subject:
09 BIOMASS FUELS; ADSORPTION; ALLOYS; BINDING ENERGY; BIOMASS; CATALYSTS; ETHYLENE; FUNCTIONALS; GASIFICATION; METRICS; NICKEL; POISONING; STEAM; SULFUR; TAR

Citation Formats

Rangan, Meghana, Yung, Matthew M, Medlin, J William, and Colorado). Experimental and computational investigations of sulfur-resistant bimetallic catalysts for reforming of biomass gasification products. United States: N. p., 2011. Web. doi:10.1016/j.jcat.2011.06.009.
Rangan, Meghana, Yung, Matthew M, Medlin, J William, & Colorado). Experimental and computational investigations of sulfur-resistant bimetallic catalysts for reforming of biomass gasification products. United States. https://doi.org/10.1016/j.jcat.2011.06.009
Rangan, Meghana, Yung, Matthew M, Medlin, J William, and Colorado). 2011. "Experimental and computational investigations of sulfur-resistant bimetallic catalysts for reforming of biomass gasification products". United States. https://doi.org/10.1016/j.jcat.2011.06.009.
@article{osti_1024495,
title = {Experimental and computational investigations of sulfur-resistant bimetallic catalysts for reforming of biomass gasification products},
author = {Rangan, Meghana and Yung, Matthew M and Medlin, J William and Colorado)},
abstractNote = {A combination of density functional theory (DFT) calculations and experimental studies of supported catalysts was used to identify H{sub 2}S-resistant biomass gasification product reforming catalysts. DFT calculations were used to search for bimetallic, nickel-based (1 1 1) surfaces with lower sulfur adsorption energies and enhanced ethylene adsorption energies. These metrics were used as predictors for H{sub 2}S resistance and activity toward steam reforming of ethylene, respectively. Relative to Ni, DFT studies found that the Ni/Sn surface alloy exhibited enhanced sulfur resistance and the Ni/Ru system exhibited an improved ethylene binding energy with a small increase in sulfur binding energy. A series of supported bimetallic nickel catalysts was prepared and screened under model ethylene reforming conditions and simulated biomass tar reforming conditions. The observed experimental trends in activity were consistent with theoretical predictions, with observed reforming activities in the order Ni/Ru > Ni > Ni/Sn. Interestingly, Ni/Ru showed a high level of resistance to sulfur poisoning compared with Ni. This sulfur resistance can be partly explained by trends in sulfur versus ethylene binding energy at different types of sites across the bimetallic surface.},
doi = {10.1016/j.jcat.2011.06.009},
url = {https://www.osti.gov/biblio/1024495}, journal = {J. Catal.},
issn = {0021-9517},
number = (2) ; 09, 2011,
volume = 282,
place = {United States},
year = {Thu Nov 17 00:00:00 EST 2011},
month = {Thu Nov 17 00:00:00 EST 2011}
}