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Title: Understanding Sulfur Poisoning and Regeneration of Nickel Biomass Conditioning Catalysts using X-Ray Absorption Spectroscopy

Abstract

The production of biofuels can proceed via a biomass gasification to produce syngas, which can then undergo catalytic conditioning and reforming reactions prior to being sent to a fuel synthesis reactor. Catalysts used for biomass conditioning are plagued by short lifetimes which are a result of, among other things, poisoning. Syngas produced from biomass gasification may contain between 30-300 ppm H2S, depending on the feedstock and gasification conditions, and H2S is a key catalyst poison. In order to overcome catalyst poisoning, either an H2S-tolerant catalyst or an efficient regeneration protocol should be employed. In this study, sulfur K-edge X-ray absorption near edge spectroscopy (XANES) was used to monitor sulfur species on spent catalyst samples and the transformation of these species from sulfides to sulfates during steam and air regeneration on a Ni/Mg/K/Al2O3 catalyst used to condition biomass-derived syngas. Additionally, nickel K-edge EXAFS and XANES are used to examine the state of nickel species on the catalysts. Post-reaction samples showed the presence of sulfides on the H2S-poisoned nickel catalyst and although some gaseous sulfur species were observed to leave the catalyst bed during regeneration, sulfur remained on the catalyst and a transformation from sulfides to sulfates was observed. The subsequent H2more » reduction led to a partial reduction of sulfates back to sulfides. A proposed reaction sequence is presented and recommended regeneration strategies are discussed.« less

Authors:
; ;
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy Biomass Program
OSTI Identifier:
1087205
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Conference
Resource Relation:
Conference: American Chemical Society. Abstracts of Papers of the 245th ACS National Meeting, 7-11 April 2013, New Orleans, Louisiana; Related Information: Abstract No. CATL-130
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES; Bioenergy

Citation Formats

Yung, M. M., Cheah, S., and Kuhn, J. N. Understanding Sulfur Poisoning and Regeneration of Nickel Biomass Conditioning Catalysts using X-Ray Absorption Spectroscopy. United States: N. p., 2013. Web.
Yung, M. M., Cheah, S., & Kuhn, J. N. Understanding Sulfur Poisoning and Regeneration of Nickel Biomass Conditioning Catalysts using X-Ray Absorption Spectroscopy. United States.
Yung, M. M., Cheah, S., and Kuhn, J. N. Tue . "Understanding Sulfur Poisoning and Regeneration of Nickel Biomass Conditioning Catalysts using X-Ray Absorption Spectroscopy". United States.
@article{osti_1087205,
title = {Understanding Sulfur Poisoning and Regeneration of Nickel Biomass Conditioning Catalysts using X-Ray Absorption Spectroscopy},
author = {Yung, M. M. and Cheah, S. and Kuhn, J. N.},
abstractNote = {The production of biofuels can proceed via a biomass gasification to produce syngas, which can then undergo catalytic conditioning and reforming reactions prior to being sent to a fuel synthesis reactor. Catalysts used for biomass conditioning are plagued by short lifetimes which are a result of, among other things, poisoning. Syngas produced from biomass gasification may contain between 30-300 ppm H2S, depending on the feedstock and gasification conditions, and H2S is a key catalyst poison. In order to overcome catalyst poisoning, either an H2S-tolerant catalyst or an efficient regeneration protocol should be employed. In this study, sulfur K-edge X-ray absorption near edge spectroscopy (XANES) was used to monitor sulfur species on spent catalyst samples and the transformation of these species from sulfides to sulfates during steam and air regeneration on a Ni/Mg/K/Al2O3 catalyst used to condition biomass-derived syngas. Additionally, nickel K-edge EXAFS and XANES are used to examine the state of nickel species on the catalysts. Post-reaction samples showed the presence of sulfides on the H2S-poisoned nickel catalyst and although some gaseous sulfur species were observed to leave the catalyst bed during regeneration, sulfur remained on the catalyst and a transformation from sulfides to sulfates was observed. The subsequent H2 reduction led to a partial reduction of sulfates back to sulfides. A proposed reaction sequence is presented and recommended regeneration strategies are discussed.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2013},
month = {1}
}

Conference:
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