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Title: Aqueous Phase Reforming of Glycerol for Hydrogen Production Over Pt-Re Supported on Carbon

Abstract

Hydrogen production from the aqueous phase reforming of glycerol over several 3%Pt-Re/C catalysts (1-4.5% Re) has been studied in the absence and presence of base, and the results compared with a Re-free 3%Pt/C catalyst. Although the Pt/C catalyst is very selective toward the production of hydrogen, catalytic activity is low. Addition of Re significantly increases the conversion of glycerol, at some loss of hydrogen selectivity to light hydrocarbons and water-soluble oxygenates. Addition of 1%KOH to the feedstock increases the selectivity of the Pt-Re/C catalysts toward hydrogen, but selectivity toward aqueous phase oxygenates also increases except for 3%Pt-3%Re/C, where it remains constant. The increase in hydrogen selectivity with base addition arises primarily from reducing the selectivity toward methane and higher alkanes, products that consume H2. For comparison, KOH addition to the glycerol feed with the Re-free 3%Pt/C catalyst provides an increase in glycerol conversion but results in a decline in both H2 and alkanes relative to aqueous phase oxygenates. This indicates that alternative pathways have been enabled by base addition. The highest hydrogen productivity among the catalysts tested is achieved with a 3%Pt-3%Re/C catalyst with added KOH base, but this hydrogen productivity declines with time on stream. The observed product distributionsmore » as well as deactivation with base can be understood in terms of the different reaction pathways that become emphasized depending on catalyst composition and pH.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
992358
Report Number(s):
PNNL-SA-71141
Journal ID: ISSN 0926-3373; ACBEE3; EB4201000; TRN: US201022%%284
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Applied Catalysis. B, Environmental, 99(1-2):206-213
Additional Journal Information:
Journal Volume: 99; Journal Issue: 1-2; Journal ID: ISSN 0926-3373
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 03 NATURAL GAS; ALKANES; CARBON; CATALYSTS; DEACTIVATION; GLYCEROL; HYDROCARBONS; HYDROGEN; HYDROGEN PRODUCTION; METHANE; PRODUCTION; PRODUCTIVITY

Citation Formats

King, David L, Zhang, Liang, Xia, Guanguang, Karim, Ayman M, Heldebrant, David J, Wang, Xianqin, Peterson, Thomas H, and Wang, Yong. Aqueous Phase Reforming of Glycerol for Hydrogen Production Over Pt-Re Supported on Carbon. United States: N. p., 2010. Web. doi:10.1016/j.apcatb.2010.06.021.
King, David L, Zhang, Liang, Xia, Guanguang, Karim, Ayman M, Heldebrant, David J, Wang, Xianqin, Peterson, Thomas H, & Wang, Yong. Aqueous Phase Reforming of Glycerol for Hydrogen Production Over Pt-Re Supported on Carbon. United States. doi:10.1016/j.apcatb.2010.06.021.
King, David L, Zhang, Liang, Xia, Guanguang, Karim, Ayman M, Heldebrant, David J, Wang, Xianqin, Peterson, Thomas H, and Wang, Yong. Tue . "Aqueous Phase Reforming of Glycerol for Hydrogen Production Over Pt-Re Supported on Carbon". United States. doi:10.1016/j.apcatb.2010.06.021.
@article{osti_992358,
title = {Aqueous Phase Reforming of Glycerol for Hydrogen Production Over Pt-Re Supported on Carbon},
author = {King, David L and Zhang, Liang and Xia, Guanguang and Karim, Ayman M and Heldebrant, David J and Wang, Xianqin and Peterson, Thomas H and Wang, Yong},
abstractNote = {Hydrogen production from the aqueous phase reforming of glycerol over several 3%Pt-Re/C catalysts (1-4.5% Re) has been studied in the absence and presence of base, and the results compared with a Re-free 3%Pt/C catalyst. Although the Pt/C catalyst is very selective toward the production of hydrogen, catalytic activity is low. Addition of Re significantly increases the conversion of glycerol, at some loss of hydrogen selectivity to light hydrocarbons and water-soluble oxygenates. Addition of 1%KOH to the feedstock increases the selectivity of the Pt-Re/C catalysts toward hydrogen, but selectivity toward aqueous phase oxygenates also increases except for 3%Pt-3%Re/C, where it remains constant. The increase in hydrogen selectivity with base addition arises primarily from reducing the selectivity toward methane and higher alkanes, products that consume H2. For comparison, KOH addition to the glycerol feed with the Re-free 3%Pt/C catalyst provides an increase in glycerol conversion but results in a decline in both H2 and alkanes relative to aqueous phase oxygenates. This indicates that alternative pathways have been enabled by base addition. The highest hydrogen productivity among the catalysts tested is achieved with a 3%Pt-3%Re/C catalyst with added KOH base, but this hydrogen productivity declines with time on stream. The observed product distributions as well as deactivation with base can be understood in terms of the different reaction pathways that become emphasized depending on catalyst composition and pH.},
doi = {10.1016/j.apcatb.2010.06.021},
journal = {Applied Catalysis. B, Environmental, 99(1-2):206-213},
issn = {0926-3373},
number = 1-2,
volume = 99,
place = {United States},
year = {2010},
month = {3}
}