Renewable hydrogen by autothermal steam reforming of volatile carbohydrates

P. J. Dauenhauer; J. R. Salge; L. D. Schmidt

doi:10.1016/j.jcat.2006.09.011

Renewable hydrogen by autothermal steam reforming of volatile carbohydrates

P. J. Dauenhauer, J. R. Salge, L. D. Schmidt

Chemical Engineering and Materials Science

Research output: Contribution to journal › Article › peer-review

196 Scopus citations

Abstract

The autothermal reforming of methanol, ethylene glycol, and glycerol and their solutions in water was examined over platinum- and rhodium-based catalysts supported on alumina foams at a contact time of ∼10 ms. Catalyst, washcoat, carbon-to-oxygen ratio, and steam-to-carbon ratio were varied to maximize selectivity to H₂. Rhodium catalysts with the addition of ceria on a γ-Al₂O₃ washcoat layer exhibited the best combination of high fuel conversion and high selectivity to H₂ near equilibrium. Steam addition increased selectivity to H₂ to 89% from methanol, 92% from ethylene glycol, and 79% from glycerol. Selectivity to minor products such as acetaldehyde, ethylene, and methane was <2% at optimum conditions for all experiments. The results are interpreted as occurring primarily through surface reactions initiated by adsorption on metals through hydroxyl oxygen lone pairs to form surface alkoxides, which decompose almost exclusively to H₂ and C₁ carbon compounds.

Original language	English (US)
Pages (from-to)	238-247
Number of pages	10
Journal	Journal of Catalysis
Volume	244
Issue number	2
DOIs	https://doi.org/10.1016/j.jcat.2006.09.011
State	Published - Dec 10 2006

Bibliographical note

Funding Information:
This research was partially supported by grants from the Minnesota Corn Growers Association, the Initiative for Renewable Energy and the Environment at the University of Minnesota, and the U.S. Department of Energy (grant DE-FG02-88ER13878).

Keywords

Autothermal
Carbohydrates
Glycerol
Reforming
Rhodium

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title = "Renewable hydrogen by autothermal steam reforming of volatile carbohydrates",

abstract = "The autothermal reforming of methanol, ethylene glycol, and glycerol and their solutions in water was examined over platinum- and rhodium-based catalysts supported on alumina foams at a contact time of ∼10 ms. Catalyst, washcoat, carbon-to-oxygen ratio, and steam-to-carbon ratio were varied to maximize selectivity to H2. Rhodium catalysts with the addition of ceria on a γ-Al2O3 washcoat layer exhibited the best combination of high fuel conversion and high selectivity to H2 near equilibrium. Steam addition increased selectivity to H2 to 89% from methanol, 92% from ethylene glycol, and 79% from glycerol. Selectivity to minor products such as acetaldehyde, ethylene, and methane was <2% at optimum conditions for all experiments. The results are interpreted as occurring primarily through surface reactions initiated by adsorption on metals through hydroxyl oxygen lone pairs to form surface alkoxides, which decompose almost exclusively to H2 and C1 carbon compounds.",

keywords = "Autothermal, Carbohydrates, Glycerol, Reforming, Rhodium",

author = "Dauenhauer, {P. J.} and Salge, {J. R.} and Schmidt, {L. D.}",

note = "Funding Information: This research was partially supported by grants from the Minnesota Corn Growers Association, the Initiative for Renewable Energy and the Environment at the University of Minnesota, and the U.S. Department of Energy (grant DE-FG02-88ER13878).",

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AU - Salge, J. R.

AU - Schmidt, L. D.

N1 - Funding Information: This research was partially supported by grants from the Minnesota Corn Growers Association, the Initiative for Renewable Energy and the Environment at the University of Minnesota, and the U.S. Department of Energy (grant DE-FG02-88ER13878).

PY - 2006/12/10

Y1 - 2006/12/10

N2 - The autothermal reforming of methanol, ethylene glycol, and glycerol and their solutions in water was examined over platinum- and rhodium-based catalysts supported on alumina foams at a contact time of ∼10 ms. Catalyst, washcoat, carbon-to-oxygen ratio, and steam-to-carbon ratio were varied to maximize selectivity to H2. Rhodium catalysts with the addition of ceria on a γ-Al2O3 washcoat layer exhibited the best combination of high fuel conversion and high selectivity to H2 near equilibrium. Steam addition increased selectivity to H2 to 89% from methanol, 92% from ethylene glycol, and 79% from glycerol. Selectivity to minor products such as acetaldehyde, ethylene, and methane was <2% at optimum conditions for all experiments. The results are interpreted as occurring primarily through surface reactions initiated by adsorption on metals through hydroxyl oxygen lone pairs to form surface alkoxides, which decompose almost exclusively to H2 and C1 carbon compounds.

AB - The autothermal reforming of methanol, ethylene glycol, and glycerol and their solutions in water was examined over platinum- and rhodium-based catalysts supported on alumina foams at a contact time of ∼10 ms. Catalyst, washcoat, carbon-to-oxygen ratio, and steam-to-carbon ratio were varied to maximize selectivity to H2. Rhodium catalysts with the addition of ceria on a γ-Al2O3 washcoat layer exhibited the best combination of high fuel conversion and high selectivity to H2 near equilibrium. Steam addition increased selectivity to H2 to 89% from methanol, 92% from ethylene glycol, and 79% from glycerol. Selectivity to minor products such as acetaldehyde, ethylene, and methane was <2% at optimum conditions for all experiments. The results are interpreted as occurring primarily through surface reactions initiated by adsorption on metals through hydroxyl oxygen lone pairs to form surface alkoxides, which decompose almost exclusively to H2 and C1 carbon compounds.

KW - Autothermal

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KW - Reforming

KW - Rhodium

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Renewable hydrogen by autothermal steam reforming of volatile carbohydrates

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