Catalysis during methanol gasification in supercritical water

Gregory J. DiLeo, Phillip E. Savage

Research output: Contribution to journalArticle

51 Citations (Scopus)

Abstract

We report on the effect of nickel metal on the gasification of methanol in supercritical water at 500 and 550 °C. The reactions were conducted in sealed quartz tubes, which allowed the homogeneous and heterogeneous rates to be quantified separately for the first time. In the absence of nickel, conversions up to 20% were reached after 2 h. The pseudo-first-order rate constant for homogeneous gasification is 4.0 ± 2.7 × 10-5 s-1 at 550 °C. In the presence of a Ni wire that ran the entire length of the reactor, conversions of up to 90% were reached in less than 5 min. The pseudo-first-order rate constants for Ni-catalyzed gasification are 0.0032 ± 0.0013 and 0.0040 ± 0.0012 cm/s at 500 and 550 °C. These results show that homogeneous, uncatalyzed gasification in supercritical water is slow, but rates are greatly increased by added Ni. Hydrogen, carbon monoxide and carbon dioxide were the major products detected. Hydrogen was always the most abundant. With multiple uses, the Ni wire showed deactivation as a catalyst for methanol gasification.

Original languageEnglish (US)
Pages (from-to)228-232
Number of pages5
JournalJournal of Supercritical Fluids
Volume39
Issue number2
DOIs
StatePublished - Dec 1 2006

Fingerprint

gasification
Gasification
Catalysis
catalysis
Methanol
methyl alcohol
Water
water
Nickel
Hydrogen
Rate constants
nickel
wire
Wire
Quartz
hydrogen
Carbon Monoxide
dioxides
Carbon Dioxide
Carbon monoxide

All Science Journal Classification (ASJC) codes

  • Chemical Engineering(all)
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry

Cite this

@article{79902a73cbc44ba5a25725793ec6fc44,
title = "Catalysis during methanol gasification in supercritical water",
abstract = "We report on the effect of nickel metal on the gasification of methanol in supercritical water at 500 and 550 °C. The reactions were conducted in sealed quartz tubes, which allowed the homogeneous and heterogeneous rates to be quantified separately for the first time. In the absence of nickel, conversions up to 20{\%} were reached after 2 h. The pseudo-first-order rate constant for homogeneous gasification is 4.0 ± 2.7 × 10-5 s-1 at 550 °C. In the presence of a Ni wire that ran the entire length of the reactor, conversions of up to 90{\%} were reached in less than 5 min. The pseudo-first-order rate constants for Ni-catalyzed gasification are 0.0032 ± 0.0013 and 0.0040 ± 0.0012 cm/s at 500 and 550 °C. These results show that homogeneous, uncatalyzed gasification in supercritical water is slow, but rates are greatly increased by added Ni. Hydrogen, carbon monoxide and carbon dioxide were the major products detected. Hydrogen was always the most abundant. With multiple uses, the Ni wire showed deactivation as a catalyst for methanol gasification.",
author = "DiLeo, {Gregory J.} and Savage, {Phillip E.}",
year = "2006",
month = "12",
day = "1",
doi = "10.1016/j.supflu.2006.01.004",
language = "English (US)",
volume = "39",
pages = "228--232",
journal = "Journal of Supercritical Fluids",
issn = "0896-8446",
publisher = "Elsevier",
number = "2",

}

Catalysis during methanol gasification in supercritical water. / DiLeo, Gregory J.; Savage, Phillip E.

In: Journal of Supercritical Fluids, Vol. 39, No. 2, 01.12.2006, p. 228-232.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Catalysis during methanol gasification in supercritical water

AU - DiLeo, Gregory J.

AU - Savage, Phillip E.

PY - 2006/12/1

Y1 - 2006/12/1

N2 - We report on the effect of nickel metal on the gasification of methanol in supercritical water at 500 and 550 °C. The reactions were conducted in sealed quartz tubes, which allowed the homogeneous and heterogeneous rates to be quantified separately for the first time. In the absence of nickel, conversions up to 20% were reached after 2 h. The pseudo-first-order rate constant for homogeneous gasification is 4.0 ± 2.7 × 10-5 s-1 at 550 °C. In the presence of a Ni wire that ran the entire length of the reactor, conversions of up to 90% were reached in less than 5 min. The pseudo-first-order rate constants for Ni-catalyzed gasification are 0.0032 ± 0.0013 and 0.0040 ± 0.0012 cm/s at 500 and 550 °C. These results show that homogeneous, uncatalyzed gasification in supercritical water is slow, but rates are greatly increased by added Ni. Hydrogen, carbon monoxide and carbon dioxide were the major products detected. Hydrogen was always the most abundant. With multiple uses, the Ni wire showed deactivation as a catalyst for methanol gasification.

AB - We report on the effect of nickel metal on the gasification of methanol in supercritical water at 500 and 550 °C. The reactions were conducted in sealed quartz tubes, which allowed the homogeneous and heterogeneous rates to be quantified separately for the first time. In the absence of nickel, conversions up to 20% were reached after 2 h. The pseudo-first-order rate constant for homogeneous gasification is 4.0 ± 2.7 × 10-5 s-1 at 550 °C. In the presence of a Ni wire that ran the entire length of the reactor, conversions of up to 90% were reached in less than 5 min. The pseudo-first-order rate constants for Ni-catalyzed gasification are 0.0032 ± 0.0013 and 0.0040 ± 0.0012 cm/s at 500 and 550 °C. These results show that homogeneous, uncatalyzed gasification in supercritical water is slow, but rates are greatly increased by added Ni. Hydrogen, carbon monoxide and carbon dioxide were the major products detected. Hydrogen was always the most abundant. With multiple uses, the Ni wire showed deactivation as a catalyst for methanol gasification.

UR - http://www.scopus.com/inward/record.url?scp=33750350484&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=33750350484&partnerID=8YFLogxK

U2 - 10.1016/j.supflu.2006.01.004

DO - 10.1016/j.supflu.2006.01.004

M3 - Article

AN - SCOPUS:33750350484

VL - 39

SP - 228

EP - 232

JO - Journal of Supercritical Fluids

JF - Journal of Supercritical Fluids

SN - 0896-8446

IS - 2

ER -