Flow reactor studies and kinetic modeling of the H2/O2/NOx and CO/H2O/O2/NOx reactions

Mark A. Mueller, R. A. Yetter, F. L. Dryer

Research output: Contribution to journalArticle

126 Citations (Scopus)

Abstract

Flow reactor experiments were performed over wide ranges of pressure (0.5-14.0 atm) and temperature (750-1100 K) to study H2/O2 and CO/H2O/O2 kinetics in the presence of trace quantities of NO and NO2. The promoting and inhibiting effects of NO reported previously at near atmospheric pressures extend throughout the range of pressures explored in the present study. At conditions where the recombination reaction H+O2 (+M) = HO2 (+M) is favored over the competing branching reaction, low concentrations of NO promote H2 and CO oxidation by converting HO2 to OH. In high concentrations, NO can also inhibit oxidative processes by catalyzing the recombination of radicals. The experimental data show that the overall effects of NO addition on fuel consumption and conversion of NO to NO2 depend strongly on pressure and stoichiometry. The addition of NO2 was also found to promote H2 and CO oxidation but only at conditions where the reacting mixture first promoted the conversion of NO2 to NO. Experimentally measured profiles of H2, CO, CO2, NO, NO2, O2, H2O, and temperature were used to constrain the development of a detailed kinetic mechanism consistent with the previously studied H2/O2, CO/H2O/O2, H2/NO2, and CO/H2O/N2O systems. Model predictions generated using the reaction mechanism presented here are in good agreement with the experimental data over the entire range of conditions explored.

Original languageEnglish (US)
Pages (from-to)705-724
Number of pages20
JournalInternational Journal of Chemical Kinetics
Volume31
Issue number10
DOIs
StatePublished - Jan 1 1999

Fingerprint

Carbon Monoxide
reactors
Kinetics
kinetics
recombination reactions
fuel consumption
oxidation
Pressure
Genetic Recombination
low concentrations
stoichiometry
atmospheric pressure
Oxidation
Temperature
Atmospheric Pressure
temperature
profiles
predictions
Fuel consumption
Stoichiometry

All Science Journal Classification (ASJC) codes

  • Biochemistry
  • Physical and Theoretical Chemistry
  • Organic Chemistry
  • Inorganic Chemistry

Cite this

@article{fe86e17464084c46a3425928fd458042,
title = "Flow reactor studies and kinetic modeling of the H2/O2/NOx and CO/H2O/O2/NOx reactions",
abstract = "Flow reactor experiments were performed over wide ranges of pressure (0.5-14.0 atm) and temperature (750-1100 K) to study H2/O2 and CO/H2O/O2 kinetics in the presence of trace quantities of NO and NO2. The promoting and inhibiting effects of NO reported previously at near atmospheric pressures extend throughout the range of pressures explored in the present study. At conditions where the recombination reaction H+O2 (+M) = HO2 (+M) is favored over the competing branching reaction, low concentrations of NO promote H2 and CO oxidation by converting HO2 to OH. In high concentrations, NO can also inhibit oxidative processes by catalyzing the recombination of radicals. The experimental data show that the overall effects of NO addition on fuel consumption and conversion of NO to NO2 depend strongly on pressure and stoichiometry. The addition of NO2 was also found to promote H2 and CO oxidation but only at conditions where the reacting mixture first promoted the conversion of NO2 to NO. Experimentally measured profiles of H2, CO, CO2, NO, NO2, O2, H2O, and temperature were used to constrain the development of a detailed kinetic mechanism consistent with the previously studied H2/O2, CO/H2O/O2, H2/NO2, and CO/H2O/N2O systems. Model predictions generated using the reaction mechanism presented here are in good agreement with the experimental data over the entire range of conditions explored.",
author = "Mueller, {Mark A.} and Yetter, {R. A.} and Dryer, {F. L.}",
year = "1999",
month = "1",
day = "1",
doi = "10.1002/(SICI)1097-4601(1999)31:10<705::AID-JCK4>3.0.CO;2-#",
language = "English (US)",
volume = "31",
pages = "705--724",
journal = "International Journal of Chemical Kinetics",
issn = "0538-8066",
publisher = "John Wiley and Sons Inc.",
number = "10",

}

Flow reactor studies and kinetic modeling of the H2/O2/NOx and CO/H2O/O2/NOx reactions. / Mueller, Mark A.; Yetter, R. A.; Dryer, F. L.

In: International Journal of Chemical Kinetics, Vol. 31, No. 10, 01.01.1999, p. 705-724.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Flow reactor studies and kinetic modeling of the H2/O2/NOx and CO/H2O/O2/NOx reactions

AU - Mueller, Mark A.

AU - Yetter, R. A.

AU - Dryer, F. L.

PY - 1999/1/1

Y1 - 1999/1/1

N2 - Flow reactor experiments were performed over wide ranges of pressure (0.5-14.0 atm) and temperature (750-1100 K) to study H2/O2 and CO/H2O/O2 kinetics in the presence of trace quantities of NO and NO2. The promoting and inhibiting effects of NO reported previously at near atmospheric pressures extend throughout the range of pressures explored in the present study. At conditions where the recombination reaction H+O2 (+M) = HO2 (+M) is favored over the competing branching reaction, low concentrations of NO promote H2 and CO oxidation by converting HO2 to OH. In high concentrations, NO can also inhibit oxidative processes by catalyzing the recombination of radicals. The experimental data show that the overall effects of NO addition on fuel consumption and conversion of NO to NO2 depend strongly on pressure and stoichiometry. The addition of NO2 was also found to promote H2 and CO oxidation but only at conditions where the reacting mixture first promoted the conversion of NO2 to NO. Experimentally measured profiles of H2, CO, CO2, NO, NO2, O2, H2O, and temperature were used to constrain the development of a detailed kinetic mechanism consistent with the previously studied H2/O2, CO/H2O/O2, H2/NO2, and CO/H2O/N2O systems. Model predictions generated using the reaction mechanism presented here are in good agreement with the experimental data over the entire range of conditions explored.

AB - Flow reactor experiments were performed over wide ranges of pressure (0.5-14.0 atm) and temperature (750-1100 K) to study H2/O2 and CO/H2O/O2 kinetics in the presence of trace quantities of NO and NO2. The promoting and inhibiting effects of NO reported previously at near atmospheric pressures extend throughout the range of pressures explored in the present study. At conditions where the recombination reaction H+O2 (+M) = HO2 (+M) is favored over the competing branching reaction, low concentrations of NO promote H2 and CO oxidation by converting HO2 to OH. In high concentrations, NO can also inhibit oxidative processes by catalyzing the recombination of radicals. The experimental data show that the overall effects of NO addition on fuel consumption and conversion of NO to NO2 depend strongly on pressure and stoichiometry. The addition of NO2 was also found to promote H2 and CO oxidation but only at conditions where the reacting mixture first promoted the conversion of NO2 to NO. Experimentally measured profiles of H2, CO, CO2, NO, NO2, O2, H2O, and temperature were used to constrain the development of a detailed kinetic mechanism consistent with the previously studied H2/O2, CO/H2O/O2, H2/NO2, and CO/H2O/N2O systems. Model predictions generated using the reaction mechanism presented here are in good agreement with the experimental data over the entire range of conditions explored.

UR - http://www.scopus.com/inward/record.url?scp=0032664116&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=0032664116&partnerID=8YFLogxK

U2 - 10.1002/(SICI)1097-4601(1999)31:10<705::AID-JCK4>3.0.CO;2-#

DO - 10.1002/(SICI)1097-4601(1999)31:10<705::AID-JCK4>3.0.CO;2-#

M3 - Article

AN - SCOPUS:0032664116

VL - 31

SP - 705

EP - 724

JO - International Journal of Chemical Kinetics

JF - International Journal of Chemical Kinetics

SN - 0538-8066

IS - 10

ER -