Abstract
Results and analysis of the oxidation of methane in supercritical water by oxygen over a pressure range from 35 to 270 bar and a temperature range from 390 to 440°C are presented. Raman spectroscopy is used as an in situ diagnostic to monitor the concentration of methane, oxygen, carbon monoxide, and carbon dioxide in a constant volume reactor. Reaction orders with respect to methane and oxygen at 270 bar and at methane concentrations near 0.1 mol/L are close to two and zero, respectively. A nonmonotonic dependence of reaction rates on water concentration is observed. With temperature and initial concentrations held constant, methane consumption rates first increase with water concentration but reach a maximum near 5 mol/L. Further increases in water concentration lead to a sharp decrease in the rate of methane consumption. An existing, highpressure elementary reaction mechanism reproduces this downturn in rates and provides insight into the reasons for this behavior.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 184-189 |
| Number of pages | 6 |
| Journal | Journal of Physical Chemistry |
| Volume | 100 |
| Issue number | 1 |
| State | Published - Jan 4 1996 |
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ASJC Scopus subject areas
- Physical and Theoretical Chemistry
- Engineering(all)
Cite this
Kinetics measurements of methane oxidation in supercritical water. / Steeper, Richard R.; Rice, Steven F.; Kennedy, Ian M.; Aiken, Jason D.
In: Journal of Physical Chemistry, Vol. 100, No. 1, 04.01.1996, p. 184-189.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Kinetics measurements of methane oxidation in supercritical water
AU - Steeper, Richard R.
AU - Rice, Steven F.
AU - Kennedy, Ian M.
AU - Aiken, Jason D.
PY - 1996/1/4
Y1 - 1996/1/4
N2 - Results and analysis of the oxidation of methane in supercritical water by oxygen over a pressure range from 35 to 270 bar and a temperature range from 390 to 440°C are presented. Raman spectroscopy is used as an in situ diagnostic to monitor the concentration of methane, oxygen, carbon monoxide, and carbon dioxide in a constant volume reactor. Reaction orders with respect to methane and oxygen at 270 bar and at methane concentrations near 0.1 mol/L are close to two and zero, respectively. A nonmonotonic dependence of reaction rates on water concentration is observed. With temperature and initial concentrations held constant, methane consumption rates first increase with water concentration but reach a maximum near 5 mol/L. Further increases in water concentration lead to a sharp decrease in the rate of methane consumption. An existing, highpressure elementary reaction mechanism reproduces this downturn in rates and provides insight into the reasons for this behavior.
AB - Results and analysis of the oxidation of methane in supercritical water by oxygen over a pressure range from 35 to 270 bar and a temperature range from 390 to 440°C are presented. Raman spectroscopy is used as an in situ diagnostic to monitor the concentration of methane, oxygen, carbon monoxide, and carbon dioxide in a constant volume reactor. Reaction orders with respect to methane and oxygen at 270 bar and at methane concentrations near 0.1 mol/L are close to two and zero, respectively. A nonmonotonic dependence of reaction rates on water concentration is observed. With temperature and initial concentrations held constant, methane consumption rates first increase with water concentration but reach a maximum near 5 mol/L. Further increases in water concentration lead to a sharp decrease in the rate of methane consumption. An existing, highpressure elementary reaction mechanism reproduces this downturn in rates and provides insight into the reasons for this behavior.
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M3 - Article
AN - SCOPUS:0030568145
VL - 100
SP - 184
EP - 189
JO - Journal of Physical Chemistry
JF - Journal of Physical Chemistry
SN - 0022-3654
IS - 1
ER -