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Research Papers

NOx-Hydrocarbon Kinetics Model Validation Using Measurements of H2O in Shock-Heated CH4/C2H6 Mixtures With NO2 as Oxidant

[+] Author and Article Information
O. Mathieu

Department of Mechanical Engineering,
Texas A&M University,
College Station, TX 77845
e-mail: olivier.mathieu@tamu.edu

C. R. Mulvihill, E. L. Petersen

Department of Mechanical Engineering,
Texas A&M University,
College Station, TX 77845

H. J. Curran

Department of Chemistry,
National University of Ireland,
Galway, Ireland

1Corresponding author.

Manuscript received September 12, 2018; final manuscript received September 16, 2018; published online November 8, 2018. Editor: Jerzy T. Sawicki.

J. Eng. Gas Turbines Power 141(4), 041007 (Nov 08, 2018) (8 pages) Paper No: GTP-18-1607; doi: 10.1115/1.4041659 History: Received September 12, 2018; Revised September 16, 2018

One method frequently used to reduce NOx emissions is exhaust gas recirculation, where a portion of the exhaust gases, including NOx, is reintroduced into the combustion chamber. While a significant amount of research has been performed to understand the important fuel/NOx chemistry, more work is still necessary to improve the current understanding on this chemistry and to refine detailed kinetics models. To validate models beyond global kinetics data, such as ignition delay time or flame speed, the formation of H2O was recorded using a laser absorption diagnostic during the oxidation of a mixture representing a simplistic natural gas (90% CH4/10% C2H6 (mol)). This mixture was studied at a fuel lean condition (equivalence ratio = 0.5) and at atmospheric pressure. Unlike in conventional fuel-air experiments, NO2 was used as the oxidant to better elucidate the important, fundamental chemical kinetics by exaggerating the interaction between NOx and hydrocarbon-based species. Results showed a peculiar water formation profile, compared to a former study performed in similar conditions with O2 as oxidant. In the presence of NO2, the formation of water occurs almost immediately before it reaches more or less rapidly (depending on the temperature) a plateau. Modern, detailed kinetics models predict the data with fair to good accuracy overall, while the GRI 3.0 mechanism is proven inadequate for reproducing CH4/C2H6 and NO2 interactions.

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Figures

Grahic Jump Location
Fig. 1

Evolution of the H2O mole fraction as a function of time for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar at around 1 atm

Grahic Jump Location
Fig. 2

Evolution of the H2O mole fraction as a function of time for a mixture of 90% CH4/10% C2H6 (mol), with NO2 or O2 as oxidant, ϕ = 0.5, diluted in 99% Ar at around 1 atm. Data with O2 as oxidant are from Mathieu et al. [18].

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Fig. 3

Definition of the inflection delay time measurement

Grahic Jump Location
Fig. 4

Evolution of the inflection delay time with the inverse of the temperature

Grahic Jump Location
Fig. 5

Comparison between experiments and literature models of the formation of water with time at 1303 K, 1.35 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 6

Comparison between experiments and literature models of the formation of water with time at 1342 K, 1.35 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 7

Comparison between experiments and literature models of the formation of water with time at 1480 K, 1.48 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 8

Comparison between experiments and literature models of the formation of water with time at 1541 K, 1.33 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 9

Comparison between experiments and literature models of the formation of water with time at 1626 K, 1.36 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 10

Normalized sensitivity coefficients for reactions involved with H2O formation at 1303 K, 1.35 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 11

Normalized sensitivity coefficients for reactions involved with H2O formation at 1626 K, 1.36 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar

Grahic Jump Location
Fig. 12

Rate of production analysis for H2O formation at 1303K, 1.35 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar with the model of Deng et al. [15]

Grahic Jump Location
Fig. 13

Rate of production analysis for H2O formation at 1303 K, 1.35 atm for a mixture of 90% CH4/10% C2H6 (mol), with NO2 as oxidant, ϕ = 0.5, diluted in 99% Ar with the model of Mendiara and Glarborg [25,26]

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