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Research Papers: Gas Turbines: Combustion, Fuels, and Emissions

Thermochemical Mechanism Optimization for Accurate Predictions of CH Concentrations in Premixed Flames of C1–C3 Alkane Fuels

[+] Author and Article Information
Philippe Versailles

Mem. ASME
Department of Mechanical Engineering,
McGill University,
Montréal, QC H3A 0C3, Canada
e-mail: philippe.versailles@mail.mcgill.ca

Graeme M. G. Watson

Combustion Engineer,
Siemens Canada Limited,
Montréal, QC H9P 1A5, Canada
e-mail: graeme.watson@siemens.com

Antoine Durocher

Mem. ASME
Department of Mechanical Engineering,
McGill University,
Montréal, QC H3A 0C3, Canada
e-mail: antoine.durocher@mail.mcgill.ca

Gilles Bourque

Fellow ASME
Combustion Key Expert,
Siemens Canada Limited,
Montréal, QC H9P 1A5, Canada;
Adjunct Professor
Department of Mechanical Engineering,
McGill University,
Montréal, QC H3A 0C3, Canada
e-mail: gilles.bourque@siemens.com;
gilles.bourque@mcgill.ca

Jeffrey M. Bergthorson

Mem. ASME
Associate Professor
Department of Mechanical Engineering,
McGill University,
Montréal, QC H3A 0C3, Canada
e-mail: jeff.bergthorson@mcgill.ca

1Corresponding author.

Contributed by the Combustion and Fuels Committee of ASME for publication in the JOURNAL OF ENGINEERING FOR GAS TURBINES AND POWER. Manuscript received July 26, 2017; final manuscript received August 30, 2017; published online February 27, 2018. Editor: David Wisler.

J. Eng. Gas Turbines Power 140(6), 061508 (Feb 27, 2018) (14 pages) Paper No: GTP-17-1401; doi: 10.1115/1.4038416 History: Received July 26, 2017; Revised August 30, 2017

Increasingly stringent regulations on NOx emissions are enforced by governments owing to their contribution in the formation of ozone, smog, fine aerosols, acid rains, and nutrient pollution of surface water, which affect human health and the environment. The design of high-efficiency, low-emission combustors achieving these ever-decreasing emission standards requires thermochemical mechanisms of sufficiently high accuracy. Recently, a comprehensive set of experimental data, collected through laser-based diagnostics in atmospheric, jet-wall, stagnation, premixed flames, was published for all isomers of C1–C4 alkane and alcohol fuels. The rapid formation of NO through the flame front via the prompt (Fenimore) route was shown to be strongly coupled to the maximum concentration of the methylidyne radical, [CH]peak, and the flow residence time within the CH layer. A proper description of CH formation is then a prerequisite for accurate predictions of NO concentrations in hydrocarbon–air flames. However, a comparison against the Laser-induced fluorescence (LIF) experimental data of Versailles, P., et al. (2016, “Quantitative CH Measurements in Atmospheric-Pressure, Premixed Flames of C1–C4 Alkanes,” Combust. Flame, 165, pp. 109--124) revealed that (1) modern thermochemical mechanisms are unable to accurately capture the stoichiometric dependence of [CH]peak, and (2) for a given equivalence ratio, the predictions of different mechanisms span over more than an order of magnitude. This paper presents an optimization of the specific rate of a selection of nine elementary reactions included in the San Diego combustion mechanism. A quasi-Newton algorithm is used to minimize an objective function defined as the sum of squares of the relative difference between the numerical and experimental CH–LIF data of Versailles, P., et al. (2016, “Quantitative CH Measurements in Atmospheric-Pressure, Premixed Flames of C1–C4 Alkanes,” Combust. Flame, 165, pp. 109--124), while constraining the specific rates to physically reasonable values. A mechanism properly describing CH formation for lean to rich, C1–C3 alkane–air flames is obtained. This optimized mechanism will enable accurate predictions of prompt-NO formation over a wide range of equivalence ratios and alkane fuels. Suggestions regarding which reactions require further investigations, either through experimental or theoretical assessments of the individual specific rates, are also provided.

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Figures

Grahic Jump Location
Fig. 1

Logarithmic sensitivity of the maximum CH mole fraction to the specific rate of individual reactions, L.S.(XCH,peak, i). The reactions are sorted in decreasing order of ∑CmHn,ϕL.S.(XCH,peak,i)2. For each reaction, the bands are colored according to a blue (top, ϕ = 0.7) to red (bottom, ϕ = 1.5) rainbow colormap.

Grahic Jump Location
Fig. 2

Product of L.S.(XCH,peak, i) with Δki/ki. The relative errors are obtained from the upper uncertainty limits estimated in Refs. [21] and [23]. The black, dashed lines correspond to L.S.(XCH,peak,i)·Δki/ki=±0.6.

Grahic Jump Location
Fig. 3

Measured [7] and simulated values of SLIF/SR and δCH for methane, ethane, and propane premixed flames. Legend: experiments, SD (unmodified),  fi,orig (Table 3), fi,inv (Table 4), ◇GRI (unmodified), and GRI with the rate coefficients of Table 3. The solid blue and green symbols correspond to data points included in the optimization and adjusted against the experimental targets presented in Table 2. Note the logarithmic scale on plots (a), (c), and (e).

Grahic Jump Location
Fig. 4

Logarithmic sensitivity of the maximum CH mole fraction to the heat of formation of individual species, L.S.(XCH,peak, k). The species are sorted in decreasing order of ∑CmHn,ϕL.S.(XCH,peak,k)2.

Grahic Jump Location
Fig. 5

Product of L.S.(XCH,peak, k) with Δ(ΔfHk°)/ΔfHk°. The relative errors are obtained from Ref. [28].

Grahic Jump Location
Fig. 6

qnet (top) and k (bottom) of the reaction CH+O2↔products. Legend: SD, USC, GRI, NUIG1, KON, Baulch et al. [21] with corresponding uncertainty estimates (ki/fi and ki · fi) , bounds on active parameters fi,low and fi,high, and optimized specific rates corresponding to fi,orig and fi,inv, see Tables 3 and 4, respectively.

Grahic Jump Location
Fig. 7

qnet (top) and k (bottom) of the reaction CH2+OH↔CH+H2O. Same legend as Fig. 6, supplemented with Ref. [34].

Grahic Jump Location
Fig. 8

qnet (top) and k (bottom) of the reaction CH2+H↔CH+H2. Same legend as Fig. 6, supplemented with NUIG2 -- - - --, and Baulch et al. (1992) [22] .

Grahic Jump Location
Fig. 9

qnet (top) and k (bottom) of the reaction H+CH3(+M)↔CH4(+M). Same legend as Fig. 6.

Grahic Jump Location
Fig. 10

qnet (top) and k (bottom) of the reaction CH3+OH↔CH2*+H2O. Same legend as Fig. 6, supplemented with Ref. [35].

Grahic Jump Location
Fig. 11

qnet (top) and k (bottom) of the reaction CH+H2O↔CH2O+H. Same legend as Fig. 8.

Grahic Jump Location
Fig. 12

Normalized net reaction rate of the reaction CH2+O2↔CO+OH+H (top) and sum of the specific rates of reactions CH2+O2→products. Same legend as Fig. 8, supplemented with data from the CRECK mechanism (version 1412) [30] , and [29].

Grahic Jump Location
Fig. 13

qnet (top) and k (bottom) of the reaction CH2CO+O↔CH2+CO2. Same legend as Fig. 12, supplemented with Ref. [42].

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