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Title: The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame

Abstract

The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame was investigated by numerical simulation. A detailed gas-phase reaction scheme and a simplified soot model were employed. The results show that the formation of NO has little effect on that of soot. However, the formation of soot in the flame significantly suppresses the formation of NO. The peak NO concentration and NO emission index are reduced by 28 and 46%, respectively, due to the formation of soot. The influence of soot on NO formation is caused by not only the radiation-induced thermal effect, but also the reaction-induced chemical effect. Relatively the thermal effect is more significant, causing 25 and 38% reduction, respectively, in peak NO concentration and NO emission index. The chemical effect is caused by the competition for acetylene (C{sub 2}H{sub 2}) between soot and NO formation. The formation of soot consumes acetylene in the flame and thus lowers the formation rate of radical CH. This reduces the reaction rate of CH + N{sub 2} = HCN + N, which is the rate-limiting step of the prompt NO formation route, the dominant route in the studied flame. (author)

Authors:
;  [1]
  1. Institute for Chemical Process and Environmental Technology, National Research Council Canada, 1200 Montreal Road, Ottawa, ON, K1A 0R6 (Canada)
Publication Date:
OSTI Identifier:
20880651
Resource Type:
Journal Article
Resource Relation:
Journal Name: Combustion and Flame; Journal Volume: 149; Journal Issue: 1-2; Other Information: Elsevier Ltd. All rights reserved
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; SOOT; ACETYLENE; ETHYLENE; AIR; AXIAL SYMMETRY; LAMINAR FLAMES; DIFFUSION; HYDROCYANIC ACID; COMBUSTION KINETICS; SYNTHESIS; NITRIC OXIDE; COMPUTERIZED SIMULATION; RADICALS

Citation Formats

Guo, Hongsheng, and Smallwood, Gregory J. The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame. United States: N. p., 2007. Web. doi:10.1016/J.COMBUSTFLAME.2006.11.006.
Guo, Hongsheng, & Smallwood, Gregory J. The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame. United States. doi:10.1016/J.COMBUSTFLAME.2006.11.006.
Guo, Hongsheng, and Smallwood, Gregory J. Sun . "The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame". United States. doi:10.1016/J.COMBUSTFLAME.2006.11.006.
@article{osti_20880651,
title = {The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame},
author = {Guo, Hongsheng and Smallwood, Gregory J.},
abstractNote = {The interaction between soot and NO formation in a laminar axisymmetric coflow ethylene/air diffusion flame was investigated by numerical simulation. A detailed gas-phase reaction scheme and a simplified soot model were employed. The results show that the formation of NO has little effect on that of soot. However, the formation of soot in the flame significantly suppresses the formation of NO. The peak NO concentration and NO emission index are reduced by 28 and 46%, respectively, due to the formation of soot. The influence of soot on NO formation is caused by not only the radiation-induced thermal effect, but also the reaction-induced chemical effect. Relatively the thermal effect is more significant, causing 25 and 38% reduction, respectively, in peak NO concentration and NO emission index. The chemical effect is caused by the competition for acetylene (C{sub 2}H{sub 2}) between soot and NO formation. The formation of soot consumes acetylene in the flame and thus lowers the formation rate of radical CH. This reduces the reaction rate of CH + N{sub 2} = HCN + N, which is the rate-limiting step of the prompt NO formation route, the dominant route in the studied flame. (author)},
doi = {10.1016/J.COMBUSTFLAME.2006.11.006},
journal = {Combustion and Flame},
number = 1-2,
volume = 149,
place = {United States},
year = {Sun Apr 15 00:00:00 EDT 2007},
month = {Sun Apr 15 00:00:00 EDT 2007}
}
  • The effect of carbon monoxide addition on soot formation in an ethylene/air diffusion flame is investigated by experiment and detailed numerical simulation. The paper focuses on the chemical effect of carbon monoxide addition by comparing the results of carbon monoxide and nitrogen diluted flames. Both experiment and simulation show that although overall the addition of carbon monoxide monotonically reduces the formation of soot, the chemical effect promotes the formation of soot in an ethylene/air diffusion flame. The further analysis of the details of the numerical result suggests that the chemical effect of carbon monoxide addition may be caused by themore » modifications to the flame temperature, soot surface growth and oxidation reactions. Flame temperature increases relative to a nitrogen diluted flame, which results in a higher surface growth rate, when carbon monoxide is added. Furthermore, the addition of carbon monoxide increases the concentration of H radical owing to the intensified forward rate of the reaction CO + OH = CO{sub 2} + H and therefore increases the surface growth reaction rates. The addition of carbon monoxide also slows the oxidation rate of soot because the same reaction CO + OH = CO{sub 2} + H results in a lower concentration of OH. (author)« less
  • A numerical study of an axisymmetric coflow laminar ethylene-air diffusion flame at atmospheric pressure was conducted using detailed chemistry and complex thermal and transport properties and two different methodologies: (1) the direct simulation method of solving the two-dimensional axisymmetric elliptic governing equations, and (2) the steady-state stretched diffusion flamelet model. Soot formation and radiative heat transfer were not taken into account in these calculations, both for simplicity and to avoid the complications associated with the issues of how to incorporate these chemical and physical processes into the flamelet model. The same reaction mechanism and thermal and transport properties were usedmore » in the 2D direct simulation and the generation of the flamelet library. The flamelet library was generated from the solutions of counterflow ethylene-air diffusion flames at a series of stretch rates. Results of the 2D direct simulation and the flamelet model are compared in physical space. Although the overall results of the flamelet model are qualitatively similar to those of the direct simulation, significant differences exist between the results of the two methods even for temperature and major species. The direct simulation method predicts that the peak concentrations of CO{sub 2} and H{sub 2}O occur in different regions in the flame, while the flamelet model results show that the peak concentrations of CO{sub 2} and H{sub 2}O occur in the same region. The flamelet model predicts an overly rapid approach to the equilibrium structure in the downstream region, leading to significantly higher flame temperatures. The main reason for the failure of the flamelet model in the downstream region is due to the neglect of the effects of multidimensional convection and diffusion and the fundamental difference in the chemical structure between a coflow diffusion flame and a counterflow diffusion flame. The findings of this paper are highly relevant to understanding the flamelet model results in the calculations of multidimensional turbulent diffusion flames. (author)« less
  • A numerical and experimental study of an axisymmetric coflow laminar methane-air diffusion flame at pressures between 5 and 40 atm was conducted to investigate the effect of pressure on the flame structure and soot formation characteristics. Experimental work was carried out in a new high-pressure combustion chamber described in a recent study [K.A. Thomson, O.L. Gulder, E.J. Weckman, R.A. Fraser, G.J. Smallwood, D.R. Snelling, Combust. Flame 140 (2005) 222-232]. Radially resolved soot volume fraction was experimentally measured using both spectral soot emission and line-of-sight attenuation techniques. Numerically, the elliptic governing equations were solved in axisymmetric cylindrical coordinates using the finitemore » volume method. Detailed gas-phase chemistry and complex thermal and transport properties were employed in the numerical calculations. The soot model employed in this study accounts for soot nucleation and surface growth using a semiempirical acetylene-based global soot model with oxidation of soot by O{sub 2}, OH, and O taken into account. Radiative heat transfer was calculated using the discrete-ordinates method and a nine-band nongray radiative property model. Two soot surface growth submodels were investigated and the predicted pressure dependence of soot yield was compared with available experimental data. The experiment, the numerical model, and a simplified theoretical analysis found that the visible flame diameter decreases with pressure as P{sub a}{sup -0.5}. The flame-diameter-integrated soot volume fraction increases with pressure as P{sub a}{sup 1.3} between 5 and 20 atm. The assumption of a square root dependence of the soot surface growth rate on the soot particle surface area predicts the pressure dependence of soot yield in good agreement with the experimental observation. On the other hand, the assumption of linear dependence of the soot surface growth rate on the soot surface area predicts a much faster increase in the soot yield with pressure than that observed experimentally. Although pressure affects the gas-phase chemistry, the increased soot production with increasing pressure seems primarily due to enhanced mixture density and species concentrations in the pressure range investigated. The increased pressure causes enhanced air entrainment into the fuel stream around the burner rim, leading to accelerated fuel pyrolysis. In the pressure range of 20 to 40 atm both the model and experiment show a diminishing sensitivity of sooting propensity to pressure with a greater decrease in the predicted sensitivity of soot propensity to pressure than the experimental results. (author)« less
  • A detailed soot growth model in which the equations for particle production have been coupled to the flow and gaseous species conservation equations has been developed for an axisymmetric, laminar, coflow diffusion flame. Results from the model have been compared to experimental data for a confined methane-air flame. The two-dimensional system couples detailed transport and finite rate chemistry in the gas phase with the aerosol equations in the sectional representation. The formulation includes detailed treatment of the transport, inception, surface growth, oxidation, and coalescence of soot particulates. Effects of thermal radiation and particle scrubbing of gas-phase growth and oxidation speciesmore » are also included, Predictions and measurements of temperature, soot volume fractions, and selected species are compared over a range of heights and as a function of radius. Flame heights are somewhat overpredicted and local temperatures and volume fractions are underpredicted. The authors believe the inability to reproduce accurately bulk flame parameters directly inhibits the ability to predict soot volume fractions and these differences are likely a result of uncertainties in the experimental inlet conditions. Predictions of the distributions of particle sizes indicate the existence of (relatively) low-molecular-weight species along the centerline of the burner and trace amounts of the particles that escape from the flame, unoxidized. Oxidation of particulates is dominated by reactions with hydroxyl radicals which attain levels approximately 10 times higher than calculated equilibrium levels. Gas cooling effects due to radiative low are shown to have a very significant effect on predicted soot concentrations.« less
  • Soot aggregate formation in a two-dimensional laminar coflow ethylene/air diffusion flame is studied with a pyrene-based soot model, a detailed sectional aerosol dynamics model, and a detailed radiation model. The chemical kinetic mechanism describes polycyclic aromatic hydrocarbon formation up to pyrene, the dimerization of which is assumed to lead to soot nucleation. The growth and oxidation of soot particles are characterized by the HACA surface mechanism and pyrene-soot surface condensation. The mass range of the solid soot phase is divided into thirty-five discrete sections and two equations are solved in each section to model the formation of the fractal-like sootmore » aggregates. The coagulation model is improved by implementing the aggregate coagulation efficiency. Several physical processes that may cause sub-unitary aggregate coagulation efficiency are discussed. Their effects on aggregate structure are numerically investigated. The average number of primary soot particles per soot aggregate n{sub p} is found to be a strong function of the aggregate coagulation efficiency. Compared to the available experimental data, n{sub p} is well reproduced with a constant 20% aggregate coagulation efficiency. The predicted axial velocity, OH mole fraction, and C{sub 2}H{sub 2} mole fraction are validated against experimental data in the literature. Reasonable agreements are obtained. Finally, a sensitivity study of the effects of particle coalescence on soot volume fraction and soot aggregate nanostructure is conducted using a coalescence cutoff diameter method. (author)« less