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The in\ufb02uence of oxygen concentration and carbon dioxide as diluents in the oxidizer side on soot formation was studied by Time Resolved Laser Induced Incandescence (TIRE-LII) and TEM photography in non-premixed co-\ufb02owing \ufb02ames. TIRE-LII method was used to measure the distribution of two-dimensional soot volume fraction and primary particle size. The soot was directly sampled by the thermophoretic method, and its diameter was examined by TEM photography. Two suitable delay times of the TIRE-LII method affecting measurable range and sensitivity were determined by comparing TEM photographs with the TIRE-LII signal. The effects of oxygen concentration and carbon dioxide as diluents in the oxidizer side on soot formation were investigated with these calibrated techniques. An O2C(CO2, N2, and [ArCCO2]) mixtures in co-\ufb02ow were used to isolate carbon dioxide effects systematically. The primary particle number concentration and soot volume fraction were abruptly decreased by the addition of carbon dioxide to co-\ufb02ow. This suppression was resulted from the short residence time in inception region because of the late nucleation and the decrease of surface growth distance by the low \ufb02ame temperature due to the higher thermal capacity and the chemical change of carbon dioxide. The increase of oxygen concentration in the co-\ufb02ow caused an enhancement of soot nucleation and thus the residence time increase, but the speci\ufb01c growth rate showed almost the same value regardless of the co-\ufb02ow mixture in the growth region. This result suggests that the speci\ufb01c growth rate has a weak dependence on the relative change of co-\ufb02ow conditions in non-premixed co-\ufb02owing \ufb02ames.
Recently many combustion systems such as EGR (Exhaust Gas Recirculation) systems and oxygen combustors with CO2recycling have been proposed to reduce pollutant emissions and to enhance thermal ef\ufb01ciency. However, the proposed systems are mostly accompanied by drawbacks; namely, nitric oxide (NOX) and soot particles emissions[1\u2013
mechanisms of NOXformation and its reduction methods, there are still many ambiguities in the explanations of soot emission due to various changes in the features of soot aggregates (particle diameter, aggregate size, the number concentration of primary particles, soot volume fraction, etc.) in \ufb02ames.
A number of investigations have been focused on reducing soot emission by introducing several techniques, including the use of different fuels and addition of diluents[3\u201311] on the oxidizer or fuel side. However, it is still dif\ufb01cult to elucidate the effects of diluents on soot formation in \ufb02ames because soot particle diameter, volume fraction, and the number density of particles are strongly dependent on location within a \ufb02ame.
oxygen to methane suppresses soot formation chemically, while oxygen addition enhances the soot formation by direct chemical interaction for propane andn-butane. Through the measurement of the soot inception limit, reported that CO2, whether added to the fuel or oxidizer side, could suppress soot formation chemically in a counter diffusion \ufb02ame. But because parameters that previous researchers had used to examine CO2 effects generally, those are, maximum soot volume fraction
neither where, nor how the effects independently act on apparently. Therefore, despite these advances in the understanding of soot formation, the work done to date does not provide a clear picture on the effect of addition of diluents due to the de\ufb01cient information of the features of soot in \ufb02ames.
Several experimental techniques have been developed to identify the features of soot aggregates in \ufb02ames. Optical techniques are generally considered to be the best one suitable for this purpose because of their non-intrusiveness; for example, light scattering for aggregates size, various scattering and extinction methods[13,14] for measuring of both soot volume fraction and cluster structure, and multi-wavelength analysis for soot volume fraction. Unfortunately, it is impossible to identify soot characteristics on the whole combustion \ufb01eld simultaneously with these methods because of their pointwise or line-of-sight character. Alternatively, laser induced incandes- cence (LII) techniques have been used successfully for two- dimensional soot volume fraction measurements in a wide range of combustion processes[9,16]. Recently, there have been some attempts to combine LII, elastic scattering, and the TIRE-LII (time-resolved LII) method to measure soot characteristics simultaneously[1,17].
In this study, we tried to improve the measuring technique for primary particle diameter by proper determination of two delay times through a calibration procedure of the TIRE-LII signal with TEM photographs. With this calibrated technique, we obtained characteristic value of soot, such as soot volume fraction (fv), particle size (dp) and the number concentration of primary soot particles (Np), in laminar non-premixed \ufb02ames. The effects of oxygen concentration (25\u201345%) in the oxidizer side, and diluents (N2, CO2, ArCCO2) were investigated in the soot inception and growth regions.
The Laser Induced Incandescence (LII) method has been applied to the measurement of soot volume fraction (fv) in many combustion systems. LII involves the heating of soot particles to temperatures above the surrounding gas tempera- ture via the absorption of laser energy, and subsequent detection of blackbody radiation corresponding to the elevated temperature of the soot particles. If one assumes a suf\ufb01ciently loose structure of soot aggregates, which may be regarded as justi\ufb01ed with the typical fractal dimension of soot aggregates in the range 1.6\u20131.8, and ignores gas radiation, the energy balance of soot is governed by the size of the primary
To,surrounding gas temperature
M, molar mass of solid carbon
In order to improve soot measurement techniques such as LII and TIRE-LII methods, there have been many detailed examinations about the heat transfer paths in heated soot particles by many researchers[18\u201320]; the absorption of laser irradiance, the heat transfer to ambient gas, vaporization, blackbody radiation, and the change of particle temperature.
Melton showed that the intensity of the LII signal, SLII, for a group of soot particles has a dependence on primary particle diameter as follows
whereNpis the number concentration of primary particles,dpis the diameter of the primary particles, andlemis the measured wavelength. Forlembetween 700 and 400 nm, for example, the LII signal is proportional to the primary soot particle diameter raised to the power of 3.22\u20133.38, or approximately to the soot volume fraction.
Ni and Quay[16,21] reported that initially the LII signal increases rapidly as laser power increases (linear region) and once laser power reaches a saturation threshold, the LII signal shows a small increase (saturation region).Fig. 1 shows the intensity of the LII signal to the laser \ufb02uence at different positions in a \ufb02ame. The intensity of the LII signal shows the same trend as the result of Ni and Quay. The laser \ufb02uence in a saturated region was used to compensate a slightly inhomo- geneous laser pro\ufb01le.
In this experiment, a planar laser sheet was formed using a cylindrical lens and convex lenses, and the edge of the laser sheet, which is weaker in intensity, was cut off by a slit to obtain a sheet having a more uniform pro\ufb01le (I/ImaxO0.75 at test section). The \ufb02uence distribution of the laser sheet was con\ufb01rmed with the Laser Rayleigh Scattering (LRS) method. Extinction method was used to quantify the relative soot volume fraction obtained by the LII method.
The TIRE-LII technique is based on the fact that after a laser pulse, smaller particles cool down faster than larger ones due to their larger speci\ufb01c surface[19,20,22]. There are three paths for the energy loss, which can be elucidated from the energy balance equation (Eq. (1)): vaporization, heat conduction to the surrounding gas, and radiation. Will et al. showed that the temperature of soot particles abruptly changes within 100 ns
after irradiance by a laser pulse due to the vaporization of soot and the temperature decay rates were governed by a conduction loss. Therefore the initial LII signal, within 100 ns, is similar regardless of the soot particle diameter, but the decay trend of the LII signal depends on the primary particle size in the region is governed by the conduction term due to its speci\ufb01c surface. The ratio of the LII signals, measured at two different delay times after the laser pulse irradiation, is known to be the function of soot diameter.
The decay curves of the LII signal after the absorption of laser energy are shown inFig. 2. The temporal pro\ufb01le of LII signal changes to a laser \ufb02uence; that is the parameter determining the initial particle temperature. As the laser \ufb02uence decreases, the cooling rate decreases due to the small temperature difference between soot particles and ambient, but there is little difference of the decay rate of LII signal above
saturation region. In the present study, the error in measure- ment of soot particle size resulted from inhomogeneous heating pro\ufb01le is estimated withinG3 nm from the calibration curve (Fig. 6a).
measurement systems for LII and TIRE-LII techniques and a thermophoretic soot sampling system to measure quantitative soot particle diameter.
The inner diameter of the fuel nozzle is 5 mm and the contraction nozzle with a cut-area ratio of 1/6.5 around the fuel nozzle was used to obtain the uniform co-\ufb02owing velocity and to block the ambient air. CO2CO2, [0.61ArC0.39CO2]CO2, and N2CO2mixtures in the oxidizer side (co-\ufb02ow) were used to discriminate the CO2effects. Blow-off of \ufb02ame occurs at 19% of oxygen concentration and 27% of oxygen concen- tration in the case of N2and CO2dilution, respectively. Therefore, experiments carried out in the stable \ufb02ame region, those are, 25\u201345% of oxygen concentration for the N2dilution and 30\u201345% of oxygen concentration for the CO2dilution. The adiabatic \ufb02ame temperature (Tad) was used as the representa- tive \ufb02ame temperature. The experimental conditions and \ufb02ame lengths are shown inTable 1.
A second harmonic Nd:Yag laser (lZ532 nm,ImaxZ 500 mJ/pulse) was used as a laser source and its duration of pulse (w7 ns) was very short. A laser sheet of 40 mm width and 500mm thickness was formed across the \ufb02ame axis by using a cylindrical lens and a convex lens. The detection part consisted of a \ufb01lter to obtain the monochromatic signal, 450 nm (G10 nm) in LII measurement and 532 nm (G10 nm) in Rayleigh scattering in the air-\ufb02ow to con\ufb01rm the uniformity of the laser sheet, an ICCD camera for two-dimensional measurement and a pulse generator for synchronization between the laser and the ICCD camera. The camera has
0.265 J/cm2 0.465 J/cm2 0.737 J/cm2 1.08 J/cm2
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