Effects of benzene and naphthalene addition on soot inception in a well-stirred reactor/plug flow reactor

A well-stirred reactor (WSR) followed by a plug flow reactor (PFR) is being used to study soot inception. Soot size distributions were measured using two different dilution probes followed by a nano-differential mobility analyzer (nano-DMA). One of the dilution probes was developed for the PFR section, while the second probe was specifically developed for use in the WSR section. Results are presented on the effect of residence time on the soot size distributions obtained for fixed dilution ratio and equivalence ratio. In addition, a technique to inject aromatics and PAH species in the transition region between the WSR and PFR was developed. Results are presented on the effect of benzene and naphthalene on the soot size distributions obtained for differing seeding concentrations and residence times. The results demonstrate for the first time the sensitivity of the soot particle size distribution to the seeding of aromatic species in a WSR/PFR.     

An aerosol model to predict size and structure of soot particles

An aerosol model to simulate soot formation and growth was developed using moving- and fixed-sectional methods. The new model is composed of a set of subroutines that can be easily combined with the Chemkin package. Using the model, we have simulated soot formation and growth in plug flow reactors.

Our model was compared with a previously published method of moments model for a simulation of the plasma pyrolysis of methane in a plug flow reactor. Inclusion of the transition correction factor for the condensation coefficient led to the prediction of a smaller condensation rate compared with the method of moments model. The average coagulation rate calculated by the sectional model was much higher than that by the method of moments model for a broad particle size distribution. The two models predicted significantly different soot precursor concentration and rates of aerosol processes, but substantially similar particle mass and number for the pyrolysis process.

We have also simulated soot formation and growth in a jet-stirred/plug flow reactor (JSR/PFR) system for which soot size distribution measurements are available in the literature. It is shown that the adjusted-point fixed-sectional method can provide comparable accuracy to the moving-sectional model in a simulation of soot formation and growth. It is also shown that the measured surface growth rate could be much higher than the value used in this study. Soot mass concentrations and size distributions for particles larger than 10 nm were well predicted with a surface reaction enhancement. The primary particle size was underpredicted by only about 30% compared with the measurements, without any model adjustments. As the new model can predict both the particle size distribution and structure, and is suitable for application in complex flows, its application to diverse soot formation conditions will enhance our knowledge on the evolution of soot structures.     

Soot particle size distribution measurements in a turbulent ethylene swirl flame

There is a need to better understand particle size distributions (PSDs) from turbulent flames from a theoretical, practical and even regulatory perspective. Experiments were conducted on a sooting turbulent non-premixed swirled ethylene flame with secondary (dilution) air injection to investigate exhaust and in-burner PSDs measured with a Scanning Mobility Particle Sizer (SMPS) and soot volume fractions (f_v) using extinction measurements. The focus was to understand the effect of systematically changing the amount and location of dilution air injection on the PSDs and f_v inside the burner and at the exhaust. The PSDs were also compared with planar Laser Induced Incandescence (LII) calibrated against the average f_v. LII provides some supplemental information on the relative soot amounts and spatial distribution among the various flow conditions that helps interpret the results. For the flame with no air dilution, f_v drops gradually along the centreline of the burner towards the exhaust and the PSD shows a shift from larger particles to smaller. However, with dilution air f_v reduces sharply where the dilution jets meet the burner axis. Downstream of the dilution jets f_v reduces gradually and the PSDs remain unchanged until the exhaust. At the exhaust, the flame with no air dilution shows significantly more particles with an f_v one to two orders of magnitude greater compared to the Cases with dilution. This dataset provides insights into soot spatial and particle size distributions within turbulent flames of relevance to gas turbine combustion with differing dilution parameters and the effect dilution has on the particle size. Additionally, this work measures f_v using both ex situ and in situ techniques, and highlights the difficulties associated with comparing results across the two. The results are useful for validating advanced models for turbulent combustion.     

燃油分级多点喷射低污染燃烧室的化学反应网络模型分析

本文采用基于详细化学反应机理的化学反应网络模型分析了航空发动机燃油径向分级多点喷射低污染燃烧室的NO_x排放特性。该分级燃烧室不同于传统燃烧室,头部由值班区和主燃区两个不同的燃烧区域,根据CFD得到的流场特性和当量比的分布特性对燃烧室进行分区构建化学反应器网络模型,研究了值班级当量比以及值班级和主燃级两级供油比例对排放的影响。同时,还分析了空气进口温度对NO_x排放的影响。得到了较为合理的变化趋势,为低污染燃烧室的初步设计提供了有益的指导。     

In-situ monitoring of UF5 nanoparticle growth in a plug-flow reactor by a low-pressure differential mobility analyzer

The dependence of UF₅ nanoparticle size distribution on growth time was investigated for various initial concentrations of UF₅ monomers. UF₅ nanoparticles prepared by photodissociation of UF₆ in a mixed-flow reactor were allowed to pass through a plug-flow reactor (PFR), and their size distribution was measured by an in-situ size-monitoring system, namely a low-pressure differential mobility analyzer. By changing the length of the PFR, the growth time in the PFR was controlled from 0 to 30 s. An analysis using Lee’s coagulation model revealed that the growth mechanism of the UF₅ nanoparticles involved a Brownian coagulation process and that the sticking probability of the nanoparticles was approximately unity. Received: 27 August 2001 / Accepted: 6 September 2001 / Published online: 20 December 2001     

Influence of polydisperse distributions of both primary particle and aggregate size on soot temperature in low-fluence LII

An improved aggregate-based low-fluence laser-induced incandescence (LII) model has been developed. The shielding effect in heat conduction between aggregated soot particles and the surrounding gas was modeled using the concept of the equivalent heat transfer sphere. The diameter of such an equivalent sphere was determined from direct simulation Monte Carlo calculations in the free molecular regime as functions of the aggregate size and the thermal accommodation coefficient of soot. Both the primary soot particle diameter and the aggregate size distributions are assumed to be lognormal. The effective temperature of a soot particle ensemble containing different primary particle diameters and aggregate sizes in the laser probe volume was calculated based on the ratio of the total thermal radiation intensities of soot particles at 400 and 780 nm to simulate the experimentally measured soot particle temperature using two-color optical pyrometry. The effect of primary particle diameter polydispersity is in general important and should be considered. The effect of aggregate size polydispersity is relatively unimportant when the heat conduction between the primary particles and the surrounding gas takes place in the free-molecular regime; however, it starts to become important when the heat conduction process occurs in the near transition regime. The model developed in this study was also applied to the re-determination of the thermal accommodation coefficient of soot in an atmospheric pressure laminar ethylene diffusion flame. PACS 44.05.+e; 61.46.Df; 65.80.+n     

Investigation of the transition from lightly sooting towards heavily sooting co-flow ethylene diffusion flames

Laminar, sooting, ethylene-fuelled, co-flow diffusion flames at atmospheric pressure have been studied experimentally and theoretically as a function of fuel dilution by inert nitrogen. The flames have been investigated experimentally using a combination of laser diagnostics and thermocouple-gas sampling probe measurements. Numerical simulations have been based on a fully coupled solution of the flow conservation equations, gas-phase species conservation equations with complex chemistry and the dynamical equations for soot spheroid growth. Predicted flame heights, temperatures and the important soot growth species, acetylene, are in good agreement with experiment. Benzene simulations are less satisfactory and are significantly under-predicted at low dilution levels of ethylene. As ethylene dilution is decreased and soot levels increase, the experimental maximum in soot moves from the flame centreline toward the wings of the flame. Simulations of the soot field show similar trends with decreasing dilution of the fuel and predicted peak soot levels are in reasonable agreement with the data. Computations are also presented for modifications to the model that include: (i) use of a more comprehensive chemical kinetics model; (ii) a revised inception model; (iii) a maximum size limit to the primary particle size; and (iv) estimates of radiative optical thickness corrections to computed flame temperatures.     

Detonation propagation across a stratified layer with a diffuse interface

A study was conducted to examine detonation propagation in a stratified layer of hydrogen-oxygen-nitrogen above an inert gas in a horizontal narrow channel. The stratified layer was produced by a gravity current, generated by retracting a door initially separating a hydrogen-oxygen-nitrogen mixture in the predetonator and a heavier inert gas in the test-section. A steady detonation wave generated in the predetonator was transmitted into the stratified layer. The reactivity of the predetonator mixture was varied via the hydrogen-oxygen equivalence ratio and the amount of nitrogen dilution. Schlieren photography was used to visualize the detonation front in the test-section, and soot foils were used to obtain the cellular structure. Schlieren imaging showed a curved detonation front that decoupled at about mid channel height, into a shock wave and trailing contact surface. Both the hydrogen-oxygen-nitrogen reactivity and the type of inert gas initially in the test-section affected the distance travelled by the detonation wave in the stratified layer. The mixture composition distribution within the test-section before ignition was obtained via a three-dimensional CFD simulation. The lateral extent of the cellular structure captured on the soot foil, coincided with the calculated inert gas mole fraction contour that corresponds to a sharp increase in the ZND induction zone length, e.g., 70% argon dilution for a stoichiometric hydrogen-oxygen predetonator mixture.     

Soot and NO emissions control in a natural gas/diesel fuelled RCCI engine by φ-T map analysis

Soot and NO emissions are considered as major pollutants to the atmosphere from compression ignition engines. Researchers have been dedicated to the reduction of soot and NO emissions. Thus, an advance combustion regime, i.e. reactivity controlled compression ignition (RCCI), was proposed to mitigate the formation of these emissions. In this study, the dynamic ?-T (equivalence ratio vs. temperature) map analysis was applied to visualise the combustion processes associated with the in-cylinder temperature and equivalence ratio in an RCCI engine. Therefore, the soot and NO emissions can be efficiently reduced by controlling the combustion process out of the emissions islands on the ?-T map. This analysis method employs KIVA4-CHEMKIN and SENKIN code to construct ?-T maps under various conditions. To find out the significant parameters of controlling combustion process and emissions formation, four parameters were taken into consideration in a natural gas (NG) and diesel fuelled RCCI engine: NG percentage, the first start of injection (SOI) timing, split fraction of diesel and exhaust gas recirculation (EGR) rate. Each parameter was varied at three levels. Finally, the ?-T maps and final soot and NO emissions were compared among varied conditions for each parameter. It is found that the increased NG percentage can significantly reduce soot because of the absence of C-C bond in NG and the reduced diesel fuel impingement on the surface of the piston or cylinder wall. Increasing EGR can decrease the peak combustion temperature due to the dilution effect and thermal effect, consequently maintaining RCCI at low temperature combustion region. This study also indicates that dynamic ?-T map analysis is efficient at manipulating the combustion process to mitigate the soot and NO emissions formation.     

Influence of soot particle aggregation on time-resolved laser-induced incandescence signals

Laser-induced incandescence (LII) is a versatile technique for quantitative soot measurements in flames and exhausts. When used for particle sizing, the time-resolved signals are analysed as these will show a decay rate dependent on the soot particle size. Such an analysis has traditionally been based on the assumption of isolated primary particles. However, soot particles in flames and exhausts are usually aggregated, which implies loss of surface area, less heat conduction and hence errors in estimated particle sizes. In this work we present an experimental investigation aiming to quantify this effect. A soot generator, based on a propane diffusion flame, was used to produce a stable soot stream and the soot was characterised by transmission electron microscopy (TEM), a scanning mobility particle sizer (SMPS) and an aerosol particle mass analyzer coupled in series after a differential mobility analyzer (DMA-APM). Despite nearly identical primary particle size distributions for three selected operating conditions, LII measurements resulted in signal decays with significant differences in decay rate. However, the three cases were found to have quite different levels of aggregation as shown both in TEM images and mobility size distributions, and the results agree qualitatively with the expected effect of diminished heat conduction from aggregated particles resulting in longer LII signal decays. In an attempt to explain the differences quantitatively, the LII signal dependence on aggregation was modelled using a heat and mass transfer model for LII given the primary particle and aggregate size distribution data as input. Quantitative agreement was not reached and reasons for this discrepancy are discussed.     

Multi-lognormal soot particle size distribution for time-resolved laser induced incandescence in diesel engines

In-cylinder and exhaust soot particle size measurements were carried out using time-resolved laser induced incandescence and electrical mobility spectrometer techniques in a single cylinder optical diesel engine and multi-cylinder high-speed diesel engine. The temporal decay of the laser induced incandescence signal from a polydisperse nanoparticle ensemble of soot during transient diesel combustion is shown to be described by both a single-lognormal distribution as well as multi-lognormal size distribution. However, a multi-lognormal particle size distribution is introduced in the existing model for a comprehensive characterisation and realistic reconstruction of the size distribution. Detailed theoretical analysis of multi-lognormal size distribution along with its application to the experimentally measured soot particle size is validated in this work. These results were also qualitatively compared and independently verified by the experimental results obtained by the electrical mobility spectrometer and published transmission electron microscopy data. These findings reveal that the in-cylinder and the exhaust soot particle size distributions in engines are better represented by a multi-lognormal size distribution.     

Picosecond laser-induced fluorescence from gas-phase polycyclic aromatic hydrocarbons at elevated temperatures. II. Flame-seeding measurements

Picosecond laser-induced radiative emission from flames injected with aromatic substances has been measured spectrally and temporally resolved. The measurements were performed in various seeded regions and for different stoichiometric ratios of the surrounding gas. The wavelength of the excitation radiation was 266 nm. Changes in the lifetime and the spectral composition of the emission were observed with changes in the equivalence ratio and the position in the flame. Considerable agreement with previously reported cell measurements was obtained for those regions close to the injection zone. Temperatures were determined from spectrally and temporally resolved measurements. The comparison with elastic scattering gave reasonable results at low seeding rates for naphthalene, and is hoped to be improved even further in future experiments by increasing the time resolution and the signal-to-noise ratio of the measurements. Downstream and towards the surrounding gas, the lifetimes increased and the spectral profiles shifted and broadened towards the red. This effect increased when the equivalence ratio for the surrounding gas decreased and the oxygen concentration increased. The study was also directed towards characterizing features in the emission that could be indicative of a transition from the seeded aromatic substance to the formation of soot. An indicator for molecular or particle growth was the composition of the spectral emission in terms of UV, blue and green–yellow bands and the ratio between elastic-scattering signal and total emission signal. Spatially resolved measurements across the seeding region using a gated intensified CCD camera allowed a closer study of the molecular-growth region from the parent aromatic substance seeded to the soot formed. The fluorescence properties of dimers and their cyclodehydrogenated compounds and polymers containing aryl units are also discussed. Received: 11 July 2000 / Revised version: 30 October 2000 / Published online: 21 February 2001     

Hydrogen enrichment enhances soot formation in swirl-stabilized non-premixed turbulent combustion of ethylene in a model gas turbine combustor

A switch from fossil fuels to hydrogen is currently not feasible mostly due to supply and infrastructure issues. One of the possible approaches, and this is now practiced to a limited extent in industrial gas turbines, is to blend relatively small amounts of hydrogen with fossil fuels curbing the carbon dioxide emissions. However, studies assessing the influence of modest amounts of hydrogen blending with hydrocarbon fuels on soot processes yielded contradictory results. Most of these experimental and numerical studies were performed on laminar diffusion flames and studies on turbulent flames are scarce. One of the confounding factors in assessing the influence of hydrogen is selection of a control experiment in which the fossil fuel is blended with the same amount of an inert diluent. Using helium in the control experiment is preferable because of its similar transport properties and heat capacity to those of hydrogen. Hence, we studied the soot processes in a model gas turbine combustor in which the flame is stabilized by an air swirl. Swirl-stabilized platform ensures that with and without hydrogen/helium dilution, the hydrodynamics of the combustor stays fixed. Base fuel ethylene is supplemented with hydrogen or helium by the same amount to separate the dilution affects and assess the direct chemical interaction of hydrogen related to soot formation. Soot volume fraction and primary soot particle diameters were measured by auto-compensating laser induced-incandescence for all cases. Flow field data obtained using stereoscopic particle image velocimetry is utilized to ascertain the hydrodynamic effects on soot distribution due to addition of lighter species. Soot formation was found to be enhanced by the addition of hydrogen when allowance was made for the dilution effect using the helium doped flame experiments. Possible causes of this observation including the molecular diffusivities of hydrogen and helium, and chemical interaction are discussed.     

Investigation on the influence of soot size on prompt LII signals in flames

Theoretical papers predict that prompt LII signals are weakly dependent on the soot size due to the fact that larger particles reach higher temperatures during the heating process by nanosecond laser pulses. This question is of crucial importance for establishing LII as a practical technique for soot volume fraction measurements. In this work two-color prompt LII measurements have been performed in several locations of diffusion and rich premixed ethylene-air flames. The experimental apparatus was carefully designed with a probe volume of uniform light distribution and sharp edges, a 4 ns integration time around the signal pulse peak and narrow spectral bandwidth. Measurements did not confirm the theoretical predictions concerning an increase of temperature for larger particles. On the contrary, larger particles in richer premixed flames exhibit a lower 400/700 signal ratio. This can probably be attributed to small differences in the refractive index of soot.     

Buoyancy induced limits for nanoparticle synthesis experiments in horizontal premixed low-pressure flat-flame reactors

Premixed low-pressure flat-flame reactors can be used to investigate the synthesis of nanoparticles. The present work examines the flow field inside such a reactor during the formation of carbon (soot) and iron oxide (from Fe(CO)₅) nanoparticles, and how it affects the measurements of nanoparticle size distribution. The symmetry of the flow and the impact of buoyancy were analysed by three-dimensional simulations and the nanoparticle size distribution was obtained by particle mass spectrometry (PMS) via molecular beam sampling at different distances from the burner. The PMS measurements showed a striking, sudden increase in particle size at a critical distance from the burner, which could be explained by the flow field predicted in the simulations. The simulation results illustrate different fluid mechanical phenomena which have caused this sudden rise in the measured particle growth. Up to the critical distance, buoyancy does not affect the flow, and an (almost) linear growth is observed in the PMS experiments. Downstream of this critical distance, buoyancy deflects the hot gas stream and leads to an asymmetric flow field with strong recirculation. These recirculation zones increase the particle residence time, inducing very large particle sizes as measured by PMS. This deviation from the assumed symmetric, one-dimensional flow field prevents the correct interpretation of the PMS results. To overcome this problem, modifications to the reactor were investigated; their suitability to reduce the flow asymmetry was analysed. Furthermore, ‘safe’ operating conditions were identified for which accurate measurements are feasible in premixed low-pressure flat-flame reactors that are transferrable to other experiments in this type of reactor. The present work supports experimentalists to find the best setup and operating conditions for their purpose.     

碳氢混合燃料（C5~C6）气云爆轰胞格结构实验研究

 改进烟迹技术之后，在初始为常温常压的条件下，进行了碳氢混合燃料（C₅~C₆）的气云爆轰胞格结构实验研究，得到了清晰的胞格烟迹记录，同时讨论了燃料气云的当量比和起爆能对胞格结构的影响。实验表明：C₅~C₆混合燃料的爆轰波胞格宽度和胞格长度均随当量比的增加而线性增大；随着起爆能的不断增大，混合燃料的胞格宽度和胞格长度均是先增大后减小，且当起爆能足够高时，在胞格结构内可观察到精细结构的存在。     

Determination of Soot Particle Size in a Premixed Flame: a Static and Dynamic Light Scattering Study

In this contribution we report upon our static and dynamic light scattering experiments to characterize soot particles in flames. We studied sooting laminar premixed flame with acetylene as fuel mixed with air as oxidizer. The air equivalence ratio of the combustion was larger than one. We used a Kaskan type burner with circular geometry and a stabilizing flow of nitrogen around the flame. We focused on the determination of the size of the soot particles in the center of the flame as a function of height above burner. In addition we investigated the influence of the mixing ratio of the gases on the size of the particles. Our results show that static light scattering is better suited than dynamic light scattering for a fast and reliable characterization of soot particles in flames. The latter needs detailed a priori information about the flame to allow the unique determination of sizes from the diffusion measurements. The soot particles grow monotonously with height above burner and with decreasing air equivalence ratio. The aggregates have a fractal dimension lower than two.     

Influence of gas flow rate and reactor length on NO removal usingpulsed power

A short duration of 100-ns pulsed power has been used to remove nitric oxide (NO) in a mixture of nitrogen, oxygen, water vapor, and NO, simulating flue gases from a power station. The effects of the gas flow rate, the reactor length, and the pulse repetition rate on the percentage of NO removal and its energy efficiency are reported. The percentage of NO removal at a fixed gas flow rate increased with increasing pulse repetition rate due to the increased energy into the discharge. At a fixed pulse rate, the removal of NO increased with decreasing gas flow rate due to the increased residence time of the gas in the discharge reactor, thus facilitating the creation of increased radicals of O and N which then decreased NO. The energy removal efficiency of NO (in mol/kWh) decreased with increasing gas flow rate and increasing removal ratio of NO. The removal of NO increased with increasing energy density (J/I), input into the discharge at different reactor length     

Effect of O2 concentration in ambient mixture and multiphase radiation on pollutant formation in ECN spray-A

This study investigates the formation and evolution of soot and NO _X in a high-pressure constant-volume combustion chamber. This work focuses on the effect of multiphase thermal radiation and O₂ dilution in ambient/exhaust gases, sometimes also referred to as exhaust gas recirculation (EGR), qualitatively and quantitatively. The spray-A case (n-dodecane as fuel) from Engine Combustion Network (ECN) is used as the target condition. Two different soot modelling approaches have been considered: a semi-empirical two-equation model and a detailed method of moments with interpolative closure (MOMIC) model. A multiphase photon Monte Carlo (PMC) solver with line-by-line (LBL) spectral data is used to resolve radiative heat transfer. Results show that the effect of radiation on soot is minimal in spray-A. Inclusion of radiation modelling, on the other hand, marginally reduces NO prediction. Both peak soot and NO formation increase with O₂ content in the ambient gas. Oxygen content in ambient gas is also found to have significant effect on soot sizes as the mean soot diameter increases along with considerable widening of the diameter distribution with the increase of O₂ percentage in the ambient gas.     

Measurement of radiative gas and particle emissions in biomass flames

Radiation is the dominant mode of heat transfer near the burner of coal and biomass-fired boilers. Predicting and measuring heat transfer is critical to the design and operation of new boiler concepts. The individual contributions of gas and particle phases are dependent on gas and particle concentration, particle size, and gas and particle temperature which vary with location relative to the flame. A method for measuring the contributions of both gas and particle radiation capable of being applied in harsh high temperature and pressure environments has been demonstrated using emission from particles and water vapor using an optical fiber probe transmitting a signal to a Fourier Transform Infrared (FTIR) spectrometer. The method was demonstrated in four environments of varying gas and particle loading using natural gas and pulverized wood flames in a down-fired 130?kW_th cylindrical reactor. The method generates a gas and particle temperature, gas concentrations (H₂O and CO₂), total gas and particle intensities, and gas and particle total effective emissivity from line-of-sight emission measurements. For the conditions measured, downstream of the luminous flame zone, water vapor and CO₂ radiation were the dominant modes of heat transfer (effective emissivity 0.13–0.19) with particles making a minor contribution (effective emissivity 0.01–0.02). Within a lean natural gas flame, soot emission was low (effective emissivity 0.02) compared to gas (0.14) but within a luminous flame of burning wood particles (500?µm mean diameter) the particles (soot and burning wood) produced a higher effective emissivity (0.17) than the gas (0.12). The measurement technique was therefore found to be effective for several types of combustion environments.