Zari Musavi1, Yao Zhang2, Etienne Robert2, Klas Engvall1. 1. Dept. of Chemical Engineering, KTH Royal Institute of Technology, Stockholm SE-10044, Sweden. 2. Dept. of Mechanical Engineering, Polytechnique Montréal, Montréal QC H3T 1J4, Canada.
Abstract
The formation of soot in a swirling flow is investigated experimentally and numerically in the context of biogas combustion using a CO2-diluted methane/oxygen flame. Visualization of the swirling flow field and characterization of the burner geometry is obtained through PIV measurements. The soot particle size distributions under different fuel concentrations and swirling conditions are measured, revealing an overall reduction of soot concentration and smaller particle sizes with increasing swirling intensities and leaner flames. An axisymmetric two-dimensional CFD model, including a detailed combustion reaction mechanism and soot formation submodel, was implemented using a commercial computational fluid dynamics (CFD) code (Ansys Fluent). The results are compared with the experiments, with similar trends observed for the soot size distribution under fuel-lean conditions. However, the model is not accurate enough to capture soot formation in fuel-rich combustion cases. In general, soot particle sizes from the model are much smaller than those observed in the experiments, with possible reasons being the inappropriate modeling in Fluent of governing mechanisms for soot agglomeration, growth, and oxidation for CH4-CO2 mixtures.
The formation of soot in a swirling flow is investigated experimentally and numerically in the context of biogas combustion using a CO2-diluted methane/oxygen flame. Visualization of the swirling flow field and characterization of the burner geometry is obtained through PIV measurements. The soot particle size distributions under different fuel concentrations and swirling conditions are measured, revealing an overall reduction of soot concentration and smaller particle sizes with increasing swirling intensities and leaner flames. An axisymmetric two-dimensional CFD model, including a detailed combustion reaction mechanism and soot formation submodel, was implemented using a commercial computational fluid dynamics (CFD) code (Ansys Fluent). The results are compared with the experiments, with similar trends observed for the soot size distribution under fuel-lean conditions. However, the model is not accurate enough to capture soot formation in fuel-rich combustion cases. In general, soot particle sizes from the model are much smaller than those observed in the experiments, with possible reasons being the inappropriate modeling in Fluent of governing mechanisms for soot agglomeration, growth, and oxidation for CH4-CO2 mixtures.
Soot formation has traditionally been a problem in diesel internal
combustion engines, open fires, and large boilers.[1,2] Soot
particles are produced as a result of incomplete combustion processes
in gas phase reactions, where hydrocarbon molecules may start growing,
eventually condensing and agglomerating to form dense particles.[3] Soot formation is generally undesirable; it represents
an energy loss from unreacted carbon, although its presence can be
beneficial to enhance radiative heat transfer. Soot causes significant
harm because of its polluting effects. It is responsible for certain
health problems associated with inhaling fine soot particles, as well
as changing the planet albedo by deposition on frozen surfaces. Soot
formation also brings problems in industrial processes downstream
of the combustion itself, such as polymerization and clogging of equipment,
which can result in process shutdowns.Thermochemical or biological
biomass conversion processes yield
gas mixtures of varying compositions such as syngas and biogas. These
gas mixtures can be used as they are but are often processed into
hydrocarbons suitable for replacing fossil fuels, such as biomethane
and liquid biofuels. Chemical reactions such as partial oxidation
(POX)[4,5] and catalytic reforming play a critical
role in such conversion processes. They are, however, very sensitive
to soot formation and fouling.Combustion and soot formation
modeling are challenging tasks to
begin with, especially when dealing with a complex mixture of combustible
gases. In general, a combustion reaction mechanism is developed for
specific fuels. Examples include the GRI-3 mechanism,[6] the Konnov 0.5 mechanism,[7] and
the Petersen mechanism[8] for methane and
natural gas oxidation reactions, the USC II mechanism[9] for C1–C4, benzene, and toluene oxidation, as well
as the LLNL mechanism[10] for oxidation of
C7–C20 hydrocarbons. However, model complexity increases dramatically
when the complex molecules involved in soot formation are considered.
For instance, a model developed by MIT (296 species and 1322 reactions)
includes the formation and destruction of soot particles and PAHs
up to three condensed rings in addition to combustion of hydrocarbons
up to benzene.[11] Numerical models implementing
these mechanisms in CFD simulations of realistic conditions of burners
and POX reactors are very computationally expensive, with experimental
datasets essential to assess the validity of the choices made in model
development.Numerous works combining chemical kinetics modeling
and experiments
in combustion and soot formation in laminar premixed and non-premixed
flames have been performed.[12−19] Model results compared with experiments show that even in simple
flames, there are difficulties in predicting soot.[20,21] These kinetic models are developed and evaluated using programs
such as FlameMaster, RMG, REACTION, and ANSYS Chemkin. Although many
studies and fundamental research efforts aim to increase the understanding
of soot formation mechanisms, combining detailed combustion mechanisms
with realistic flow field to capture the effects of choices made in
the numerical model on soot inception, growth, and oxidation has seldom
been done. Verification of the models is mainly done comparing ignition
delay and flame speed in zero- or one-dimensional models and the experiments.[20,22−26] Gas mixtures encountered in syngas and biogas conversion processes
are rarely considered in soot studies, and research efforts are needed
to assess the capabilities of available numerical tools.[5,27]In the present study, experimental and numerical modeling
tools
were combined to investigate the interactions between soot formation,
chemical kinetics, and turbulence in a swirling non-premixed burner
geometry. A burner with adjustable swirl was built and an axisymmetric
two-dimensional CFD model was implemented in the same geometry. The
combination refers to the specification of the boundary conditions
for the numerical model from measurements of the flow field obtained
at the same location. The computational domain is also defined to
precisely match the burner geometry. Accurate flow components at the
inlets, measured through the experiments, are applied as boundary
conditions to the simulated model. Detailed combustion kinetics and
soot mechanisms are used to model the dynamics of the reacting flow,
including soot formation, oxidation, particle size growth, and size
distribution in a realistic geometry and flow field. To model the
biogas composition, a mixture of methane and carbon dioxide is selected
for simplicity in this initial modeling approach. Oxygen is selected
as the oxidizing agent, diluted with CO2, as oxycombustion
is more common in secondary gas treatment, and CO2 is one
of the species present in the raw gas with a typical concentration
in the range of 10–19% for different processes.[27]The experimental and numerical methods
are described in the Methodology section.
The results from experimental
datasets were obtained for both cold and reacting flows, with comparison
with numerical simulations presented in the Results
and Discussion section.
Methodology
In this
work, a swirling jet flame is investigated both numerically
and experimentally. This configuration was selected as it is simple
enough to allow for numerical modeling at a reasonable computational
cost while still providing a mean to control the effect of the fluid
mechanics on the chemical kinetics through the swirl number.
Experimental Section
Experimental Setup
Requirements
for an adjustable swirl burner along with the ability to preheat the
reactants to high temperature guided the choice of the Cambridge–Sandia
swirl burner geometry for this investigation.[28] Unlike most other swirl burners described in the literature,[29−32] the Cambridge–Sandia design allows control of the swirl number
without moving parts. The whole burner assembly can therefore be placed
in an oven as shown in Figure a, and the swirl number is changed from the outside using
flow controllers, adjusting the gas flow rate sent through the different
channels of the burner. The burner consists of two cylindrical annular
channels, one where the gas injection is purely axial (inlet A in Figure a), surrounded by
a swirling channel (inlets B and C) where the gas can be injected
either axially or tangentially. The swirl number is changed through
the ratio between the axial and tangential flow rates in the swirling
channel. Compared to the original Cambridge–Sandia burner geometry,
two modifications were made in the present study. First, all tubes
were shortened by 100 mm to extend the swirling number range. Second,
thin separators were added between the tubes to achieve a consistent
alignment and better flow field uniformity.
Figure 1
(a) Schematic representation
of the modified Cambridge–Sandia
swirl burner used in this study, which is enclosed in an oven for
reactant preheating; (b) two-dimensional geometry used for numerical
studies; (c) entire mesh; (d) close view of the mesh near to and far
from the inlet boundaries.
(a) Schematic representation
of the modified Cambridge–Sandia
swirl burner used in this study, which is enclosed in an oven for
reactant preheating; (b) two-dimensional geometry used for numerical
studies; (c) entire mesh; (d) close view of the mesh near to and far
from the inlet boundaries.The combustion takes place in a transparent quartz chamber to enable
access for optical diagnostic tools. The burner has an axisymmetric
geometry, providing the benefit of allowing 2D velocity measurements
to be used to reconstruct the 3D flow fields, thereby significantly
reducing experimental complexity. The region of highest interest is
found from the burner exit to 100 mm downstream, where gas mixing
and heat release occur followed by partial oxidation; soot formation
is thought to begin in this area.To enable a comparison between
experiment and numerical simulation,
the boundary conditions of the flow field were carefully assessed
using Particle Image Velocimetry (PIV) in cold flow conditions. The
swirl number of the burner was also characterized from these cold
flow measurements. The PIV technique consists of a pulsed laser (Nd:YAG),
a double-framing camera, optical lenses, and an aerosol generator
to seed the flow (TOPAS ATM 221). Image processing and analysis was
performed using the DaVis software from LaVision.
Cold Flow Characterization
The
flow swirl improves the mixing of gases, extending the flame stability
limits. To characterize the swirl behavior, a combination of 2D velocity
fields, acquired at the burner upstream boundary, was used to calculate
the swirl number. Equation , as specified by Chigier and Beér,[33] was used for calculating the swirl number, where R is the radius of the outer inlet annulus and w and u are the tangential and axial velocity components.The axial
velocity
component, u, is extracted from a 2D velocity field
taken in a plane perpendicular to the burner axis. The tangential
velocity component, w, is extracted from the velocity
field taken in a plane parallel to the burner axis. The PIV measurements
used to characterize swirl number are acquired at an axial location
5 mm above the burner exit, captured by a lens with high magnification
and a narrow field of view (f = 105 mm, Nikon), which
allows for a fine spatial resolution close to the burner exit.
Reacting Flow Conditions
For the
reacting flow cases investigated, methane was used as a fuel, and
oxygen was used as an oxidizer. Both the fuel and the oxidizer were
diluted with carbon dioxide. The fuel mixture was injected to the
inner channel, and the oxidizer mixture was injected through the outer
channel, as it requires a larger cross section to achieve the desired
velocities. A range of fuel concentrations was investigated, with
mixture strengths ranging from 0.46 to 1.15 to cover lean, stoichiometric,
and rich conditions. The swirl number was also varied to cover low-,
medium-, and high-swirl conditions.All flow conditions considered
here are listed in Table . Note that the mixture strength φ defines the stoichiometrically
weighted ratio of the fuel mass flow rate to the oxidizer mass flow
rate in both annular inlets of the burner, where all cases at φ
< 1 and at φ > 1 are fuel-lean and fuel-rich, respectively.
Table 1
List of Reacting Flow Cases
case number
SN
inner flow rate (L/min)
methane flow
rate (L/min)
total outer flow rate (L/min)
oxygen flow rate (L/min)
mixture strength, φ
c1
0.29
5
2
10
8
0.46
c2
0.29
5
3
10
8
0.69
c3
0.29
5
4
10
8
0.92
c4
0.29
5
5
10
8
1.15
c5
0.51
5
2
10
8
0.46
c6
0.51
5
3
10
8
0.69
c7
0.51
5
4
10
8
0.92
c8
0.51
5
5
10
8
1.15
c9
0.82
5
2
10
8
0.46
c10
0.82
5
3
10
8
0.69
c11
0.82
5
4
10
8
0.92
c12
0.82
5
5
10
8
1.15
To assess
the effects of the flame chemistry and swirl number on
soot formation, soot particle size distributions and concentrations
were measured using a Scanning Mobility Particle Analyzer Sizer (SMPS)
(TSI Incorporated Model 3980). The particle size range that can be
detected with the operating conditions implemented is between 9 and
311 nm. This range covers the vast majority of particles that are
present downstream of the reaction zone, but very small incipient
soot particles that might form in lean combustion conditions could
not be detected experimentally. Although the presence of such small
particles might be relevant in some applications, they have a negligible
impact on the total mass of particulate matter generated by the flame.
When such particles are of interest, the modeling tools evaluated
here can be a valuable option to overcome the limitations of experimental
tools to detect very small particle sizes.The SMPS measurements
were carried out well downstream of the reaction
zone 60 cm from the injection of the burner nozzle, corresponding
to approximately two times the flame height. The flow was continuously
sampled through a 4 mm inner diameter stainless steel tube with sample
flow rate of 0.3 L/min and sheath flow rate of 8 L/min, resulting
in conditions in the sampling line where aggregation is expected to
be negligible.[23] However, the sampling
approach implemented in the present work does not allow the mapping
of soot concentration and size distribution in space or time; the
measurement collected provides only an average value of the soot characteristics
downstream of the reaction zone.
Numerical
Analysis
ANSYS Workbench
and ANSYS Meshing were used for preparing the geometry and building
the computation grid, respectively. ANSYS Chemkin-Pro was used in
preparing, combining, and reducing the chemical reaction mechanisms
to be coupled with the CFD in the ANSYS Fluent.
General
Flow Model
A two-dimensional
(2D) axisymmetric geometry is considered as shown in Figure b–d. The symmetric nature
of the flow field inside the reaction zone was verified against the
PIV results with no significant azimuthal variations. The dimensions
of the inlet boundaries are shown in Figure b, with detailed parameters defined in Figure a and reported in Table S1.
Figure 2
(a) Geometry of all boundaries and (b)
dimensions of the inlet
boundaries in mm.
(a) Geometry of all boundaries and (b)
dimensions of the inlet
boundaries in mm.No curvatures and complex
elements exist in the burner geometry,
as shown in Figure b, and therefore equilateral or equiangular elements, i.e., quad
mesh, could be used to create the grid. Three different grids, based
on the maximum mesh sizes of 0.4, 0.3, and 0.2 mm, were constructed.
To achieve a better resolution around the inlet boundaries, a finer
mesh of 0.05 mm was implemented locally. A comparison between the
meshes in terms of number of nodes and elements, the mesh quality,
and the standard deviation of mesh quality is given in Table . To find a suitable compromise
between mesh size and computation requirements, the meshes were pre-evaluated
and compared with experimental results for the nonreacting cases.
Two mesh sizes (0.3 and 0.2 mm) were able to capture the results well,
and the finer mesh was used in all following CFD cases. This is important
for reacting flow simulation, where details in the spatial distribution
of the reaction rate can be captured more accurately with the finer
mesh shown in Figure c–d.
Table 2
Mesh Data for Three Differently Constructed
Meshes
max element size (mm)
number of nodes
number of elements
element quality,
average
element quality, standard deviation
0.4
222,972
219,476
0.9218
0.23793
0.3
384,147
379,505
0.93938
0.21044
0.2
802,312
799,971
0.9829
0.064251
The
experimentally measured flow fields at the inlet boundaries
were used as input for the model boundary conditions. The axial (u) and radial (v) velocity components for
the inner inlet boundary followed a parabolic distribution along the
radius of the jet. For the outer annular (swirling) inlet boundary,
the measured velocity component (w) deviated from
a purely parabolic and symmetric distribution, with the maximum velocity
located toward the outer wall. Functions were fitted to these experimentally
measured velocity profiles and used as boundary conditions in the
numerical model through user-defined functions (UDFs).The Transition
SST model with standard constants[34] was
applied to model the flow and turbulence. The model
is based on the coupling of the κ–ω transport equations
(two equations) with two other transport equations, one for the intermittency
and one for the transition onset criteria, in terms of the momentum–thickness
Reynolds number. Two other methods, RSM (Reynolds stress model) and
RNG k-ε (renormalized group k-epsilon),[34] were compared to the SST model on a cold flow case, and the results
showed that the Transition SST has much better agreement with the
experimental results. A comparison between the k-ε and the SST
model on the reacting flow also supported the choice of the SST model,
although the k-ε turbulence model showed a smoother convergence.
A comparison of mean velocity contours between three turbulent models
and the experimentally measured data is available in Figure S1 in the Supporting Information.
Reactive Model
A reaction mechanism
based on GRI-Mech 3.0 [6] was coupled to the flow model to account
for the gas phase combustion reactions. Since the oxidizer stream
excluded nitrogen, a reduced version of the GRI-3 mechanism (36 species
and 219 reactions) was prepared using Chemkin-Pro (see files in the Supporting Information). To obtain soot particle
distribution information, the Method of Moments[35] was used with three moments applied.To account for
radiation effects, a semitransparent model for the walls was implemented.
Mixed radiation, conduction, and convection heat transfers were included
in the modeling of the outer wall of the burner. Interactions between
soot formation, turbulence, and radiation are also included in the
CFD model. The effect of soot on radiation is considered by its effect
on the absorption coefficient. A summary of all numerical settings
and models is given in Table S2.Mesh independence analysis was conducted first through examining
residuals for all equations (momentum, turbulence, species, soot,
energy, and radiation) decreased to 1e–6. Then,
stability of the values of interest was examined at monitor points
and along defined lines, as well as along their contours in the whole
zone, to ensure reliable results. The monitored values consisted of
concentrations of main species and radicals CH4/O2/CO2/H2O/OH/C2H2, temperature,
and flow field. Furthermore, the net flux imbalance through the domain
boundaries was assessed, which was at an accepted level of 0.5% imbalance.
Results and Discussion
Cold
Flow
Figure shows the global flow field obtained from
PIV measurements. The dimension of field of view is 80 mm × 110
mm, allowing the observation of large-scale features in the flow field.
Figure 3
Global
flow field behavior with different swirling level ((a, d)
weak swirl, SN = 0.29; (b, e) moderate swirl, SN = 0.51; (c, f) high swirl, SN = 0.82).
The top row is the front view. The bottom row is the top view.
Global
flow field behavior with different swirling level ((a, d)
weak swirl, SN = 0.29; (b, e) moderate swirl, SN = 0.51; (c, f) high swirl, SN = 0.82).
The top row is the front view. The bottom row is the top view.As shown in Figure a, with a weak swirl (SN = 0.29),
the flow field
remains largely uniform as an annular jet in solid rotation. In Figure b, when increasing
the swirl intensity, shear layer instabilities appear at the interface
between the swirling and axial inlets, and the jet opens at a height
of approximately 60 mm. When the swirling magnitude is at its maximum
(SN = 0.82), as shown from the top view in Figure f, a recirculation
zone appears approximately 80 mm above the burner exit plane in the
middle of the jet.The comparison of cold flow fields from PIV
measurements and CFD
simulations from different cases are reported in Figure . In each figure, experimental
results (left) and CFD simulations (right) are placed side by side.
Overall, they agreed with each other very well; some minor differences
are caused by the following possible reasons. First, the color scales
are slightly different as the numerical results provide more resolutions
for the velocity. Second, in some experimental results, a slight asymmetry
is observed between the two sides of the burner as shown in Figure . This asymmetry
could be caused by slight misalignment of the coaxial tubes comprising
the burner inlet. When using experimentally measured velocity profiles
as boundary conditions for the numerical model, the average value
of the axial component measured on both sides of the jet is used.
For the tangential component, the information is extracted from transverse
velocity fields, and any asymmetry caused by misalignment is therefore
reflected in the boundary. The numerical results are close to an average
between the right and left side of the burner. The asymmetry is higher
in cases with large flow difference between u and w, such as cases SN = 0.09 and SN = 0.43. The characterization cases gathered in cold flow
are used as input parameters for reacting flow calculations.
Figure 4
Comparison
of 2D longitudinal velocity field between experiments
and numerical results for respective cases: (a) case SN = 0.13; (b) SN = 0.22; (c) SN =
0.26; and (d) SN = 0.31.
Figure 5
2D velocity
fields (m/s) showing slightly transient asymmetry in
two of the experimental cases compared to their respective computational
results.
Comparison
of 2D longitudinal velocity field between experiments
and numerical results for respective cases: (a) case SN = 0.13; (b) SN = 0.22; (c) SN =
0.26; and (d) SN = 0.31.2D velocity
fields (m/s) showing slightly transient asymmetry in
two of the experimental cases compared to their respective computational
results.The swirl number in the burner
depends exclusively on the total
flow rate and the ratio of the axial to the tangential flow rate in
the swirling annular inlets, with the other axial channel also contributing
to the total flow rate. To investigate the effect of those two parameters,
the analysis presented in the following covers three datasets—two
datasets with constant system total flow rates of 10 and 15 L/min
and one dataset with variable total flow rates.Numerical swirl
numbers were calculated as described in Section using the
2D flow field in a plane 5 mm above the inlets. The results from the
experiments and simulations (Figure ) are in good agreement, demonstrating that the user-defined
functions used as boundary conditions in the numerical model adequately
represent the inlet flow.
Figure 6
Characterization of swirl number for different
total flow rates;
experimental results are shown with points and numerical results are
shown in lines.
Characterization of swirl number for different
total flow rates;
experimental results are shown with points and numerical results are
shown in lines.When the total flow rate is kept
constant in the swirling channel,
the swirl number increases approximately linearly with the ratio of
axial and tangential injection flow rates. A higher swirl number can
be achieved up to a point with higher total flow rates. Note that
the availability of a dataset with a constant flow rate in the swirling
channel is important to study the effect of swirl number at constant
mixture strength.When the total flow rate is varied along with
the ratio of tangential
to axial flow injection, to maximize the swirl number, a plateau is
observed with a maximum value of approximately 0.8. Conclusively,
the experimental configuration is therefore suitable for covering
situations typically referred to as weak (SN <
0.3), moderate (0.3 > SN < 0.6), and high (SN > 0.6) swirl levels.
Reactive
Flow
Measurement of Soot Formation
Figure shows the results
from these SMPS measurements as a function of mixture strength and
swirl number. When burning under very fuel-lean conditions (φ
= 0.46), soot formation for all swirl number cases is very low, which
is less than 0.1% of the values measured under the other fuel conditions.
Considering the background aerosol measured in the lab, measured without
a flame in the chamber, soot formation under such ultra-lean conditions
can be disregarded. The other combustion cases, φ = 0.69, 0.92,
and 1.15, exhibit rather narrow size distributions, with particle
sizes from 9 nm (the lower detection limit) up to 80 nm. This is close
to the size range of 20 to 60 nm (standard deviations of 15–25%)
typically observed for primary soot particles,[36] which are the building blocks for larger aggregate particles
formed continuously[37] and are only visible
in our measurements in low numbers for the richest flame condition.
Particles with diameters over 311 nm or below 9 nm are therefore not
expected in significant amounts under the test conditions investigated.
Figure 7
Experimentally
measured soot size distribution for different reacting
flow cases, where N = soot particle number density
(particles/m3), and the normalized number concentration,
dN/dlogDp, is calculated by dividing
dN by the geometric width of the size channel.
Experimentally
measured soot size distribution for different reacting
flow cases, where N = soot particle number density
(particles/m3), and the normalized number concentration,
dN/dlogDp, is calculated by dividing
dN by the geometric width of the size channel.A significant effect of the swirling flow fields
can be observed
for all other burning conditions (φ = 0.69, 0.92, and 1.15)
in Figure . In general,
the highest swirl number results in lower soot particle concentration
and particle sizes. This is potentially due to a better mixing between
the fuel and the oxidizer provided by the swirl, resulting in a more
efficient combustion process and better soot oxidation and, thus,
a reduced production of smaller soot particles.For lean flames
(φ = 0.69), the swirl is very effective at
mitigating soot formation. Under those conditions with high swirl
number, the flames are almost soot-free in sharp contrast to the measurement
at low or medium swirl number. For close-to-stoichiometric and rich
flames (φ = 0.95, φ = 1.15), although the swirl still
reduces the amount of soot present, there is no such drastic suppression
of soot formation. High and medium swirl numbers, however, still appear
to yield similar effects at higher mixture strength, reducing the
production of soot particles although only to a certain extent. Considering
that acquiring such experimental datasets is very time-consuming,
only representative cases were investigated. To cover flame conditions
ensuring an adequate validation of the numerical model, a 3 ×
4 full factorial experimental design was implemented to assess the
effect of swirl intensity and mixture strength.
Numerical Simulation of Soot Formation
Figure shows the
numerically calculated soot particle size distributions and number
density for different mixture strengths for high-swirling intensity
cases c9–c12 evaluated at the location where the experimental
data was taken. The trend for the growth of the soot particle size
as a function of the fuel strength is similar to the trend observed
in the SMPS measurements, with progressively richer flows yielding
larger particles, ultra-lean (φ = 0.46) < stoichiometric
(φ = 0.92) < fuel-lean (φ = 0.69) < fuel-rich (φ
= 1.15). This is an expected result since all fuel-lean cases with
φ < 1 could achieve complete combustion. The numerical results
capture well that such lean flames have a very low amount of soot
formation and are supported by the experimental results, where insignificant
amounts of soot were measured for particle sizes above 9 nm. For the
fuel-rich case (φ = 1.15), the particle sizes from the numerical
results show growth up to 900 nm, which are much larger particle sizes
compared to the limit value of 311 nm that could be measured by the
SMPS in the configuration used in the experiments. However, the amount
of such large particles is insignificant compared to the total amount.
Thus, this is not the most interesting region of this study, since
most of the particles are within the region below 200 nm.
Figure 8
Particle size
distribution obtained from the numerical model for
high-swirl cases (cases c9–c12); results for different mixture
strengths 0.46, 0.69, 0.92, and 1.15.
Particle size
distribution obtained from the numerical model for
high-swirl cases (cases c9–c12); results for different mixture
strengths 0.46, 0.69, 0.92, and 1.15.Comparing soot particle sizes obtained from the numerical simulations
and the experimental measurements for the fuel-lean cases, φ
< 1, reveals that the simulations predict particles much smaller
than those observed in the experiments. This can be due to either
an underestimation of the soot growth rate or an overestimation of
the soot oxidation rate in the numerical model. The latter case appears
to influence the results more substantially. When looking at soot
growth over the entire combustion chamber, the numerical results reveal
the existence of very large soot particles in the range of 150 to
230 nm formed for cases c3, c7, and c11. These large particles are
subsequently oxidized and therefore not detected 60 cm above the nozzle,
where the comparison with the experiments is carried out. As a result,
the average particle sizes at the outlet sampling point for fuel-lean
cases remain below 5 nm (Figures –10). This discrepancy is most likely caused by an overestimation in
the model of the radical concentration (O and OH) in the postflame
region of the combustion chamber. These radicals are known to rapidly
oxidize soot.[24,38−41] The cause of this overestimation
is, however, not known but could originate in the boundary conditions
used for radiation or in the reduced chemical kinetics used. This
could be better understood by the validation of concentrations of
radical species in this zone against experiments. Unfortunately, the
present experimental setup does not have this possibility. For fuel-rich
cases such as c12 (shown in Figure ), there is no possibility for the model to overestimate
the concentration of radical oxidants (O and OH) in absence of excess
oxygen; consequently, the numerical results tend to exhibit similar
trends to those observed in the experiment.
Figure 10
Particle
size distribution obtained from the numerical model for
low-swirl cases (cases c1–c4); results for different mixture
strengths 0.46, 0.69, 0.92, and 1.15.
Particle size distribution
obtained from the numerical model for
medium-swirl cases (cases c5–c8); results for different mixture
strengths 0.46, 0.69, 0.92, and 1.15.Particle
size distribution obtained from the numerical model for
low-swirl cases (cases c1–c4); results for different mixture
strengths 0.46, 0.69, 0.92, and 1.15.Soot particle size distributions predicted numerically for medium-swirling
flow fields for different mixture strengths are shown in Figure , revealing a mode
heavily skewed toward much smaller particles compared to what was
observed experimentally. Keeping in mind that the SMPS does not allow
measurements of particles smaller than 10 nm, the main peak shown
in the simulation results could therefore not be captured experimentally.
For the fuel-rich case (Figure ), the soot mean diameter () among the sampled numerical particles
is 44 nm. This is slightly smaller compared to 57 nm from the experimental
results. However, the maximum diameter for soot particles is 178 nm,
which is significantly smaller than the experimentally measured size
of 311 nm. One potential factor that affects the numerical soot sizes
is the average soot particle density of 1800 kg/m[3] used for all numerical cases, which is the most often used
value in the literature.[26] This density
is more relevant to fuel-rich cases, and therefore, particle sizes
deviate more from experimental results in fuel-lean cases.
Figure 9
Particle size distribution
obtained from the numerical model for
medium-swirl cases (cases c5–c8); results for different mixture
strengths 0.46, 0.69, 0.92, and 1.15.
The
soot particle size distributions obtained from the numerical
model for low-swirl flow fields for different mixture strengths are
shown in Figure . For all φ, the soot particle sizes predicted by simulations
are much smaller than those observed in experiments. This is even
seen for the fuel-rich case, φ = 1.15, in contrast with the
moderate- and high-swirl cases described above and shown in Figures and 9.The effect of swirl on numerically predicted soot
particle size
is shown in Figure for φ = 0.92 and 1.15. Comparing soot number density between
medium- (red) and high-swirl (black) flows, it is seen that increasing
the swirl helps in soot number reduction for both cases.
Figure 11
Particle
size distribution obtained from the numerical model as
a function of swirl number for mixture strengths 0.92 and 1.15.
Particle
size distribution obtained from the numerical model as
a function of swirl number for mixture strengths 0.92 and 1.15.The comparison between numerical and experimental
results in terms
of the soot particle size distribution demonstrates that the numerical
model captures well the effect of the flow field. Moreover, these
results show that the agreement is better for high-swirl number cases.
However, the soot model itself has a poor ability to accurately predict
the soot size distribution and number density measured experimentally.
The coupling of several numerical submodels in this work to cover
combustion kinetics, soot formation, and population development, radiation,
and swirling effects showed that even when using very accurate experimental
data for the boundary conditions, the simulation tool cannot give
a quantitative prediction of soot particle size distributions. Although
the commercial codes can be used to assist in the design of partial
oxidation reactors, users should be aware of their limitations in
the prediction of soot size distribution.
Conclusions
In the present study, experimental and numerical
tools are used
to investigate soot formation in a swirling burner. A burner allowing
control over the swirl intensity was manufactured and operated to
cover weak-, moderate-, and high-swirl conditions for a methane/oxygen
flame with variable stoichiometry. The soot particle size distribution
was obtained from a scanning mobility particle sizer (SMPS), with
results showing that increased swirl has a significant effect in reducing
soot concentration and sizes under all burning conditions. For lean
flames, swirling is very effective at mitigating soot formation. However,
for rich flames, swirl helps reduce the production of soot particles
but only to a certain extent.The numerical modeling of soot
particle sizes and concentrations
is attempted using a commercial CFD code (ANSYS Fluent), including
the effect of turbulence, detailed combustion kinetics, radiation,
soot formation, and oxidation. For a few flame conditions, the simulation
yielded trends similar to those observed in the experiments, but in
general, the numerically simulated soot particle sizes are much smaller
than those measured. Possible reasons for these differences include
limitations in soot-related submodels and the fact that the available
SMPS instrument could not detect particles below 10 nm, a size range
for which the numerical model predicted very high concentrations.The numerical modeling of soot particle sizes has always been a
challenging problem. The agreement between the results of the numerical
simulation and the experimental measurements could be slightly improved
by tweaking the parameters of the soot model, for instance, by using
different average soot particle densities for fuel-rich and fuel-lean
cases. However, as our results demonstrate, quantitative numerical
prediction of soot concentrations and size distributions in complex
turbulent flows would require the development and implementation of
significantly more advanced models for soot particle nucleation, growth,
aggregation, and oxidation.