Energies 07 04710
Energies 07 04710
3390/en7074710
OPEN ACCESS
energies
ISSN 1996-1073
www.mdpi.com/journal/energies
Article
School of Mechanical, Electronic and Control Engineering, Beijing Jiaotong University, Beijing 100044,
China; E-Mails: [email protected] (H.-M.L.); [email protected] (Z.-Y.S.);
[email protected] (Y.Z.); [email protected] (Z.-H.Z.)
Received: 2 April 2014; in revised form: 10 July 2014 / Accepted: 15 July 2014 /
Published: 22 July 2014
Keywords: premixed flame; syngas flame; intrinsic instabilities; critical flame radius
Energies 2014, 7 4711
1. Introduction
With the increased energy demands and concerns about environmental protection, the development
and the application of high efficiency clean combustion has attracted more and more attention.
Lean mixture combustion has a number of positive features such as providing high thermal efficiency
and reducing emissions [1–5]. Synthesis gas (syngas) has attracted significant interest in the field of
energy and combustion as a promising alternative and an environmentally clean fuel [6,7].
Syngas primarily consists of H2 and CO and can be derived from numerous sources. Syngas can be
used in many power devices, such as gas turbines for integrated gasification combined cycle systems
(IGCC) [8]. However, designing suitable combustors is a big challenge because of the significant
variations in the composition of syngas due to the feedstock and gasification techniques [9]. Hence,
the study of the fundamental combustion characteristics of H2/CO premixed flames under different
hydrogen fractions is important for further applications of syngas.
In a premixed flame, the appearance of cellular instabilities wrinkles the flame front and accelerates
flame propagation, flame front instabilities may also contribute to the transition from deflagration to
detonation [10]. The intrinsic instabilities of premixed flames are caused by hydrodynamic,
diffusive-thermal, and body-force instabilities [11]. Hydrodynamic instability, which is caused by the
expansion across the flame sheet [12,13], is present in all flames [14–16]. Diffusive-thermal instability,
which is caused by the preferential diffusion of mass and heat [17,18], is only present in the flames with
Lewis number (Le) < 1 [19–22]. Body-force instability, which is caused by the effect of buoyancy [23],
is only apparent when the laminar propagation speed of the flame is low [24].
Up to now, a few studies have reported the cellular instabilities from experimental investigations;
some scholars have studied the cellular instabilities of premixed hydrogen-air flames [25–29]. The
cellular instabilities of mixtures of premixed hydrogen-hydrocarbon-air flames have also been studied
by many scholars [30–35]. Nevertheless, studies about cellular instabilities of premixed syngas flames
are relatively sparse, and most of the reported articles were mainly focused on cellular instabilities
induced by the addition of inert gas or hydrocarbon under selected hydrogen fractions [36–40]. As a
matter of fact, syngas is a blended fuel which mainly consists of H2 and CO, so the cellular instabilities
of syngas premixed flames are very complex due to the hydrogen fraction variation. To provide more
information about the cellular instabilities of syngas premixed flame, this study focuses on lean and
stoichiometric premixed H2/CO/air flames as the research object to perform a systematic study on the
cellular instabilities of syngas premixed flames under different hydrogen fraction conditions. The
phenomena of cellular instabilities of lean premixed syngas flames have been observed at different
hydrogen fractions (from 0% to 100%), equivalence ratios (φ, from 0.4 to 1.0) and elevated initial
pressure of 0.3 MPa.
The experimental method used in this study is mainly composed of six parts: a closed combustion
vessel, discharge system, ignition system, optical access system, high-speed camera and data
acquisition and control system (Figure 1).
Energies 2014, 7 4712
Surroundings
6052C
Vacuum pump
Digital camera
Digital camera
The closed combustion vessel is made of stainless steel and has a cubic inner chamber with a length
of 140 mm. The 2-quartz windows of the vessel have effective diameters of 100 mm and are
oppositely mounted. The discharge system includes five individual passages, namely, hydrogen bottle,
carbon monoxide bottle, air bottle, vacuum pump and environment. The ignition system consists of a
12 V transistorized automotive ignition coil and a pair of tungsten–copper electrodes that are
oppositely mounted on the two sides of the vessel other than the windows. The optical access system is
Z-shaped and is mainly composed of one lamp, two flat reflectors, two slits and two concave mirrors
with diameters of 200 mm and focal lengths of 2000 mm. The high-speed camera used is an IDT Motion
Pro-Y4 (IDT, Newark, NJ, USA) operating at 10,000 frames per second with a resolution of
256 pixels × 256 pixels, the individual frame exposure is 3 μs with lamp power of 200 W. The data
acquisition and control system mainly consists of two electrical pressure transmitters, one piezoelectric
absolute pressure transducer associated with a charge amplifier and a data acquisition system. The two
electrical pressure transmitters employed, namely, a DPA01M-P (with a band from −100.0 to
100.0 kPa) and DPA10M-P (with a band from −0.001 to 0.999 MPa), were produced by the Delta Group
(Taiwan). The piezoelectric absolute pressure transducer is Kistler 6052C, and the discharge ampler is
Kistler 5018A (Kistler, Winterthur, Switzerland). The synchronizer trigger employed is developed by
the authors.
Procedurally, the vessel evacuated, and the mixture is prepared by adding hydrogen, carbon
monoxide and air according to Dalton’s law of additive pressure under the monitoring of the
DPA01M-P and/or DPA10M-P units. The discharge process in the present investigation can be divided
into the following stages: (i) the vessel is filled with hydrogen and carbon monoxide until the reading
shown at the panel of the DPA01M-P has reached the desired value; (ii) the vessel is filled with air
until the reading shown at the panel of DPA01M-P or DPA10M-P has reached the initial mixture
pressure; (iii) once the desired mixture is prepared, 20 min is required to ensure the homogeneity and
quiescence of the mixture. Finally, a control signal is sent to activate both the ignition system and
high-speed camera synchronously, and the delay from the ignition to capture is set to
4 ms. The propagation of flame within the vessel is captured by the camera, whereas the variation of
pressure on the inner wall of the vessel is recorded by the Kistler pressure transducer. Prior to refilling
Energies 2014, 7 4713
for the next set of experiment, the vessel is flushed twice with dry air to remove any residual products.
Thereafter, the vessel is evacuated again. In this study, the hydrogen is pure hydrogen with a purity of
99.995%, the carbon monoxide is pure carbon monoxide with a purity of 99.95% and the air is
commercial grade compressed dry air with an oxygen-to-nitrogen volume ratio of 21:79.
In the study, at least three measurements have been performed at each condition for obtaining the
average value. The initial pressure is measured by a pressure transmitter which accuracy is 0.001 MPa; the
variation in initial pressure is 0.3 ± 0.001 MPa, so the relative error for the initial pressure is 0.3%.
The high-speed camera is operated at 10,000 frames per second with a resolution of
256 pixels × 256 pixels, and the spatial resolution is 0.39 mm/pixel. The error bars in the figure
reflects the corresponding standard deviations of laminar burning velocity and critical flame radius on
the multi-times repeated experiments.
Within the closed combustion vessel, the premixed flame outwardly propagates spherically.
The stretched flame propagation speed (Sb) can be derived from the data of flame radius versus time:
dR
Sb (1)
dt
where R is the instantaneous flame radius and t is the elapsed time from the spark ignition. The flame
propagation is affected by the electrodes when the flame is small, such as during the initial propagation
period, and by the wall when the flame is sufficiently large, such as when constant pressure is absent in
the spatial environment wherein the flame propagates. Thus, only flame radii between 6 [41] and 20 mm
(about 0.3 times the radius of the wall [42]) are employed to avoid the aforementioned effects.
K is the temporal rate of the change of a flame surface element of area A:
d(ln A) 1 dA
K (2)
dt A dt
K is defined as follows in the case of a spherically expanding laminar flame:
1 d 4πR 2 dR 2
2
1 dA
K Sb (3)
A dt 4πR 2 dt R dt R
A linear relationship exists between the laminar flame propagation speed and K [43]:
Sb Sb0 Lb K (4)
where Lb is the Markstein length of burned mixtures and can be obtained as the negative value of the
slope of the Sb K curve. Sb is the unstretched flame propagation speed and can be considered the
0
0
flame propagation speed without any stretch effect on the flame front; thus, Sb can be obtained as the
intercept value at K = 0.
During the initial propagation period, the flame can be considered to propagate under constant
pressure. Su0 can be calculated from the mass conservation across the thin flame:
ρ
Su0 Sb0 b (5)
ρu
Energies 2014, 7 4714
where ρb is the density of the burned mixture and ρu is the density of the unburned mixture calculated
with the chemical equilibrium program GASEQ.
Darrieus and Landau discovered that hydrodynamic instabilities are mainly caused by thermal
expansion, which can be indicated by the thermal expansion ratio and flame thickness [26].
The thermal expansion ratio (σ) is defined as the ratio of unburned gas density to that of burned gas,
which is calculated as:
σ ρu / ρb (6)
where ρu and ρb, the unburned and burned gas densities, respectively, can be obtained via
thermodynamic calculation. The higher the density jump is, the stronger the destabilization becomes.
Flame thickness (δ) can be determined by the temperature profile of the flame structure [40], which is
calculated as:
Tad Tu
δ (7)
(dT / dx)max
where Tad is the adiabatic temperature; Tu is the unburned gas temperature; and (dT/dx)max is the
maximum slope of the temperature profile. The (dT/dx)max is determined using the premixed flame
code PREMIX of the CHEMKIN-PRO package and the GRI3.0 Mechanism is used [44], since these
where in close agreement with the present experimental laminar burning velocity data. With the
decrease in flame thickness, the hydrodynamic instability increases due to the weaker influence of
curvature and the enhanced intensity of induced baroclinic torque [26].
The diffusive-thermal instability is caused by the competing effects of heat conduction and the
reactant diffusion [45] and can always be quantitatively determined using the Lewis number (Le),
which is defined as the ratio of the heat diffusivity to mass diffusivity of the deficient reactant to the
abundant inert [46] and is used to describe diffusive-thermal instabilities, LeH2 and LeCO can be
calculated as expressed by the equation:
λ / Cp
Le (8)
ρD
where λ C p ρ is the thermal diffusivity; Cp is the specific heat at constant pressure; λ is the heat
conductivity; ρ is the density of the unburned mixture; and D is the mass diffusivity. For premixed
syngas flames, two fuels exist in the reactants, and the Lewis number can thus be evaluated using the
method by Law et al. [30], which is expressed as:
qH2 ( LeH 2 1) qCO ( LeCO 1)
Le 1 (9)
q
where q = qH2 + qCO is the total heat release, with qi (i refers to H2 or CO) being the non-dimensional
heat release associated with the consumption of species i, defined as qi = QYi/CpTu, where Q is the heat
Energies 2014, 7 4715
of reaction; Yi is the supply mass fraction of species i; cp is the specific heat of the unburned gas; and
Tu is the unburned gas temperature. LeH2 and LeCO are the Lewis numbers of H2-air mixture and CO-air
mixture at φH2 and φCO, respectively, where φH2 = (nH2/nA)/(nF/nA)st, φCO = (nCO/nA)/(nF/nA)st are the
H2, and CO-based equivalence ratios, respectively, nH2, nCO, nF, nA are the mole fractions of H2, CO,
fuel and air in the reactant mixtures [33,37]. The diffusive-thermal instability is enhanced with the
decrease of Lewis number [26].
Published results of laminar burning velocities of H2/CO/air mixtures at 0.3 MPa are lacking, but
there are lots of published experiment data of laminar burning velocity with hydrogen fractions of 10%
and 50% at 0.1 MPa.
To validate our experimental results, the additional laminar burning velocity of syngas/air mixtures
at the pressure of 0.1 MPa has been measured and compared with previously published results. Figure 2
shows the measured laminar burning velocity of H2/CO/air mixtures compared with those of previous
studies [42,47–52]; all the data were measured with a spherically propagating flame at Pu = 0.1 MPa and
all data are in good agreement. This proves the correctness of the data obtained in this investigation.
0.8
Su0(m/s)
0.6
0.4
0.2
0
0.5 0.6 0.7 0.8 0.9 1 1.1
Equivalence ratio
Krejci MC,2013(50%H2-50%CO) Bouvet,2011(50%H2-50%CO)
Burke,2009(50%H2-50%CO) Prathap,2008(50%H2-50%CO)
Sun,2007(50%H2-50%CO) Hassan,1997(50%H2-50%CO)
McLean,1994(50%H2-50%CO) Bouvet,2011(10%H2-90%CO)
Hassan,1997(10%H2-90%CO) Present work(50%H2-50%CO)
Present work(10%H2-90%CO)
Figure 3 gives the unstretched laminar burning velocity versus hydrogen fraction for mixtures with
various equivalence ratios at Pu = 0.3 MPa. The data of Park [39] for a 50%H2/50%CO mixture at
φ = 1.0 is also plotted in the figure and present work gives value consistent with Park’s experimental
Energies 2014, 7 4716
results. Simulations using the GRI Mesh 3.0 mechanism are also plotted in the figure and in general
give good predictions on the unstretched laminar burning velocities of H2/CO mixtures, although the
predicted results are higher than the experimental results for some cases, so the mechanism is also used
to ccalculate (dT/dx)max for getting the flame thickness. The unstretched laminar burning velocity of
H2/CO mixtures increases with increasing hydrogen fraction and equivalence ratio.
1.6
Experiment(φ = 0.6)
1.4 Experiment(φ = 0.8) 0.3MPa
Experiment(φ = 1.0)
1.2
Park,2010(φ = 1.0)
Simulation(φ = 0.6)
1
Su0(m/s)
Simulation(φ = 0.8)
0.8 Simulation(φ = 1.0)
0.6
0.4
0.2
0
0% 10% 20% 30% 40% 50% 60%
Hydrogen fraction
Figures 4 and 5 show the Schlieren images of premixed syngas-air flames with R = 20 mm with
different hydrogen fractions and equivalence ratios, respectively. As shown in Figure 4, for the syngas
premixed flame with φ = 0.4, the geometric centre of the flame was obviously lifted up from the initial
position (namely, the ignition position) when the hydrogen fraction is below 50%, which means that
the body-force instabilities are enhanced. Flames with lower hydrogen fractions show the body-force
instabilities more evidently. With the increase of hydrogen fraction for all the equivalence ratios, more
cells appear on the flame front. When the hydrogen fraction is higher than 50%, as shown in Figure 5,
small cells become uniform over the entire flame front, which means the destabilisation propensity
tends to be progressively promoted. From the observation, the cellular instability phenomena are
obviously enhanced with the increase in hydrogen fraction for the same equivalence ratio.
However, for the same hydrogen fraction, the effects of equivalence ratio on the variation of cellular
instability vary. As shown in Figure 5, with hydrogen fractions above 50%, the flame tends to become
more unstable with the decrease in equivalence ratio. This phenomenon is similar to seen for natural
gas-hydrogen-air premixed flames reported by Huang et al. [35].
However, with hydrogen fractions below 50%, the flame tends to be more stable with the decrease in
equivalence ratio, as shown in Figure 4. This observation has never been reported in any previous study.
Energies 2014, 7 4717
Figure 4. Schlieren pictures for flames with hydrogen fractions from 10% to 50% at 0.3 MPa
at different equivalence ratios for 20 mm radius.
φ=0.4 φ=0.6 φ=0.8 φ=1.0
10%H2-90%CO
20%H2-80%CO
30%H2-70%CO
40%H2-60%CO
50%H2-50%CO
Figure 5. Schlieren pictures for flames with hydrogen fractions from 60% to 100% at
0.3 MPa at different equivalence ratios for 20 mm radius.
φ=0.4 φ=0.6 φ=0.8 φ=1.0
60%H2-40%CO
70%H2-30%CO
80%H2-20%CO
90%H2-10%CO
100%H2
Energies 2014, 7 4718
A detailed process of the propagation of the flames with hydrogen fraction of 30% is shown in
Figure 6. For the premixed syngas flame with hydrogen fraction of 30% and φ = 0.4, several large
cracks are induced by the ignition disturbances during the early propagation period, and those cracks
continue to develop without branching as the flame further propagates. For the premixed syngas flame
with φ = 0.6 to 1.0, the large cracks formed during the early propagation period become branched as
the flame further propagates, and the phenomenon becomes more apparent at higher equivalence
ratios. The flame tends to be more unstable with the increasing equivalence ratio. Instead, the cellular
instabilities of syngas premixed flames decrease with the increase in equivalence ratio with the
hydrogen fraction of 80%, as shown in Figure 7. To give a qualitative explanation, the parameters
reflecting flame instability were calculated.
Figure 6. Schlieren pictures for flames of 30%H2-70%CO at 0.3 MPa at different equivalence
ratios for different radius.
φ=0.4 φ=0.6 φ=0.8 φ=1.0
10mm
15mm
20mm
25mm
Figure 7. Schlieren pictures for flames of 80%H2-20%CO at 0.3 MPa at different equivalence
ratios for different radius.
φ=0.4 φ=0.6 φ=0.8 φ=1.0
10mm
15mm
20mm
25mm
Energies 2014, 7 4719
Figure 8 illustrates the variation in Lewis number with hydrogen fraction at different equivalent
ratios at a pressure of 0.3 MPa. The Lewis number generally decreases with the increase in hydrogen
fraction. The results indicate that the diffusive-thermal instability of lean syngas premixed flame is
enhanced with the increase in hydrogen fraction. In addition, with the increase in equivalence ratio
with hydrogen fractions less than 50%, the Lewis number nearly remains at the same value. For the
premixed syngas flames with hydrogen fractions of more than 50%, the Lewis number at the same
hydrogen fraction decreases with the decrease in equivalence ratio, which implies that the flame of low
equivalence ratio is more unstable in terms of diffusive-thermal instability compared with the flame of
relatively high equivalence ratio.
0.9
0.8
0.7
Le
0.6 φ = 0.4
0.5 φ = 0.6
φ = 0.8
0.4
φ = 1.0
0.3
0.3MPa
0.2
0% 10% 20% 30% 40% 50% 60% 70% 80% 90% 100%
Hydrogen fraction
Figure 9 shows the flame thickness versus the hydrogen fractions for different equivalence ratios at
0.3 MPa. The flame thickness decrease significantly with the increase in hydrogen fraction and
equivalence ratio. The decreased flame thickness results in an enhancement of the flame’s destabilising
propensity because of the weakened influence of curvature on the flame front as well as the
strengthened baroclinic torque intensity, so the hydrodynamic instability is enhanced with the increase
in hydrogen fraction and/or equivalence ratio for decreasing flame thickness.
0.035
0.03
Flame thickness(mm)
0.025
0.02
0.015
0.01
0.3MPa
0.005
φ = 0.6 φ = 0.8 φ = 1.0
0
0% 10% 20% 30% 40% 50% 60% 70% 80% 90% 100%
Hydrogen fraction
Energies 2014, 7 4720
Figure 10 shows the thermal expansion ratio versus the hydrogen fractions for different equivalence
ratios at 0.3 MPa. For a specific equivalence ratio, the thermal expansion ratio decreases
inconspicuously with the increase in hydrogen fraction. In addition, for a specific hydrogen fraction,
the thermal expansion ratio increases with the increase in equivalence ratio. The results indicate the
hydrodynamic instability is enhanced with the increase in equivalence ratio. Based on the above
discussions, for a specific hydrogen fraction, the hydrodynamic instabilities of syngas premixed flames
are enhanced with the increase in equivalence ratio for both decreasing flame thickness and increasing
thermal expansion ratio.
7.5
7
Thermal expansion ratio
6.5
5.5
4.5
0.3MPa
4
φ = 0.4 φ = 0.6 φ = 0.8 φ = 1.0
3.5
0% 10% 20% 30% 40% 50% 60% 70% 80% 90% 100%
Hydrogen fraction
In general, when the hydrogen fraction is less than 50%, the enhancement of the cellular
instabilities of the syngas premixed flame with the increase in equivalence ratio can be attributed to the
dominant effect of the hydrodynamic instabilities. Furthermore, compared with the inconspicuous
variation in thermal expansion ratio, the variation in flame thickness induced by the hydrogen fraction
dominantly influences the intensity of hydrodynamic instabilities. At hydrogen fractions greater than
50%, the decline in the cellular instabilities induced by the increase of equivalence ratio can be
attributed to the reduced diffusive-thermal instabilities rather than increasing hydrodynamic
instabilities. With the increase in hydrogen fraction, the enhancement of the cellular instabilities of
H2/CO/air premixed flames results from the diffusive-thermal instability as the Lewis number
decreases and the hydrodynamic instability as the flame thickness decreases.
During the initial flame propagation period, the cellular instabilities are suppressed by the strong
stretch, and the suppressions decline and even extinguish as the flame expands. The “critical flame radius”
(which is defined as the flame radius at which cells are smaller than the branched cracks and are no longer
suppressed) has been employed to denote the onset of cellularity. As shown in Figure 11, the point at which
the flame speed begins to accelerate rapidly with decreasing stretch defines a critical flame radius
because the onset of cellularity is the primary reason of the self-acceleration of the flame [53,54].
Energies 2014, 7 4721
7
60%H2-40%CO Pu=0.3MPa Ф=1.0
5
1000 1200 1400 1600 1800 2000 2200 2400 2600
K(1/s)
Figure 12 shows the critical flame radius versus the hydrogen fractions at different equivalence
ratios. The data of Park [39] for a 50%H2/50%CO mixture at φ = 0.8 and 1.0 is also plotted in the
figure and the same trend is found. The critical flame radius evidently decreases with the increase in
hydrogen fraction and increases with the increase in equivalence ratio at hydrogen fractions greater than
50%. However, the critical flame radius decreases with the increase in equivalence ratio at hydrogen
fractions lower than 50%. This phenomenon is consistent with the observation of flame front photos.
19
φ = 0.6
φ = 0.8
17 φ = 1.0
φ = 0.8(Park)
φ = 1.0(Park)
Critical radius(mm)
15
0.3MPa
13
11
7
20% 30% 40% 50% 60% 70% 80% 90% 100%
Hydrogen fraction
Critical Peclet number (Pecr), also representing the cellular instability, which is defined the ratio of
critical flame radius to laminar flame thickness [55]. Figure 13 shows the critical Peclet number versus
Energies 2014, 7 4722
the hydrogen fraction. Critical Peclet number is influenced by the combined effects of critical flame
radius and flame thickness. The critical Peclet number decreases with the increase in hydrogen fraction
at hydrogen fractions lower than 50%. However, with the increase in hydrogen fraction at hydrogen
fractions greater than 50%, the critical Peclet number increases with equivalence ratios of 0.8 and 1.0,
and the critical Peclet number changes little with an equivalence ratio of 0.6.
1000
900
800
Pecr
700
600
500
400
φ = 0.6 φ = 0.8 φ = 1.0
300
20% 30% 40% 50% 60% 70% 80% 90% 100%
Hydrogen fraction
4. Conclusions
In the present work, the cellular instabilities of different hydrogen/carbon monoxide blends were
studied using the outwardly propagating flame in a constant volume combustion bomb at elevated
pressure and room temperature. The laminar burning velocities of syngas/air mixtures were measured
and compared with previously published results and computed results and good agreements are
obtained. The major conclusions of the study are as follows:
(1) When hydrogen fractions are above 50%, the flame tends to be more stable as the equivalence
ratio increases; however, the instability increases for flames of lower hydrogen fractions.
(2) For the premixed syngas flames with hydrogen fractions lower than 50%, the effects of
equivalence ratio on the variation in the Lewis number can be neglected. With the increase in
equivalence ratio, the cellular instabilities become more evident because the enhanced
hydrodynamic instabilities become the dominant effect.
(3) For the premixed syngas flame with hydrogen fractions greater than 50%, the decline in
cellular instabilities induced by the increase in equivalence ratio can be attributed to the
reducing diffusive-thermal instabilities rather than the increasing hydrodynamic instabilities.
(4) For the premixed syngas flame, the enhancement of cellular instabilities induced by the
increase in hydrogen fraction is the result of both increasing diffusive-thermal and increasing
hydrodynamic instabilities.
Energies 2014, 7 4723
Acknowledgments
The present investigation is primarily supported by the Ph.D Programs Foundation of Ministry of
Education of China (No. 20110009110023) and the Fundamental Research Funds for the Central
Universities (No. M11JB00300).
Author Contributions
The author contributions list is as follows: Study concepts were proposed by Guo-Xiu Li and
Hong-Meng Li. Literature research and study were designed by Hong-Meng Li and Guo-Xiu Li.
Experimental studies and data acquisition were done by all the authors. Data analysis/interpretation
and statistical analysis were done by Hong-Meng Li, Guo-Xiu Li, and Zuo-Yu Sun. Definition of the
intellectual content of the manuscript, manuscript preparation and editing was made by Hong-Meng Li.
Manuscript revision/review was made by Hong-Meng Li and Guo-Xiu Li. Manuscript final version
was approved by Guo-Xiu Li.
Conflicts of Interest
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