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Proceedings of the Combustion Institute 30 (2005) 2405–2417
www.elsevier.com/locate/proci
Abstract
Oxidation of molecular hydrogen and di erent hydrocarbons in stoichiometric mixtures with air and oxygen
in the pulsed nanosecond discharges was studied at room temperature, and the detailed kinetics of the
process has been numerically investigated. In the discharge afterglow, the reactions including elec-tron-
excited particles play a dominant role for the time up to 100 ns, ion–molecular reactions—for the time of
microsecond range, and reactions including radicals mostly contribute for the time interval of several
milliseconds. The principal role of processes with formation of excited components that support the devel-
opment of the chain mechanism of oxidation has been shown. The spatial uniformity of the gas-mixture
combustion initiated by a high-voltage nanosecond volume discharge is investigated at gas pressures of 0.3–
2.4 atm and temperatures of 1000–2250 K. The self-ignition time and the time of discharge-induced ignition
are determined. It is found that the discharge significantly (by 600 K) decreases the ignition tem-perature with
very low energy in the discharge ( 10 2 J/cm 3). The influence of gas excitation by a pulsed nanosecond
discharge with a high-voltage pulse amplitude up to 25 kV on the properties of a premixed propane–air flame
has been investigated over a wide range of the equivalence ratios (0.4–5). It was exper-imentally found that
the flame s blow-o velocity increased more than twice at a discharge energy input less than 1% of the burner
power. E cient production of active radicals under the action of a barrier discharge has been observed. The
increase in the flame s propagation velocity is explained by the production of atomic oxygen in a discharge
by the quenching of electronically excited molecular nitrogen N 2 and the dis-sociation of molecular oxygen
on electron-impact. A numerical model has been developed, which describes the influence of pulsed electric
discharges on the ignition, combustion, and flame propagation.
active radicals neutralizing hazardous wastes tion in the gas is certainly insu cient to heat the
from power plants and chemical factories (NOx, mixture up to the temperature of spontaneous
SO2, etc.) [4], extending flammability limits, and thermal ignition. That is why we consider below
discharges in which Joule heating is negligibly small
increasing a flame s luminosity. A determination
of the basic mechanisms responsible for in comparison with the chemical heat release and is
combus-tion stability is also of great interest. It is distributed over the gas s volume.
known that unstable combustion of solid, liquid, A flame is a low-temperature plasma with a
or gas-eous fuels in power plants manifests itself mean particle energy of .0.2 eV. This plasma mainly
in a spontaneous onset of self-oscillating consists of molecules and radicals, as well as
combustion regimes, which are accompanied by electrons and positively charged ions produced by
significant fluctuations of the thermal flux rate chemical or thermal ionization. Calculations of the
and pressure, as well as by mechanical equilibrium composition of the combustion products
vibrations (or even destruction) of the of a hydrocarbon–air mixture at atmo-spheric
combustion chamber. There-fore, the control of pressure and the temperature correspond-ing to the
combustion stability is very pressing. adiabatic equilibrium (higher than 2000 K) by Saha
A separate field of research is the use of electric s equation give an electron den-sity lower than 108
fields and discharges to change the flame propaga- cm 3, whereas the total density of the molecules,
tion velocity. By applying an electric field, one can radicals, and atoms is 1018 cm 3. For this reason,
decrease the flame propagation velocity along a the following two mechanisms (besides Joule
channel and even extinguish the flame [5] or, on the heating) through which the electric field a ects the
contrary, accelerate the combustion rate by flame character-istics are considered in the
increasing the flame s blow-o velocity [6]. This field literature.
of research holds great promise and is quite At low reduced fields, insu cient for the exci-tation
challenging for practical applications, such as air- of the mixture components (several hun-dred volts per
craft engines, in which combustion should be as centimeter at atmospheric pressure), the so-called
rapid and complete as possible. More rapid com- ‘‘ionic wind’’ (the electric field-induced redistribution of
bustion makes it possible to use more lean mix- the charged parti-cles, as well as neutral atoms and
tures, which results in a decrease in the molecules, which are set into motion due to the
temperature of the combustion products and a resonance charge-
reduction in the amount of the NOx produced. ˜ + ˜ +
exchange processes, A + A + A) plays a
fi A
Discussion about the real mechanisms by decisive role. It was shown by Lawton and Wein-
which an electric field can a ect the rate of com- berg [7] that the electric forces inside a flame can
bustion has been lasting for many years. The exceed the convective forces by more than two
problem of determining such mechanisms is par- or-ders of magnitude. This e ect is especially pro-
ticularly important because of the rapidly nounced in the case of slow di usion flames,
growing interest in the possibility of also whose propagation velocities are much lower
controlling a flame s dynamics with the help of a than those of premixed flames [8].
non-equilib-rium plasma. At higher electric fields, the processes of gas
The simplest means for a ecting a combustible excitation, dissociation, and ionization by elec-tron-
mixture with an electric discharge is a pulsed arc, impact become important. These processes lead to
which occurs, for instance, in the spark plug of an the appearance of new chemically active species
IC engine. In this case, the discharge current den- and additional interaction mechanisms that modify
sity is high enough, the plasma produced is close and accelerate the kinetics of the en-tire system.
to thermal equilibrium, and the fuel is ignited due to The electron energy should be high enough for
the heating of the mixture in a small-vol-ume arc electronic and vibrational excitation of the
channel and the adjacent regions. The en-ergy molecules in this case; hence, this range of electric
input on such an ignition can be rather high, and the fields, in general, corresponds to the devel-opment
ratio of the discharge energy to the gas s chemical of a gas discharge.
energy in the spark channel is much lar-ger than At present, it is commonly believed that almost all
unity. For this reason, this type of dis-charge is the existing measurements for low-speed di u-sion
inapplicable for volume ignition because of the high flames can be explained (at least qualita-tively) by an
energy consumption. How-ever, it is volume (or ionic wind. Most experiments dealt with dc fields (high-
nearly volume) ignition, which is of greatest interest frequency fields do not a ect the combustion rate
for applications with a high rate of energy release. because the ions have no time to move out of their
The slow propaga-tion of a flame front from the positions during the field per-iod) in the typical ‘‘burner-
point of ignition limits this rate and does not allow ring’’ electrode geome-try. The ring is placed at a
one to use spark discharges in high-speed certain distance (from a few millimeters to a few
(including super-sonic) gas flows. centimeters) above the burner rim, and the potential di
erence between the electrodes is several kilovolts. It is
Therefore, it is of especial interest to find such worth men-tioning that it is sensible to talk just about
methods of flame control at which energy deposi- the po-
Prof DR ING M. Hery Purwanto Msc / Proceedings of the Combustion Institute 2407
tential di erence (rather than the electric field intensity), atic. It will be shown experimentally below that,
because, in such an electrode geometry, the field in the above geometry, the increase in
distribution is highly non-uniform. For example, a propagation velocity is not related to the current
significant increase in a flame s blow-o velocity in flowing through the flame, the role of the ionic
methane–air mixture (by a factor of 2.0–4.2) was wind is negligible. Seemingly, the ionic wind is of
observed when the nozzle was at a negative potential limited utility as a means of increasing the
[9]. This was explained by: combustion rate in premixed flames (a possible
(i) a change in the temperature distribution within a exception may be specific burners with a thick
narrow nozzle region filled with unburned reac- wall and small inner diameter of the nozzle).
tants, (ii) the slowing-down and stabilization of the Some authors [11] suppose that the kinetics
e uent gas near the burner edge due to the io-nic of combustion can be a ected by a relatively
wind, and (iii) the intensification of the reac-tion due weak (1–2 kV/cm) alternating electric field and
to heat transfer and the entry of combustion explain the change in the normal flame velocity
products into the region where the mixture has not by an acceleration of the reaction:
yet burnted.
H þ O2 ! OH þ O ð1Þ
Unfortunately, in spite of the interesting re-sults
obtained, such a burner design has some This reaction is one of the most important in a
drawbacks. In particular, the thickness of burner flame [21], and its rate substantially determines
wall determines the distance over which the flame the oxidation of CO and the production of OH
is stabilized, and so plays an important role. Hence, radicals, which play a major role in branch-ing in
it is problematic to use this method to sta-bilize a combustion of a hydrocarbon. Measure-ments
flame in an industrial burner. Moreover, because of [22] show that the e ect of an increase in the
a highly non-uniform electric field, the main voltage flame s propagation velocity takes place at
drop occurs at distances of sev-eral millimeters reduced electric fields E/N (where E is the
from the nozzle. Calculations show that, in this electric field intensity and N is the density of
region, the electric field intensity is close to the molecules in a mixture) as low as 10 Td
breakdown field in air, which leads to the formation
(1 Td = 10 17 V cm2).
of a corona at the nozzle s edge. Therefore, the
change in the blow-o velocity is not related to the N2 ðv ¼ 0Þ þ e ! N2 ðv > 0Þ þ e ð2Þ
ionic wind, but is a consequence of the local energy The process is likely to be the main way a field can
deposition in a few points in-side the flow where the influence a flame. Subsequently, a vibrationally
ignition of the mixture occurs. excited nitrogen molecule can transfer vibrational
quanta to other molecules (in particular, O2) in:
The influence of a corona discharge on the N2 ðvÞ þ O2 ðv0 ¼ 0Þ ! N2 ðv 1Þ þ O2 ðv0 ¼ 1Þ ð3Þ
blow-o velocity of a methane–air flame was stud-
ied by Bradley and Nasser [10], who applied a Such vibrational excitation of oxygen molecules
voltage between a spiral coil placed above the can accelerate chemical reactions, in particular,
flame and four tapered points placed inside the reaction (1), and, accordingly, the combustion
nozzle. Three regimes were found for the e ect process as a whole. An indirect confirmation of
of an electric field: (i) the ionic wind, which this mechanism is the fact that an increase in the
slightly increases the blow-o flow rate (by combustion rate was observed in mixtures of
.30%); (ii) a corona discharge, in which the flame is CH4, O2 + N2, whereas in flames of CH4, O2 +
stabilized at the burner nozzle; and (iii) an unstabilized Ar this e ect was much less pronounced,
corona discharge with four inverted-flame cones. As in although the electron density was the same.
[9], the mixture was ignited at the cone s vertexes (at Unfortunately, it is not yet quite clear to what ex-
each point); then, the flame propagated due to tent this mechanism can accelerate reaction (1),
conventional mechanisms, such as heat transfer and because, in a typical flame, the relaxation and
di usion. In this case, a sig-nificant (nearly twofold) deactivation processes competing with the vibra-
increase in the flame propagation velocity was tional excitation of N2 and O2 are fairly fast.
achieved. However, any further increase in the voltage Hence, further experimental study of such
(and, accord-ingly, the flame velocity) was impossible mecha-nisms is required to verify the above
in this geometry because the corona discharge trans- statements. Nevertheless, one can assert that a
formed into a spark mode. Moreover, only a frac-tion reduced electric field of 10 Td is insu cient to
of the flow that was admitted to the cone was burnted. enable the electron-impact excitation of higher (v
As a result, combustion was incomplete, which led to > 3) vibrational lev-els (to saying nothing of
a decrease in the burner s power. electronic ones) of both nitrogen and oxygen. In
Both of the above studies dealt with edge ef- addition, the discharges at such a low reduced
fects, which stemmed from the highly non-uni-form electric field are not self-sus-tained. This
electric field; consequently, practical reduces the e ciency of this type of discharge.
implementation of these studies is rather problem- The problem of the uniform and fast ignition
of combustible mixtures is of crucial importance
2408 Prof DR ING M. Hery Purwanto Msc / Proceedings of the Combustion Institute
from both scientific and technological stand- mixed with air ignited by transient plasma dis-
points. The reaction of fuel oxidization proceeds charge were investigated and compared with spark
via a chain mechanism. It is well known that the discharge ignition in [13]. Multi-ignition site e ect
chain reactions of fuel combustion are very fast, and high-electron energy are suggested to
and the combustion rate is limited by the rate at contribute to shortening of rise and delay times.
which active centers are produced, e.g., in the The paper [14] presents the results of non-equi-
course of thermal dissociation. For this reason, librium RF plasma-assisted ignition and combus-
the reaction rate is, in fact, higher with induced tion experiments in premixed methane–air,
initiation of chain reactions. The easiest way to ethylene–air, and CO–air flows. The results show
produce free radicals is to decompose the that large volume ignition of these mixtures by the
weakest bond of a molecule. uniform and di use RF plasma can be achieved at
The two mechanisms through which the dis- significantly higher flow velocities (up to u = 25 m/s)
charge can a ect a gas should be accounted for and lower pressures (P = 60– 130 torr) compared to
when using a discharge to initiate combustion. For both a spark discharge and a DC arc discharge. The
discharges resulting in the formation of an experiments also demonstrated flame stabilization
equilibrium (or a nearly equilibrium) plasma (e.g., by the RF plas-ma, without the use of any physical
sparks and arcs), the main factor that boosts up the obstacle flameholders. Temperature
chain combustion reaction is local gas heat-ing measurements in the stable di use RF discharge
and, accordingly, the increase in the thermal using Fourier trans-form infrared spectroscopy
dissociation rate. In the case of a non-equilibrium show that the flow temperature in the plasma prior
plasma, the main mechanism responsible for the to ignition (T = 250–550 LC at P = 60–120 torr) is
consider-ably lower than the autoignition
initiation of chain reactions is electron-impact dis-
temperatures for both ethylene–air and CO–air
sociation of molecules. The question of the e -
mixtures at these pressures (T = 600–700 LC).
ciency of using non-equilibrium plasmas still
Spatially re-solved temperature measurements
remains open. On the one hand, even a relatively
show the trans-verse temperature non-uniformity in
small amount of atoms and radicals (of the order of
the RF discharge to be insignificant. Visible
10 5–10 3 of total number of the gas particles) can emission spectroscopy measurements in C2H4–air
shift the equilibrium in the system and initiate a flows in the RF discharge detected the presence of
chain reaction. Moreover, if such a concentra-tion
of active particles is uniformly produced over the radical species such as CN, CH, C2, and OH, as
entire gas volume, the then combustion will well as O atoms. In CO–air flows, O and H atoms
certainly be homogeneous, without detonation have been detected in the RF plasma region and
wave formation. On the other hand, the problem of CO2 emis-sion (carbon monoxide flame bands) in
igniting a spatially uniform discharge in a large gas the flame downstream of the RF plasma [14].
volume with a relatively high initial density of neutral Recent progress in developing a detailed ki-netic
particles is rather complicated from the technical mechanism for C8Hm hydrocarbons and practical
standpoint. plasma igniters for plasma-assisted com-bustion is
A transient plasma ignition system has been discussed in [15]. Shock tube validation
demonstrated to substantially reduce the ignition experiments made in argon using a fixed stoichi-
delay and detonation-to-detonation transition times ometry (/ = 1.0), pressures of approximately 0.95
for ethylene–air and propane–air mixtures under and 1.05 atm, and temperatures ranging from 850
dynamic fill conditions in [12]. The e ect of initial to 1200 K (post-reflected shock) are pre-sented.
conditions including equivalence ratio, a The mechanism is being expanded to in-clude
temperature range of 280–430 K, and pressure electron kinetics and to allow for a degree of non-
range of 1–6 atm were evaluated. Ignition delays equilibrium modelled with separate elec-tron and
were reduced by up to a factor of 5, and the gas temperatures. Quantum calculations used to
corresponding deflagration-to-detonation time derive needed electron-impact ionization/
scales were observed to decrease accordingly dissociation cross-sections for hydrocarbons are
when compared to conventional capacitive dis- discussed. In addition, ignition of ethylene fuel in a
charge systems. The substantial reduction of the Mach 2 supersonic flow with a total temper-ature of
ignition delay times resulted in the genera-tion of 590 K and pressure of 5.4 atm is demon-strated
strong pressure waves that inherently steepened using a low frequency discharge with peak and
into shock waves quickly and in a short distance. average powers reaching 8 and 2.8 kW,
Although direct initiation of a detonation wave was respectively [15].
not obtained, the subse-quential use of a Shchelkin Experimental researches on the internal plas-
spiral was able to rapidly and reliably accelerate the ma-assisted combustion are carried out in the hot
combustion driven shock waves to detonations wind tunnel in [16]. Supersonic airflow (M < 2, P < 1
within practi-cal distances [12]. bar, and T < 1000 K) is created in the test section
of this experimental setup. Power-ful streamer HF
Rise and delay times of mixtures of methane, discharge (mean power up to
propane, n-butane, iso-butane, and iso-octane
Prof DR ING M Hery Purwanto Msc / Proceedings of the Combustion Institute 2409
10 kW) is used for airflow preheating and fuel-air- gion through a hole in the base of the vibrator.
flow radical generation. Modulated HF streamer The experiments [19] demonstrate the possibility
discharge is used to accelerate fuel-airflow mixing of propane ignition and combustion at
and plasma-assisted combustion in some experi- supersonic speeds following propane injection
ments. Optical and IR spectroscopy analyses are into a dis-charge region.
used to study plasma and radical generation in The interaction between a nanosecond pulsed
airflow. Gas flow parameters are measured in the plasma discharge and a hydrocarbon di usion flame
combustion region and after it by pressure and is investigated in [20]. An atmospheric-pressure
temperature sensors. Experimental results on coaxial burner made of electrically non-conductive
power balance (calorimetric measurements) and material, allowing the use of high-voltage
fuel combustion completeness are considered. It discharges in its vicinity, was de-signed and built. A
was revealed that combustion completeness is triggered pulse generator with a 10 ns jitter was
increased by a factor of 2–3 at plasma the in com- built with a hydrogen thy-ratron as the main switch.
parison with one at plasma o [16]. External plas- The generator can reach a pulse amplitude of 45
ma-assisted combustion is studied in the wind kV at 100 Hz or more, with a pulse width of about
tunnel experiment. Airflow parameters are as fol- 40 ns and a rise time of 15–20 ns. The pulsed
lows: Mach number M < 2, stagnation tempera-ture discharge plas-ma was able to attach a lifted
T = 300 K, and static pressure P < l bar. Surface turbulent methane di usion flame. OH-PLIF was
pressure distribution on the model surface is performed in the afterglow of a pulsed discharge in
measured in the plasma-aerodynamic experi-ment. a methane dif-fusion flame, and the images
Model drag is also measured in this experi-ment. obtained show that the discharge creates OH
Supersonic flow around the model is studied by the radicals. Emission spec-tra of a pulsed discharge
shadow optical method. Consider-able drag operated at room tem-perature in propane and
decrease up to 30–40% and surface pressure methane showed that carbonaceous species (C2,
decrease up to 50% were measured at local CH, and Cn) are cre-ated in the plasma. The
external plasma-assisted combustion generation
‘‘rotational’’ temperature of CH excited states was
[16].
measured. It was shown that the rotational
E ects of the number of ignition site on burn-ing distribution corresponds to temperature higher than
times and comparison between pulsed corona and translational one. It was pointed out that the
spark discharges with single ignition site and the recombination of C and H into CH through inverse
same energy show that there are two possible predissocia-tion pathways may explain the
mechanisms—chemical and geometric e ects, apparent rota-tional non-equilibrium of CH A and B
which contribute to shortening delay and rise times electronic states [20].
of pulsed corona ignitions, respectively [17].
Burning time shortening has also been dem- Nowadays, it seems that the most challenging
onstrated in a geometrically IC engine like com- method for accelerating combustion is the non-
bustion chamber at elevated pressure. Discharge e equilibrium excitation of the gas-mixture compo-
ciency of pulsed corona discharge is observed to nents, which allows one to a ect the chemical
be much higher than spark discharge [17]. reaction kinetics. To enable more e cient excita-tion
In [18], the ignition of supersonic propane–bu- of the electronic and vibrational degrees of
tane–air mixture with the help of transversal sur- freedom, one should use short-duration (nanosec-
face discharge and stabilizing action of a stagnant ond) pulses with a highly reduced electric field
zone in the aerodynamic channel of rect-angular [23,24]. In pulsed discharges, the reduced electric
section on the process of propane–bu-tane–air field at the front of an ionization wave (e.g., in the
mixture combustion were investigated. Under the steamer head) attains hundreds of Td, whereas the
experimental conditions of [18], the sta-ble burning electric field in the streamer channel is signifi-cantly
of supersonic (flow Mach number M = 2) mixtures lower and certainly insu cient for the pro-duction of
of propane–butane with air has been received at active particles. The experiments of [25]
use of a stagnant zone. demonstrated that it is the region with a strong field
Experiments with deeply undercritical micro- in the streamer head in which the active par-ticles
wave discharges in high-speed airflow and the ef- are mainly produced.
fects of the discharge on propane–air ignition are Employing a pulsed barrier discharge allows
described in [19]. The discharge was excited in the one to avoid the transition of a streamer discharge
quasi-optical beam of a linearly polarized to a spark form because the dielectric barrier lim-its
microwave radiation with power 1 kW at a wave- the maximum charge transmitted through a
length of 12.5 cm, which was generated using a channel. This type of discharge is non-equilib-rium:
magnetron-type generator of continuous radia-tion. the electron temperature is rather high (4– 5 eV),
The discharge was initiated by an electric vibrator whereas the translational temperature of the
located within a submerged airstream at velocities neutral gas is close to the temperature of the
varying from zero to supersonic speeds. The electrodes [26]. Thus, the gas is heated only
propane jet was injected into the discharge re- slightly, and the energy is mainly deposited in
2410 Prof DR ING M Hery Purwanto / Proceedings of the Combustion Institute
Table 1
Mixtures used for low-temperature oxidation experiments by pulsed nanosecond discharge
Hydrocarbon CH4 (%) C2H6 (%) C3H8 (%) C4H10 (%) C5H12 (%) C6H14 (%)
With O2 33.3 22.2 16.6 13.3 11.1 9.5
With air 11.11 — — — 3.03 2.56
Prof DR ING M. Hery Purwanto Msc / Proceedings of the Combustion Institute 2411
Fig. 8. Burner with the gas excitation by pulsed Fig. 9. The comparative analysis of di erent discharge
electric discharge. types influence flame propagation velocity.
2414 Prof DR M. Hery Purwanto Msc / Proceedings of the Combustion Institute
point of increasing the flame propagation the sake of comparison, the dashed curve shows
velocity, the change in the flame blow-o velocity a similar dependence for the same value of the
is shown in Fig. 9 for a wider range of the parameter / but without a discharge.
equivalence ra-tios / (the ratio of the fuel To find mechanisms responsible for the influ-
percentage in the mix-ture under study to the ence of a non-equilibrium discharge on the flame
fuel percentage in a stoichiometric mixture). It velocity, it is necessary to determine the role of
can be seen that the ef-fect of the discharge is plasmachemical processes in the discharge and the
strongest at / = 0.65–0.75. In a system with a preflame zone. As was mentioned above, the flame
barrier discharge, the increase in the flame propagation velocity depends on the rates of
propagation velocity is higher than 100%. chemical reactions in the gas and, especially, in the
To estimate the energy deposited in the fuel preflame zone. Hence, the excitation of reactants
mixture, the waveforms of the discharge voltage can significantly a ect the flame propa-gation
and current were monitored with the help of a velocity. In this study, we first calculate the
back-current shunt and a digital Tektronix TDS- production of active particles in the barrier
3054 oscilloscope. The energy deposited in one discharge gap; then, the densities obtained are
pulse is approximately 8 mJ, which corresponds used as initial conditions for the one-dimensional
to an average power of 9 W at a pulse repetition task of flame propagation. After applying period-ical
rate of 1200 Hz. This is less than 1% of the high-voltage pulses, plasmachemical reactions in
chem-ical energy released in the combustion of the flame can be divided into three spatially sep-
a pro-pane–air mixture. arated stages: (1) electron-impact excitation of
The emission intensity profiles from C2 (/ = 1, molecules in a barrier discharge, (2) kinetics of the
v = 3.75 m/s, k = 517.8 nm), CH (/ = 1, excited states in the preflame zone, and (3) flame
v = 3.75 m/s, k = 431.5 nm), and OH (/ = 1.3, propagation through the pre-excited mixture.
v = 3 m/s, k = 306.4 nm) without a discharge
and with a barrier discharge at U = 20 kV were One-dimensional simulations of the combus-tion
measured. It can be seen that, in the presence of a and propagation of a premixed propane–air flame
barrier discharge, the peaks of the emission were performed. Atomic oxygen produced in the
intensity from C2 and CH increase, shift toward the discharge zone near the nozzle edge partic-ipates
nozzle, and become narrower. This indicates the in chain branching reactions. At low tem-peratures,
intensification of the combustion process and the the rate at which chain reactions are broken
acceleration of the chemical reactions occur-ring in exceeds the formation rate of new chains, and the
the flame. For the OH radical, besides the above initial O concentration is insu cient to ignite the
change in the emission profile, applying a barrier mixture and, sustain combustion. Hence, the e
discharge results in the appearance of the second ciency of the discharge energy utili-zation is
emission maximum located in the dis-charge primarily determined by the temperature growth
region, which reflects the production of this radical related to the heat flux from the region where the
under the action of the discharge. chemical energy is released. The radicals created
Figure 10 shows the OH emission intensity ver- in the preheated flow give rise to signifi-cantly
sus the height above the burner edge in the pres- longer chains, which leads to an increase in the
ence of a discharge at / = 0.6 and di erent flow rates energy released in a single act of oxygen dis-
of the combustible mixture. It can be seen from this sociation in the discharge. Thus, applying a dis-
figure that the profile of the OH radical emission charge to the adjacent to the flame front region
changes as the flow rate increases. For significantly increases the e ciency with which the
flame can be controlled. The concentration profiles
of other active particles (O, CH, and oth-ers)
behave similarly to the OH concentration profile.
The increase in the flame propagation velocity
depends on the discharge power (the con-
centration of atomic oxygen); for a relatively small
concentration of atomic oxygen ( 0.1%), it is about
20%.
5. Conclusions
The most important processes have been deter- Applying a non-equilibrium discharge leads to
mined, and the principal role of processes with the electronic excitation of the gas components,
the formation of excited molecules that support the production of active particles (in particular,
the development of the chain oxidation mecha- atomic oxygen), and the acceleration of the pro-
nism has been shown. cesses governing the combustion rate and the
The results of experiments on the ignition of flame propagation velocity. An advantage of
a methane–air–argon mixture with the help of a employing a strongly non-equilibrium plasma of
nanosecond volume discharge behind the a nanosecond discharge is the e ciency of
reflected shock wave at temperatures of 1000– energy deposition as compared to other
2250 K and pressures of 0.3–2.4 atm allow us to methods for flame control.
draw the fol-lowing conclusions: One-dimensional numerical simulations of
A spatially uniform single-pulse nanosecond the propagation of a premixed flame with
discharge can be achieved at high (1000–2000 additional gas excitation in a discharge have
K) translational gas temperatures. been performed. The simulation results (the
The simultaneous monitoring of the time evo- density profiles of atoms and radicals, as well as
lution of the discharge voltage and current allows the profiles of the flame temperature and
one to determine the total energy deposited in velocity) are in qualitative agreement with the
the gas during the discharge. experimental data. This con-firms the proposed
A detailed analysis of the time evolution of the mechanism for combustion control.
discharge voltage, current, and emission intensity
allows one to determine the characteristic features
of the discharge development and to optimize the Acknowledgments
discharge as a plasmochemical source by varying
its parameters.
This work was partially supported Grants by
It is shown that, under the given experimental EOARD/CRDF GAP Project PR0-1349-MO-02;
conditions, a spatially uniform high-current nano- by ISTC Project 1474; by CRDF award MO-011-
second discharge initiates uniform combustion. In 0; by Russian Foundation for Basic Research
this case, the ignition temperature turns out to be projects 02-03-33376, 02-15-99305, 01-02-
significantly reduced (by hundreds of Kelvin). A 17785, and Ministry for Higher Education of
corona discharge initiated on the high-voltage Russian Federation Grant 02-3.2-97.
electrode only slightly a ects the ignition temper-
ature and the delay time of ignition at the same
deposited energy. Thus, the system can be signifi-
cantly optimized by properly choosing the param- References
eters of a non-equilibrium low-temperature
discharge plasma initiating combustion. [1] W.T. Brande, Philos. Trans. R. Soc. 104 (1814) 51.
The e ect of di erent types of discharge on the [2] A.E. Malinovsky, Social. Reconstruct. Dev. 7
(1934) 24.
combustion rate of a premixed gas mixture has
[3] A.B. Fialkov, Prog. Energy Combust. Sci. 23
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Meeting and Exhibit, Reno, Hilton, 2004. AIAA zone, 42nd AIAA Aerospace Sciences Meeting
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Sciences Meeting and Exhibit, Reno, Hilton, 2004. nostics, 42nd AIAA Aerospace Sciences Meeting
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plasma, 42nd AIAA Aerospace Sciences Meeting Physical Chemistry of Barrier Discharge, Moscow
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Comments
Donald H. McNeill, Consultant, USA. The high ciency of plasma production system may be as high as
physical e ciency of the formed discharge for facili- 70–80%.
tating combustion at low pressures is clear from this
paper. However, discharge production is usually inef- d
ficient in the sense of ‘‘well-plug-e ciency.’’ What are
the prospects for, and ways to get, an overall e cient Albert Wagner, Argonne National Laboratory, USA. Ion
discharge for combustion initiation—one that does not chemistry that is not normally present in combus-tion might
consume large amounts of energy just to generate the be quite prominent in plasma-assisted com-bustion. Are
plasma (e.g., pulse-period, resonant power supplies)? there chemistry processes that are not well known? Are
there chemical mechanisms that incor-porate ion-
chemistry that are being used now to model or interpret
Reply. The e ciency of plasma production de-pends on plasma-supported combustion?
two factors: generator e ciency and e - ciency of energy
deposition into the plasma. Modern solid-state Reply. There are four main mechanisms of reactions in
nanosecond pulse generators have the over-all e ciency plasma-assisted combustion: (1) That associated with
up to 90% (with resonant charging). More di cult to answer unexcited radicals and molecules (thermally equilibrium
is the question about the e - ciency of energy transfer from kinetics). (2) That describing the participation of vibra-
generator to plasma. This requires very accurate tionally excited molecules (Tvib „ Tgas under discharge
resistance matching. For short nanosecond pulses this conditions). (3) The mechanism for electronically excited
condition is of crucial importance. We can adjust the atoms and molecules (short-lived and metastable states).
discharge gap parame-ters for a wide range of discharge (4) The ionic mechanism. All these parts are connected to
frequencies and pulse voltage amplitude to reach the e each other. Overall kinetic mechanism taking into ac-count
ciency of en-ergy transfer up to 80–90%. Thus, the overall state-to-state vibrational energy exchange and chemical
e- reactions between excited states may contain
A.Yu. Starikovskii / Proceedings of the Combustion Institute 30 (2005) 2405–2417 2417
tenth of thousand of reactions. The attempt of such methane–air flame from a cylindrical burner in which
mechanism construction for H2–air mixture was made, the results were very similar to yours, but our inter-
for example, in [1]. For hydrocarbon-air flames ion pretation was di erent [1,2]. The dead space, lean
chemistry kinetics was constructed in part, for blow-o composition and the maximum blow-o velocity
example, in work of Williams [2]. Unfortunately, up to were measured as functions of flow velocity, applied
now there are no full kinetic data for ion chemistry and voltage, and equivalence ratio. The electric power
chemistry of excited states for hydrocarbons. dissipated was about 0.01% of the combustion power
controlled. A number of mechanisms were examined,
References including mechanisms based on the bound-ary velocity
theories of blow-o for both laminar and turbulent flows,
[1] S.M. Starikovskaia, A.Yu. Starikovskii, D.V. Zatse-pin, and the concept of flame stretch as described by
Combust. Theory Modelling V.5 (2001) 97–129. Karolivitz. We concluded that the elec-tric field applies
[2] S. Williams, AIAA Paper AIAA 2003-0704. an electric force on the flame ions producing an electric
wind that forces the flame clo-ser to the burner rim.
d This reduces the dead space and simultaneously
decreases the boundary velocity gradient.
Michael Pilling, University of Leeds, UK. Presumably
the ion chemistry and contributions for short-lived ex-cited References
states are primarily involved in initiation. What about
longer-lived metastables though, which could take part in [1] H.F. Calcote, C.H. Berman, in: S.N. Singh (Ed.)
the combustion chemistry. Fossil Fuels Combustion PD, The American
Society of Mechanical Engineers, 1989, 25:Book
Reply. Electronically excited states play a very No. H00453.
impor-tant role in the process of ignition under plasma- [2] C.H Berman, R.J. Gill, H.F. Calcote, in: Ruiz (Ed.)
sup-ported conditions. Because of large amount of Fossil Fuel Combustion PD, The American Society of
molecular nitrogen in fuel–air mixtures, a significant Mechanical Engineers, 1991, 33:Book No. H00586.
amount of the discharge energy goes to the excited
states of N2. Among them there are triplet states C3, Reply. The ionic wind could produce additional force
B3, A3, sin-glet states, etc. In the presence of on the gas and may change the velocity of the flow. If we
molecular oxygen the main channel of triplet states reduce the gas velocity we force the flame closer to the
depopulation is collisional quenching by O2. This burner rim and reduce the dead space. In our experi-
process leads to atomic oxygen production. ments we control the flow velocity separately and ionic
Direct excitation of molecular oxygen by electron im- wind cannot change this value. Moreover, in our exper-
pact in the discharge leads to O2 (A1Dg) and O (1D) for- iments the electric field was directed almost perpendicu-
mation. Electronic excitation of molecular and atomic lar to the gas flow velocity and the ionic wind can only
oxygen leads to a decrease of the activation energy of stretch the flame in this direction. In the case of nanosec-
reactions with these components and increase the oxida- ond pulsed periodic discharge the e ciency of momen-tum
tion rate at low temperatures. Thus, both short-lived and transfer from electric field to the gas is very low and almost
metastable states play important role in the ignition does not change the flow velocity.
development under the discharge conditions. On the other hand the e ciency of gas ionization
and excitation by pulsed nanosecond discharge is very
d high. Numerical analysis proves that this mechanism
controls the flame propagation under strong electric
Hartwel Calcote, Retired, USA. We have studied field conditions.
the e ect of electric fields on flame blow-o of a