Fundamental Mechanisms, Predictive Modeling, and Novel ...
Transcript of Fundamental Mechanisms, Predictive Modeling, and Novel ...
Fundamental Mechanisms, Predictive Modeling,
and Novel Aerospace Applications of Plasma Assisted Combustion
AFOSR
MURI Review Meeting
Andrey Starikovskiy Princeton University
October 22, 2013
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4. TITLE AND SUBTITLE Fundamental Mechanisms, Predictive Modeling, and Novel AerospaceApplications of Plasma Assisted Combustion
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Standard Form 298 (Rev. 8-98) Prescribed by ANSI Std Z39-18
Main Tasks
• High Temperature
• High Pressure
• High Speed
• High Voltage
• High Power
3000K
1000K
300K
0.01atm 1atm 100atm
Flames
(Ju, Sutton)
Flow Reactors
(Yetter,
Adamovich)
Shock Tube
(Starikovskiy)
RCM
(Starikovskiy)
MW+laser
(Miles)
JSR
(Ju) Streamer
(Adamovich)
Rapid Compression Machine: P = 10-70 atm, T = 650-1200 K
Driving chamber
Speedcontrol
chamber
Combustionchamber
Oil reservoirPiston lock chamber
g
N2
Fast active valve
P=30 bar of N2
P=1 bar
Solenoid
Piston
Oil
Scheme of the RCM
Gas Dynamic Limitations
0
5
10
15
20
25
30
0 30 60 90 120 150 180
Time (ms)
Pre
ssure
(bar)
13mm, 958 K,19.77 bar
9mm, 967 K, 20.87 bar
Gas Discharge Limitations
ICCD images of the
discharge at 1 atm dry air.
Negative polarity of the high-
voltage electrode, 22 kV, 25
ns duration, f = 40 Hz
[Kosarev et al, 2009].
Mixture C2H6:O2=2:7 at 1 bar
and ambient initial
temperature was
successfully ignited in ~100
ms in relatively large volume
[Sagulenko et al, 2009].
SDBD Development at High Pressures 1 atm 4 atm
10 kV
30 kV
1 atm, 10 kV
3 atm, 30 kV
DBD Discharges: 20 kV, 10kHz ICCD gate 50 ns
Side view: T0=500 K, ϕ=0.3 Side view: T0=300 K, ϕ=0.0, pulse#10
Front view: T0=500 K, ϕ=0.3 Front view: T0=300 K, ϕ=0.0
200 Torr
DBD Discharges: 20 kV, 10kHz ICCD gate 50 ns. P = 20 Torr
#5 #20 #50 #100 #200
Contraction
stage Gasdynamic
expansion stage
#5 #20 #50 #100 #200
Contraction
stage Gasdynamic
expansion stage
Air
Nitrogen
Energy distribution profiles.
Dynamic discharge contraction
and gasdynamic expansion
stages are clearly seen.
tinst ~ tT/gi ~ 0.1 tT gi = (d ln(ni))/(d ln(E/N))
tT ~ g/(g -1) p[Pa]/‹W› - typical heating time tinst ~ 10-4 – 10-2 s
Kinetic Analysis. Konnov’s Chemical Mechanism, T0 = 500K, P = 50 Torr
C2H6-Air. E/n = 300 Td, Different discharge energy.
Even 25% inhomogeneity will lead to order of magnitude difference in
ignition delay – and completely compromise the kinetic analysis.
Kinetic Error Analysis
-20 0 20 40 60 80 100 120 140 160 180
0
10000
20000
30000
40000
50000
60000
Inte
nsity
Pixel#
Median = 43250
Maximum = 54500
Energy Error = 26%
Ignition Error ~ 5 times
-20 0 20 40 60 80 100 120 140 160 180
-10000
0
10000
20000
30000
40000
50000
60000
Inte
nsity
Pixel#
Median = 24250
Maximum = 51250
Energy Error = 111%
Ignition Error ~ 20 times
0 20 40 60 80 100 120 140 160 180
0
10000
20000
30000
40000
50000
60000
70000
Inte
nsity
Pixel#
Median = 41250
Maximum = 61000
Energy Error = 48%
Ignition Error ~ 10 times
-20 0 20 40 60 80 100 120 140 160 180
10000
20000
30000
40000
50000
Inte
nsity
Pixel#
Median = 42500
Maximum = 48750
Energy Error = 15%
Ignition Error ~ 2.5 times
0 20 40 60 80 100 120 140 160 180
10000
20000
30000
40000
50000
60000
Inte
nsity
Pixel#
Median = 42375
Maximum = 52750
Energy Error = 25%
Ignition Error ~ 5 times
-20 0 20 40 60 80 100 120 140 160 180
20000
30000
40000
50000
Inte
nsity
Pixel#
Median = 42500
Maximum = 50000
Energy Error = 18%
Ignition Error ~ 3 times
0 20 40 60 80 100 120 140 160 180
20000
30000
40000
50000
Inte
nsity
Pixel#
Median = 44250
Maximum = 50000
Energy Error = 13%
Ignition Error ~ 2 times
0 20 40 60 80 100 120 140 160 180
0
10000
20000
30000
40000
50000
60000
Inte
nsity
Pixel#
Median = 32250
Maximum = 51750
Energy Error = 60%
Ignition Error ~ 12 times
-20 0 20 40 60 80 100 120 140 160 180
10000
20000
30000
40000
50000
Inte
nsity
Pixel#
Median = 42750
Maximum = 51250
Energy Error = 20%
Ignition Error ~ 3 times
Air C2H4-Air H2-Air
Inhomogeneous
Homogeneous?
Ignition of a stoichiometric
hydrogen-air mixture
modeling. OSU, 2009
Plasma-Assisted Ignition at High Pressures
CH4 + O CH3 + OH CH3 + OH CH2O+H2
CH3 + O2 CH2O + OH CH3 + O2 +M CH3O2 + M
T2 = 672 K, P2 = 20 bar. T2 = 794 K, P2 = 32 bar
Ignition delay time for
modified mixtures, f=1.0,
EGR=30%. Discharge 20ms
before compression stroke
Kinetics of Ignition Development
Stage 1. Discharge in
Methane‐Air mixture at
temperature ~ 330 K, 1 atm.
Production of metastable
components.
Stage 2. Fast adiabatic
compression to a
temperature of 800‐950 K.
Metastable components
decomposition and ignition
development.
alkylperoxy radicals!
CH2O CO CH3OH CH3O2H H2O2 Delay
Time
Sensitivity
0 0 0 0 0 1.00
540ppm 170 ppm 260 ppm 21 ppm 49 ppm 0.33
540 ppm 0.51 910
170 ppm 1.00 0
260 ppm 0.89 423
21 ppm 0.60 19,050 49 ppm 0.47 10,820
Non-diffusive hybrid scheme
for simulation of filamentary
discharges
AVALANCHE TO STREAMER TRANSITION IN UNIFORM ELECTRIC FIELD
(air, 1 bar, 300 K, 1 cm, various voltages)
AVALANCHE TO STREAMER TRANSITION IN UNIFORM ELECTRIC FIELD
(air, 1 bar, 300 K, 1 cm, various E/n)
PS High-Pressure Discharge E/n = 200 Td: tmax(r0) ~ 10 ns
E/n = 300 Td: tmax(r0) ~ 2 ns
r1 ~ 21r0 (P1 = 70 atm) tmax(200 Td) ~ 500 ps
tmax(300 Td) ~ 100 ps
FPG 200-01PB pulse generator
Voltage up to 200 kV
Pulse duration 350 ps
Rise time 120-140 ps
Voltage rise rate 2×1015 V/s
Air, 1 atm
Water, 1 g/cm3
Tstatic
1300K
800K
300K
1m/s 100m/s 1000m/s
Flames
(Ju, Sutton)
Cavity Flow Ignition
(Adamovich)
Shock Tunnel
(Starikovskiy)
10m/s
Discharge Formation and Flame Stabilization in High Speed Flow – Plasma Shock Tunnel
Combustion-Driven Shock Tube Vacuum Chamber 1x0.5x0.5 m3
NOZZLE
Pulser
Discharge Formation and Flame Stabilization in High Speed Flow – Plasma Shock Tunnel
Combustion-Driven Shock Tube Nozzle Pulser
100 kV, 1 MHz
12 ns, 1000 p/b
1 MHz, 50 kV, 1 ms
1 MHz, 100 kV, 1 ms
3000K
1000K
300K
0.01atm 1atm 100atm
Flames
(Ju, Sutton)
Flow Reactors
(Yetter,
Adamovich)
Shock Tube
(Starikovskiy)
RCM
(Starikovskiy)
MW+laser
(Miles)
JSR
(Ju) Streamer
(Adamovich)
PAC Kinetics at High T, Low P
Plasma Shock Tube
Plasma Shock Tube
Plasma Shock Tube
TDS-2014
Tek-370
BNC-575
431 nm
CH
MDR12 +R6357
MDR12 +R6357
306 nm
OH
TDS-2014
TDS-3054
FID 120/60
HV PS HV PS
Pulse Current Dynamics – Cable C2H6:O2:N2:Ar = 2:7:28:63
P5 = 3.3 atm
T5 = 1360 K
r5 = 1.06 kg/m3
P5 = 1.0 atm
T5 = 1610 K
r5 = 0.273 kg/m3
Pulse Current Dynamics – Shock Tube C2H6:O2:N2:Ar = 2:7:28:63
Ethane. Hayashi 1987
Argon. Tachibana 1989
Oxygen. Ionin 2007
N2. Phelps 1994
( )( ) { [ ]} ( ) ( )
nf
t
Ze
m c vnf nf S nf v E v H1
0
10 cos)()(cos)(),(l
ll vfvfPvfvf ne/nm « 1
Discharge Energy Comparison C2H6:O2:N2:Ar = 2:7:28:63
Discharge Dynamics
Ignition Delay Time C2H6:O2:N2:Ar = 2:7:28:63
0.5 0.6 0.7 0.8 0.9
10
100
1000
10000
Thermo, P ~ 3 atm
Thermo+Corona, P ~ 3 atm
pt,
s*a
tm
1000/T, K-1
Combustion model: Konnov (2005)
Ignition Delay Time C2H6:O2:N2:Ar = 2:7:28:63
Combustion model: Konnov (2005)
Measured Ignition Delay Time in Stoichiometric
С2Н6:О2:Ar and С2Н2:О2:Ar Mixtures
0.3 0.4 0.5 0.6 0.7 0.8 0.910
0
101
102
103
Ign
itio
n t
ime
, s
1000/T
C2H
2, auto
C2H
2, PAI
C2H
6, auto
C2H
6, PAI
С2Н6:О2:Ar
Kosarev et al. (2009)
С2Н2:О2:Ar
current work
Peak Reduced Electric Field and Field at the Instant of Peak Current
С2Н2:О2:Ar =
17:83:900
(φ = 0.5)
Total Specific Deposited Discharge Energy and Energy Deposited in First Pulse
С2Н2:О2:Ar =
17:83:900
(φ = 0.5)
Ignition delay time in С2Н2:О2:Ar mixtures
φ = 1
0.5 0.6 0.7 0.8 0.910
1
102
103
PAIauto
Tim
e,
s
1000/T
0.5 0.6 0.7 0.8 0.9
101
102
103
PAIauto
Tim
e,
s
1000/T
φ = 0.5
solid symbols: measurements
hollow symbols: calculations with kinetic scheme
by Wang et al. (2007)
Evolution in time of calculated mole fractions for main components
Ignition after discharge at
1130 K and 0.91 atm
102
103
10-4
10-3
10-2
10-1
H2
C2H
4
CH3
HCCO
CH2CO
H2C
4O
C4H
2
OHOH
C2H
2
H2O
CO
CO2
O2
Mo
le f
racti
on
Time, s
10-1
100
101
102
103
10-4
10-3
10-2
10-1
HO2
OH
H
O HCCO
CH3
C2H
4CH2COH
2C
4O
H2
C4H
2
H2O
CO2
COC
2H
2
O2
Mo
le f
racti
on
Time, s
Stoichiometric С2Н2:О2:Ar mixture
Autoignition
at 1115 K and 0.91 atm
Sensitivity analysis for autoignition and ignition by discharge
-0,4 -0,3 -0,2 -0,1 0,0 0,1 0,2
(ti-t
0)/(t
0)
Auto
FIW
H+O2=O+OH
HCO+O2=CO+HO
2
C2H+O
2=HCO+CO
HCCO+H=CH2*+CO
C2H
3(+M)=C
2H
2+H(+M)
C2H
2+O=HCCO+H
C2H
3+O
2=CH
2CHO+O
C2H
3+O
2=HCO+CH
2O
C4H
2+H=iC
4H
3
C4H
2+OH=H
2C
4O+H
Autoignition
1115 K and 0.91 atm
Ignition by discharge
1130 K and 0.91 atm
Stoichiometric
С2Н2:О2:Ar mixture
Ignition Delay Time, f = 0.5
0.65 0.70 0.75 0.80 0.85
0.1
1
10
100
C2H
5OH:O
2:Ar(90%)
Ign
itio
n t
ime,
s
1000/T5
exp, PAI, fi=0.5
calc, PAI, fi=0.5
exp, auto, fi=0.5
calc, auto, fi=0.5
0.65 0.70 0.75 0.80 0.85
1
10
100
1000
C2H
5OH:O
2:Ar(90%)
Ign
itio
n t
ime,
s
1000/T5
exp, PAI, fi=1
calc, PAI, fi=1
exp, auto, fi=1
calc, auto, fi=1
Ignition Delay Time, f = 1.0
Plasma Shock Tube Experiments Summary С2Н2:О2:Ar(90%)
0.5 0.6 0.7 0.8 0.9 1.010
100
1000
PAIauto
Tim
e,
s
1000/T, K-1
φ = 0.5
Combustion model: Wang et al. (2007)
C2H5OH:O2:Ar(90%) Combustion model: MARINOV (1998)
C2H6:Air:Ar(63%) Combustion model: Konnov (2005)
0.5 0.6 0.7 0.8 0.9
10
100
1000
10000
Thermo, P ~ 3 atm
Thermo+Corona, P ~ 3 atm
pt,
s*a
tm
1000/T, K-1
Combustion model: Konnov (2005)
C2H6:Air:Ar(63%)
Ignition Delay Time Decrease at 0.1 eV/mol
0.68 0.72 0.76 0.80 0.84
1
10
100
1000
Exp, f = 1.0
Calc, f = 1.0
Exp, f = 0.5
Calc, f = 0.5
t au
to/t
pla
sm
a
1000/T, K-1
tp = ta exp(-Ep/E0)
C2H5OH:O2:Ar(90%)
Plasma Ignition Sensitivity 0.1 eV/mol
0.6 0.7 0.8 0.9 1.0 1.1 1.2
100
101
102
103
104
105
106
107
108
Plasma assisted
ignition efficiency
Q = 0.1 eV/mol
H2:Air
CH4:O2:Ar
CH4:Air:Ar
C2H2:O2:Ar
C2H5OH:O2:Ar
C2H6:O2:Ar
C2H6:Air:Ar
C3H8:O2:Ar
C4H10:O2:Ar
C5H12:O2:Ar
Se
nsitiv
ity
t au
to/t
pla
sm
a
1000/T, K-1
H2-Air PAI
ta/tp ~ 8
e ~ 0.0125 eV/mol
ta/t0.01 ~ 5 (- 40%)
ta/t0.10 ~ 2×107
PAC Kinetics H2 Model Development Plasma model: • Plasma assisted combustion models for hydrogen oxidation understood for conditions of low energy
loading per molecule. It means low ionization degree – we can neglect e-e collisions and EEDF Maxwellization due to this process.
• We have complete set of cross-sections for rotational, vibrational and electronic excitation, dissociation, dissociative ionization, ionization. These cross-sections were verified both for two-term approximation of Boltzmann equation (local EEDF) and could be modified for non-local case of extremely strong electric fields (differential cross-sections are also available).
Afterglow Model:
• Because of fast relaxation we assume Ttr = Trot for ground state. • We have recombination rates for ion-electron collisions, ion-ion recombination (in some cases the
products are unknown). Rates of complex ions formation/decomposition are unknown for elevated temperatures – but these ions control the plasma recombination rate.
• Quenching rates of major states are available, in some cases products are unknown. Specifically we do not know the products of reactions N2* + H2 -> …
Chemical Model: • We have complete state-to-state model of chemical reactions including vibrationally-nonequilibrium
conditions for H2-air system since 2001. • We have verified this model for 300 K (low-P reactor), 300-800 K (1 atm streamer) and 800-1500
K (0.5 atm, reflected shock wave). Unsolved problems: • Because of huge number of reactions some pathways are still questionable. We need to investigate in
more details the products of electron-ion and ion-ion recombination, products of electronic states dissociative quenching (focus on electronically-excited products formation).
• Reaction rate coefficients of electronically and vibrationally excited species should be verified in some cases.
• We need additional analysis of the role of complex ions in recombination and chemistry at low-T conditions.
Plasma Assisted Combustion: Translational Nonequilibrium
1 10 100 10001E-3
0,01
0,1
1
H2(rot)
O2(4.5 eV)
O2(dis)
H2(el)
Rot+tr
O2(a+b)
O2(v)
H2(v)
ion
N2(el)
N2(v)
N2:O
2:H
2 = 4:1:2
En
erg
y lo
ss f
racti
on
E/N, Td
100 1000
10
20
30
40
50
60
Popov (2011)
Pancheshnyi (2009)
Popov (2001)
p=20 Tor
p=760 TorAleksandrov&Starikovskiy, 2010
B ne0
=1014
, p=20 Tor
C ne0
=1015
, p=20 Tor
D ne0
=1014
, p=1 atm
E ne0
=1015
, p=1 atm
%
E/N, Td
Mechanism of Fast Heating in Air Plasma
Potential Energy Curves of Molecular Hydrogen
r, nm
E,
eV
H2(b3Su), 8.9 eV
smax = 0.33 A2 (17 eV)
H2(a3Sg), 11.8 eV
smax = 0.12 A2 (15 eV)
H2(B1Su), 11.3 eV
smax = 0.48 A2 (40 eV)
H2(C1Pu), 12.4 eV
smax = 0.40 A2 (40 eV)
DE = 4.5-12.5 eV t = 10.5 ns
Potential Energy Curves of Molecular Oxygen
r, nm
E,
eV
O2(A3Su
+), 4.5 eV
smax = 0.18 A2 (6.6 eV)
O2(3Pg), 5.6 eV
smax = 0.16 A2 (12 eV)
O2(B3Su
-), 8.4 eV
smax = 1.0 A2 (9.4 eV)
DE ~ 1.5 eV
DE ~ 1 eV
Potential Energy Curves of Molecular Nitrogen
r, nm
E,
eV
N2(A3Su
+), 6.2 eV
smax = 0.08 A2 (10 eV)
N2(B3Pg), 7.35 eV
smax = 0.20 A2 (12 eV)
N2(C3Pu), 11.03 eV
smax = 0.98 A2 (14 eV)
Major Channels of Hot Atoms Production
N2 + e = N2(C3Pu) + e; k = f(E/n)
N2(C3Pu) + H2 = N2 + 2H(1S) + 6.55 eV; k = 3.2x10-10 cm3/s
N2(C3Pu) + O2 = N2 + 2O(3P,1D) + 3.9 eV; k = 2.7x10-10 cm3/s
O2 + e = e + 2O(3P,1D) + 1.3 eV; k = f(E/n)
H2 + e = e + 2H(1S) + 4.4 eV; k = f(E/n)
Chain Initiation/Branching Reactions
H + O2 = O + OH k = 1.6x10-10 x exp(-7470/T) cm3/s
k(300) = 2.5x10-21 cm3/s
k(hot) = 1.6x10-10 cm3/s
H + O2 + M = HO2 + M k(300, 1 atm) = 1.6x10-12 cm3/s Tcrit ~ Tautoignition
O + H2 = H + OH k = 8.5x10-20 x T2.67 x exp(-3160/T) cm3/s
k(300) = 9.3x10-18 cm3/s
k(hot) = 1.5x10-10 cm3/s
k(1D) = 1.1x10-10 cm3/s
O + O2 + M = O3 + M k(300, 1 atm) = 2.2x10-14 cm3/s Tcrit ~ 650K H(hot) + (N2,H2) = H + (N2,H2) k ~ 2m/M kgk ~ 1.6x10-10 cm3/s
O(hot) + (N2,O2) = O + (N2,O2) k ~ 2m/M kgk ~ 1.3x10-10 cm3/s
H(hot) + O2 = H + O + O
H(hot) + H2 = H + H + H
O(1D) + (M) = O + (M) k = 2.6x10-11 cm3/s (M = O2)
k = 1.3x10-11 cm3/s (M = N2)
k = 5.2x10-11 cm3/s (M = H2)
Radicals Production Increase in Cold H2-Air Mixture
Due to Hot Atoms Formation
SUMMARY - 1 Experimental Facilities
1. Rapid Compression Machine.
P = 10-70 atm, U = 120 kV
1 GW in 60 ns
1. Plasma Shock Tunnel. M = 3-5, U = 100 kV
0.5 MW during 1 ms
1. Plasma Shock Tube. T = 800 – 2000 K, U = 120 kV
SUMMARY - 2 Major Results
Two new mechanisms of PAC proposed:
1) Influence of Vibrational Excitation on Low-Temperature Kinetics
N2 + e = N2(C3) + e
N2(C3) + O2 = N2 + O + O
O2 + e = O + O + e
N2 + e = N2(v) + e
N2(v) + HO2 = N2 + HO2(v)
HO2(v) = O2 + H
Synergetic Effect of High and Low Electric Fields
2) Radicals Production Increase Due to Hot Atoms Formation
N2(C3Pu) + H2 = N2 + 2H(1S) + 6.55 eV
N2(C3Pu) + O2 = N2 + 2O(3P,1D) + 3.9 eV
O2 + e = e + 2O(3P,1D) + 1.3 eV
H2 + e = e + 2H(1S) + 4.4 eV
SUMMARY - 3 Major Results
Plasma Ignition Efficiency for Different Fuels Analyzed
0.6 0.7 0.8 0.9 1.0 1.1 1.2
100
101
102
103
104
105
106
107
108
Plasma assisted
ignition efficiency
Q = 0.1 eV/mol
H2:Air
CH4:O2:Ar
CH4:Air:Ar
C2H2:O2:Ar
C2H5OH:O2:Ar
C2H6:O2:Ar
C2H6:Air:Ar
C3H8:O2:Ar
C4H10:O2:Ar
C5H12:O2:Ar
Se
nsitiv
ity
t au
to/t
pla
sm
a
1000/T, K-1
Future Plans 1) Role of Translational and Vibrational Nonequilibrium
Analysis of non-Boltzmann,
non-Maxwell regimes of reactions
2) Reference Experiments Database for PAC
High-pressure regimes (RCM)
Low-pressure regimes (STube)
High-speed conditions (STunnel)
3) “Best Fuel for PAC”
Major International Collaborations and International Projects
Nickolay Aleksandrov (MIPT, Russia) Ilya Kosarev (MIPT, Russia) Sergey Pancheshnyi (ABB, Austria) Svetlana Starikovskaya (LPP, France) PROJECTS: PARTNER UNIVERSITY FUND “Physics and Chemistry of Plasma-Assisted Combustion” (Princeton-LPP) RUSSIAN FEDERAL PROGRAM “Plasma-Assisted Combustion Ultra-Lean Fuel-Air Mixtures for Energy Devices Efficiency Increase” (Princeton-MIPT)