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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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%


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%


-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%


-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%


0 20 40 60 80 100 120 140 160 180

20000

30000

40000

50000

Inte

nsity

Pixel#

Median = 44250

Maximum = 50000

Energy Error = 13%


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%


-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%


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


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


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)

fundamental mechanisms, predictive modeling, and novel

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