recent advances in aluminium particles combustion · automotive manufacturers explore carbon-free...

Recent advances in aluminium particles combustion

UNIVERSITE D'ORLEANS

Fabien HALTER & Christian CHAUVEAU

Presentation of ICARE-CNRS in Orléans

ORLEANS

● Combustion and reactive systems

● Atmospheric reactivity

● Propulsion and high speed flows

Director : Philippe DAGAUT – Christian CHAUVEAU

45 permanent persons

30 additional persons


Outline1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator

- Electrostatic levitator

- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design

- Aerosol combustion

3. CONCLUSIONS

1. Introduction : Aluminum as a FUEL

2. Al COMBUSTION in industrial applications

2.1 PROPULSION

- Context

- Fluidic levitator


- Burning time decrease

- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

o Energetical potential of metalic fuels

o Metal fuels are safe for the storage (protection by naturally-formed metal oxide layer)

o Al & Mg are the third & sixth most plentiful element in the crust of the earth

Metals as fuels1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Characteristic temperatures of Al combustion

0,1 1500

1000

1500

2000

2500

3000

3500

4000

4500

5000

Fusion de Al

Vaporisation de Al

Fusion de Al2O

3

Flamme Al / O2

Flamme Al / CO2

Te

mp

éra

ture

(K

)

Pression (MPa)

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Isolated Particle Combustion

o The formed oxide size depends on the combustion mechanism.

Typically, for large Al (> 20 µm):

Vapor-phase, diffusion-controlled mechanism leads to nano oxide particles.

Decreasing Al particle size (∼ 10 µm) may modify the combustion regime.

• Damköhler number becomes close to 1.

• 𝐷𝑎 =𝜏𝑏,𝑑𝑖𝑓𝑓

𝜏𝑏,𝑘𝑖𝑛=

𝑑0𝑖 𝑚𝑂,∞ 𝑘𝑠

4𝐷 ln(1+𝑖 𝑚𝑂,∞)[1]

• Kinetic rates influence the burn time.

• Oxidizer diffusion towards the particle’s surface is possible.

• Thick reaction zone and possible heterogeneous reactions [2,3].

• Drop in flame temperature

[1] Glassman, I. and Yetter, R. A. (2008), Combustion, 4th edn, Academic Press.

[2] Bazyn, T. et al. (2007). Proceedings of the Combustion Institute, 31(2), 2021–2028.

[3] Glorian, J. et al. (2016). Combustion and Flame, 168, 378-392.

Al (l) Oxidizer

Nanometric oxide condensation

Heterogeneouscombustion

Gas-phase flame

Schematic of single Al particle combustion.

Oxide layer

Gas-phase combustion

Al2O3(s)

Nanometric oxide condensation

Micrometric oxide

HEAT

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Chemical reactions

Al

AlO

AlO2 Al2O

Al2O2

Al2O3


[1]

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Solid propulsion rocket

Two different times :

- Residence time

- Combustion time

Overview of a solid propulsion rocket

Part of the particles merge and form

agglomerates before the initiation of

combustion.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Literature review

[1] Lim J, Lee S, Yoon W. A comparative study of the ignition and burning characteristics of afterburning aluminum and magnesium particles. Journal of Mechanical Science and

Technology. 2014;28:4291-300.

[1]

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Fluidic levitator

CO2 Laser

HS CAMERA

Aluminum droplet

Pyrometer

Pyrometer

Silicon windowG

aseou

sm

ixtu

re

PT

T, PH2O

Sp

ectrom

eter

Optical fiber

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Typical solid fuel rocket composition

1 - IgnitionBreaking of the alumina shell

2 - Alumina lobe formationVaporization of AlDiffusion flame

3 - Al droplet regressionAlumina lobe regression

4 - Aerodynamic instability

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS Vincent SAROU-KANIAN, PhD Thesis, CNRS (2003)

Al droplet diameter evolution

0,0 0,5 1,0 1,5 2,0 2,5 3,0 3,50,0

0,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0

d 2 (

mm

2 )

d 3 (

mm

3 )

d (

mm

)

Temps (s)

0

5

10

15

20

25

30

35

40

45

50

0

2

4

6

8

10

12

14

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Al : Combustion rate

0 10 20 30 40 50 60 70 80 90 1000,5

1,0

1,5

2,0

2,5

3,0

3,5

4,0 H 2O pur

H 2O/O

2

H 2O/CO

2

H 2O/N

2

H 2O/CO

2/N

2

H 2O/Ar

Air

CO 2/N

2

Ta

ux d

e c

om

bu

stio

n

(m

m 2/s

)

Fraction molaire (%)

(autre que H2O)

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Alumina lobe regression rate

0 20 40 60 80 1000,0

0,1

0,2

0,3

0,4

0,5

0,6

K (

mm

2/s

)

Fraction molaire (%)

(autre que H 2O)

H 2O pur

H 2O/O

2

H 2O/CO

2

H 2O/N

2

H 2O/CO

2/N

2

H 2O/Ar

CO 2/N

2

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Potential scenarii

• Flow field effect

• Dissolution in the Al droplet

• Vaporization

1‰

xO ≈ 1-2%

Al(l) + Al2O3(l) → AlxOy(g)

PAlxOy = f(Tgoutte)

Al(l)

Al2O3(l)

Al2O3

AlAl+O

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Electrostatic levitator description

Top electrode

Bottom electrode

Ring electrode

0 - 4000 Vac

10 - 100 Hz

0 - 2000 Vdc

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Electrodynamic levitation set-up

Mirrors Beam splitter

CO2 Laser

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Combustion sequence (Al-Air / 0,1MPa)

6 8 10 12 14 16 180,0

0,2

0,4

0,6

0,8

1,0

Inte

ns

ité

lu

min

eu

se

no

rma

lisé

e

Temps (ms)

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Flame / Droplet evolution (Al-Air / 0,1MPa)

5 6 7 8 9 10 11 120

1

2

3

4

5

Dfl

am

me / D

part

icu

le

Temps (ms)

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Combustion Time (Al-Ar & Al-HCl / 0,1MPa)

0,0 0,2 0,4 0,6 0,8 1,00

2

4

6

8

10

12

14 53-63 µm

Ar

HCl

Limite O2-Ar

Limite O2-HCl

t Co

mb

usti

on (

ms)

Fraction molaire O2

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Burning time

𝑡𝑐∝𝐷𝑝𝑛

with 0,8 < 𝑛 < 2,5

With : 𝑃 ∶ Pressure𝑇0 : Initial Temperature𝑋𝑖 : Molar𝑎 and 𝑛 : Cte

𝑡𝑐 =𝑎 𝐷𝑝

𝑛

𝑋𝑒𝑓𝑓 𝑃0,1 𝑇0

0,2

[1] MW Beckstead. A summary of aluminum combustion. Technical report, DTIC Document, 2004

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Modification of the experimental set-up

Long distance microscope

HS Camera

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Combustion process

77 µm

t ~ 9,8 ms

1 : Heating

2 : Diffusion flame

3 : Spinning - Jetting

4 : Explosion

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

o First stage: the radiation trace is smooth and the particle flame is spherically symmetric

o Second stage: the overall radiation intensity increases - strong oscillations in particle

radiation -> distortion from the original spherical symmetry

o Third stage: particle radiation continues to exhibit oscillations - significant “random”

changes in particle velocities

o Explosions of aluminum particles were often observed before their extinction

Mechanism of asymmetric aluminum particle combustion

[1] Dreizin EL. Effect of Phase Changes on Metal-Particle Combustion Processes. Combustion, Explosion and Shock Waves. 2003;39:681-93.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Towards Zero-Carbon Emissions

o Growing concern towards a transition to low-carbon economy

Automotive manufacturers explore carbon-free alternatives to the classic

hydrocarbon-fueled powertrain

o Most renewable energy sources are not portable nor scalable

Need for energy content, refill time, autonomy...

H2 and batteries: lacking safety and/or energy density

Concept drawing of the fuel cycle.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Powder Characterization

o Extract sufficient power from metal oxidation:

Reducing the particle size leads to improved reaction rates.

o Two main concepts have been proposed in the literature

Nanoparticles under engine-like conditions [1].

External heat engine [2].

[1] Mandilas, C. et al. (2016). Energy & Fuels, 30 (5), 4318–4330

[2] Bergthorson, J.M. et al. (2010). Applied Energy, 160, 368-382

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Towards Zero-Carbon Emissions

SEM imaging of the Al powders studied.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Experimental Setup

Schematic of the burner setup.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Flow Characterization

o Particle image velocimetry:

Flat and symmetric velocity profile

Good qualitative concentration spatial homogeneity

𝑆𝑡𝑘 ~ 10−3

Flow characterization.

(b). Mean velocity profile.

(a). Mean velocity field.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Dust Concentration

o The dispersion system is calibrated for dust concentration using 2 different methods:

Beer-Lambert’s law

Real-time weighing measurements and total flow rate

Time evolution of laser attenuation. Calibration law.Time evolution of laser attenuation. Calibration law.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Flame Tomography

o Images are formed by scattered light by the condensed-

phase species.

o Three distinct zones are observed:

Fresh mixture

Reaction zone: evaporation and drop in particle density

Burnt mixture

o Burning velocities

Integration of the dark zone contour to obtain the flame

surface

Is it representative of the flame front position? Example of Al-air flame tomography.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Direct Flame Visualization

o Direct visualization of AlO emissions

AlO radical is a well-known combustion intermediate, and is often used as an indicator

of the flame front position [1]

Planar information obtained using an inverse Abel transform.


Mean flame image based on AlO(g) emissions for Al/air flames.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Velocity Field

o PIV applied to tomography images

𝑆L is the velocity at which fresh gases cross the

combustion wave

Flame stretch is weak , 𝐾∼ 68 s−1

o Burned gases expansion is difficult to evaluate

Are the oxide products good PIV trackers?

Unburned aerosol velocity along the dashed lines.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Burning Velocity Results

o For 0,8<𝜙<1,5 , 𝑆_𝐿 remains constant, and 𝑆L= 28.5 cm/s𝑆L is the velocity at which fresh

gases cross the combustion wave

The addition of metal doesn’t dilute oxygen concentration [1].

Lower reproducibility error highlights the importance of the dispersion conditions.

Burning velocities for Al/air flames in air.

[1] Goroshin et al. (1996). Proceedings of the Combustion Institute , 26:1961-7.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Flame Temperature

o Flame temperature calculation:

AlO emissions are simulated line-by-line by optimizing temperature and optical length

[1, 2, 3].

The resulting temperature is associated with the flame temperature.

Simulated AlO emission spectrum.

[1] Arnold et al. (1969). Journal of Quantitative Spectroscopy and Radiative Transfer, 9(6), 775-798.

[2] Partridge et al. (1983). Journal of Quantitative Spectroscopy and Radiative Transfer, 30(5), 449-462.

[3] Coxon and Naxakis (1985). Journal of Molecular Spectroscopy, 111(1), 102-113.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Flame Temperature

o For 0,8<𝜙<1,5 , 𝐓𝒇 remains constant, and 𝐓𝒇∼ 3150 K.

Similar to the burning velocity measurements.

Adiabatic flame temperature: 3540 K.

Flame temperatures from aluminum/air at different dust concentrations.

1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

Conclusions1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

o Contribute to the global knowledge of metal fuel combustion

o New experimental devices were designed

o New optical diagnostics were developed

o Promising results to precise the combustion process of isolated particles

o Metal fuels can be considered as a potential candidate for a clean, renewable and dense

energy carrier.

o Good potential seems achievable but a lot of work still requested to feed a complete Life

Cycle Analysis of this new energetic vector

o Collaborative approach gathering top proficiencies are a key of success

o Strong support of Groupe PSA to further support this technology

More details in1. Al as a FUEL

2. Al COMBUSTION

2.1 PROPULSION

- Context

- Fluidic levitator


- Recent advances

2.2 HEAT GENERATION

- Context

- Burner design


3. CONCLUSIONS

• LOMBA R, HALTER F, CHAUVEAU C, BERNARD S, GILLARD P, MOUNAÏM-ROUSSELLE C, TAHTOUH T, GUEZET O. Experimentalcharacterization of combustion regimes for micron-sized aluminum powders. 53rd AIAA Aerospace Sciences Meeting,American Institute of Aeronautics and Astronautics (2015)

• LOMBA R, BERNARD S, GILLARD P, MOUNAÏM-ROUSSELLE C, HALTER F, CHAUVEAU C, TAHTOUH T, GUEZET O. Comparison ofCombustion Characteristics of Magnesium and Aluminum Powders. Combustion Science and Technology. 188, pp. 1857-77(2016)

• OSMONT A., GOKALP, I., CATOIRE L., Evaluating missile fuels. Propellants, explosives Pyrotechnics 31, pp. 343−354 (2006)

• SAROU−KANIAN, V., RIFFLET, J−C., MILLOT, F., GOKALP, I. Carbon dissolution kinetics in aluminium droplet combustion.Implications for aluminized solid propellants. Combustion and Flame (2007)

• SAROU−KANIAN, V., RIFFLET, J−C., MILLOT, F., GÖKALP, I. Aluminum combustion in wet and dry CO2: Consequences for surfacereactions. Combustion and Flame, 145, pp. 220−230 (2006)

• SAROU−KANIAN, V., RIFFLET, J−C., MILLOT, F., VERON, E., SAUVAGE, T., GÖKALP, I. On the role of carbon dioxide in thecombustion of aluminum droplets. Combustion Science and Technology, 177, pp. 2299−2326 (2005)

• SAROU−KANIAN, V., RIFFLET, J.C., MILLOT, F., MATZEN, G., and GÖKALP, I. Influence of nitrogen in almuninum dropletcombustion. Proceedings of the Combustion Institute 30, pp: 2063−2070 (2005)

• SHAFIROVICH, E., ESCOT−BOCANEGRA, P., CHAUVEAU, C., GÖKALP, I., GOLDSHLEGER, U., ROSENBAND, V., and GANY, A.Ignition of single nickel−coated aluminium particles. Proc. Combustion Institute 30, pp: 2055−2062 (2005)

• SHAFIROVICH, E., SALOMON, M., GÖKALP, I., Mars Hopper versus Mars Rover, Astronautica Acta 59, pp. 408−423 (2006)

• ESCOT-BOCANEGRA, P., CHAUVEAU, C., GÖKALP, I., Experimental studies on the burning of coated and uncoated micro andnano-sized aluminium particles. To appear in Aerospace Science and Technology, 2007

• DAVIDENKO, D., GÖKALP, I. Numerical modelling of combustion of aluminium particle clouds in air, 3rd European CombustionMeeting, Chania, Crete, Grece, 11-13 April, 2007

• SAROU-KANIAN V., OUAZAR, S., ESCOT-BOCANEGRA, P., CHAUVEAU, C., GÖKALP, I., Low temperature reactivity of aluminiumnanopowders with liquid water. 3rd European Combustion Meeting, Chania, Crete, Grece, 11-13 April, 2007

• CATOIRE, L., LEGENDRE, JF., GIRAUD, M. Kinetic model for aluminum sensitized ram accelerator combustion. Journal ofpropulsion and Power, 19:196-202 (2003)

• SHIWART, MT., CATOIRE, L., LEGRAND, B., GÖKALP, I. Rate constants for the homogeneous gas-phase Al/HCl combustionchemistry. Combustion and Flame 132: 91-101 (2003)

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