Characterization of soot particles coming from aircraft and ship emissions: unique properties and impact on the atmosphere

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Characterization of soot particles coming from aircraft and ship emissions: unique properties and impact on the

atmosphere

Victoria Tishkova, Benjamin Demirdjian, Daniel Ferry, Olga B. Popovicheva, Jana Moldanova, Erik Fridell, Alessandro Faccinetto, Cristian Focsa

To cite this version:

Victoria Tishkova, Benjamin Demirdjian, Daniel Ferry, Olga B. Popovicheva, Jana Moldanova, et al..

Characterization of soot particles coming from aircraft and ship emissions: unique properties and

impact on the atmosphere. CARBON 2009, Jun 2009, Biarritz, France. �hal-03227978�

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«Onion-like»structure

~ 0,35 nm 0,142 nm

TEM: JEOL JEM 3010, résolution 1.6 Å 002 10.

11.

000

•d002= 3,50 ±0.18 Å ( graphite : d₀₀₂= 3,35 Å )

•d10. = 2,07 ±0.11Å

•d11.= 1,19 ±0.07Å Air

N2 + O2

Fuel : CnHm+ S Perfect combustion : Gaz: CO2+ H2O + N2+ O2+ SO2

Real Combustion : Gaz: CO2+ H2O + N2+ O2+ NOx+ CxHy+ CO + SOx: gas

C

suie

particles : Directly injected in the

troposphere and in the Lower strastosphere

The low ability to predict climatic consequences (only qualitative estimates)



The paucity of data about the physicochemical properties of aircraft engine soot

Most of studies, based on laboratory-generated soot particles



show a large variation in their nucleation properties and reactivity.

This study is devoted to the comparison of laboratory soot / engine soot:

• morphology,

• microstructure,

• chemical composition,

• hygroscopic properties



determine the mechanisms responsible for the formation of CCN (contrails, clouds cirrus)

AIRCRAFT COMBUSTOR SOOT(collab. Aviation Institute, Moscow)

3 -5 4 -4.5 1250-1450 300 D30-KU

Pression (atm) Air / fuel

ratio Toutlet(K) Tinlet(K) Aircraft engine

Aviation kerosene TC1 sulfurcontent: 1100 μg.g^-1

Exhaust pipe High-volume bulk aerosol sampler

Diesel fuel contains ash 0.01 wt% and sulfur 0.5 wt%

Sampled on the end-of the pipe on beard of marine conveyer ships burning diesel and heavy fuel oil.

Heavy Fuel Oil is a residual from crude oil refinement, after gasoline and distillate

fuel oils are extracted through distillation.

It typically contains sulfur up to 3.5 wt%, ash 0.1 wt%, vanadium 0.02 wt%, calcium 0.003 wt%.

Heavy Fuel Oil is a residual from crude oil refinement, after gasoline and distillate fuel oils are extracted through distillation.

It typically contains sulfur up to 3.5 wt%, ash 0.1 wt%, vanadium 0.02 wt%, calcium 0.003 wt%.

KEROSENE FLAME TC1 SOOT

15-20 cm

Produced by burning aviation TC1 kerosene in a wick oil lamp

nm D  55





3.60 0.21

d002 d102.070.11^





1.23 0.06 d11 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 20000

24000 28000 32000

10 004 002

Intensity, a.u.

Q, Å

^-1





3.58 0.19 d002





2.050.09 d10





1.77 0.06 d11





13 2 Lc





132 La

ND SAED







 3 . 58 0 . 20

d

002

d

10

 2 . 07  0 . 10 

^ Lc212^

1 2 3 4

10000 15000 20000 25000 30000 35000

004 10 002

aircraft engine combustor soot kerosene flame TC1 soot

intensity (a.u.)

Q (Å^-1)

In fraction of impurities we observe iron- containing particles FeO FeO, , FeO(OH FeO(OH), ), copper containing CuO CuO, Cu , Cu

₂₂

O O and aluminum containing Al(OH) Al(OH)

33

.





3.500.18 d002





2.07 0.11 d10







 1 . 19 0 . 07 d

11

ND

EDS:

carbon (95.0±0.6 wt%) oxygen (5.0±0.3 wt%).

C=68,95 wt%

O=20,87 wt%

S=2,5 wt%

C=68,95 wt%

O=20,87 wt%

S=2,5 wt%

C=61,2 wt%

O=6,1 wt%

Fe=32 wt%

S=0,7 wt%

20 nm

100 nm

FeO Sulfur-rich area

Sulfur-rich area Iron-rich area Iron-rich area

AEC soot, main fraction

nm D  48

EDS:

C (96.6±0.7 wt%), O (3.1±0.5 wt%), S (0.3±0.1 wt%)

EDS:

C (96.6±0.7 wt%), O (3.1±0.5 wt%), S (0.3±0.1 wt%)

Labo soot

500 750 1000 1250 1500 1750 2000

0,000 0,002 0,004 0,006 0,008 0,010 0,012 0,014 0,016

0,018ionic sulfate a)

organics sulfate HSO4-

C-H aromatic rings

753

C=0 aliphatic C=0 aromatic

873 582

700834 1050

12301355 1419 1583

1673

absorbance

cm^-1 Engine soot

SAED

LABO SOOT; ENGINE

Bands cm^-1 hydrophilic ity CH deformation,

aromatics

650-920 Low

-C-O-C-anhydrids,

aryls 1230 Medium

C-OH stretch, phenols 1154,1112 Medium -O-aromatic ester 1154, 1112 Low O-H stretch, hydroxyl 3290 High

ENGINE ONLY Bands cm^-1 Hydrophilici ty C=O carbonyl,

aliphatic

1673 High

C=O carbonyl,

aromatic 1583 High

HSO4-ion 1355,1230

1050, 878, 582

High

Organic sulfates 1350, 1420 High

Engine soot has much more hydrophilic surface functional groups than the surrogate soot

Engine soot

Labo soot

•

Engine soot adsorbs big amounts of water at low RH and at T = 295 K

surface active sites (sulfates, carbonyls)

•

Adsorption (engine soot) >> adsorption (labo soot)

Lamp soot relatively hydrophobic (isotherm shape)

• Possible climate impacts which are still least defined in comparison with land- based transport

• Ship emission particulates can act as nuclei for the formation of cloud droplets

• Ships may produce ship tracks

The starting point for evaluating the effect of ship emission on environment is to characterize its properties (like structure, chemical composition etc) Satellite image of ship tracks

Water-soot interaction is one of the important parameters defining ability of the soot to form contrails and ship tracks Water-soot interaction is one of the important parameters defining ability of the soot to form contrails and ship tracks





3.65 0.17 d002





2.150.09

d10 d₁₁1.170.05^

EDS: Carbon (89.9±3.1 wt%), Oxygen (4.4±0.5 wt%), vanadium (2.4±0.3 wt%), and Sulfur (3.2±0.4 wt%); Nickel (0.3±0.1 wt%).

0 2 4 6 8 10

0 200 400 600 800

V O C

S

Ca V

V Fe Ni Cu

a.u. Cu

keV

dark core inside particles

SAED+EDS:Ni

₃

S

₂

, Na

6

(CO

3

)(SO

4

), Ni

2

Fe, Ni

₃

Fe, NiO, V

₂

O

₃

, NiS

Soot

Soot- -type particles type particles

Characterization of soot particles coming from aircraft and ship

Characterization of soot particles coming from aircraft and ship emissions: unique properties and impact on the atmosphere. emissions: unique properties and impact on the atmosphere.

V. Tishkova1,

V. Tishkova1, B. Demirdjian B. Demirdjian1, D. Ferry1 1, D. Ferry1 O.B. Popovicheva2 O.B. Popovicheva2 J. Moldanova3, E. Fridell3 J. Moldanova3, E. Fridell3 A. Faccinetto4 and C. Focsa4 A. Faccinetto4 and C. Focsa4 1CINaM, UPR CNRS 3118, Campus de

1CINaM, UPR CNRS 3118, Campus de Luminy Luminy, Marseille, France , Marseille, France 2SINP Moscow State University, 119991, Moscow, Russia 2SINP Moscow State University, 119991, Moscow, Russia 3IVL

3IVL Swedish Swedish Environmental Environmental Research Research Institute, SE 400 14 Gö Institute, SE 400 14 G öteborg, teborg, Sweden Sweden 4PhLAM, UMR 8523, Universit

4PhLAM, UMR 8523, Université é de Lille 1, Villeneuve d de Lille 1, Villeneuve d’ ’Ascq, France Ascq, France

Biarritz, France, June 14-19, 2009.

AIRCRAFT ENGINE COMBUSTOR SOOT

KEROSENE FLAME TC1 SOOT MAIN FRACTION OF AIRCRAFT ENGINE COMBUSTOR SOOT

FORMATION OF CARBON NANOPARTICLES (SOOT) IN THE ATMOSPHERE THE SCIENTIFIC BACKGROUND SOOT PRODUCTION

AIRCRAFT ENGINE COMBUSTOR SOOT: FRACTION OF IMPURITIES

SOOT CHEMICAL COMPOSITION: FTIR (SURFACE FUNCTIONALS GROUPS) WATER UPTAKE ON SOOT PARTICLES

SHIP EMISSION AND SAMPLING WATER UPTAKE ON DIESEL FUEL AND HEAVY FUEL OIL COMBUSTION PARTICLES MICROSTRUCTURE AND CHEMICAL COMPOSITION OF DIESEL FUEL AND HEAVY FUEL OIL EMISSION RESIDUALS

Main fraction Main fraction

FeO FeO

MgO MgCO

₃

TiO MgO MgCO

₃

TiO





3.40 0.16 d002





2.08 0.08 d10





1.23 0.06 d11

EDS of main fraction:

C=97.6±0.7 wt%

O=1.8±0.3 wt%

Fe=0.6±0.1 wt%

EDS of main fraction:

C=97.6±0.7 wt%

O=1.8±0.3 wt%

Fe=0.6±0.1 wt%

Impurities Impurities

nm D  82 DIESEL FUEL

HEAVY FUEL OIL SAMPLING: MARINE DIESEL FUEL AND HEAVY FUEL OIL COMBUSTION RESIDUALS

0.0 0.2 0.4 0.6 0.8 1.0

0 1000 2000 3000 4000 5000 6000 7000

DF

HFO

N(H2O)/mn2

P/Ps

S DF-M=0.7 m²/g, SHFO=5.4 m2/g S DF-M=0.7 m²/g, SHFO=5.4 m2/g

Water Soluble Fraction for DF and HFO are 19 and 44 wt%, respectively Water Soluble Fraction for DF and HFO are 19 and 44 wt%, respectively

600 ML

Significant uptake (up to 200, 275, and 600 ML at higher p/p

_s)

for HFO, DF-M, respectively and the presence of many hydrophilic functional groups on the surface of ship residuals indicate that the dominant mechanism of their water uptake is the water dissolution into the soluble coverage and the formation of a thick solution film surrounding the particles.

Significant uptake (up to 200, 275, and 600 ML at higher p/p

_s)

for HFO, DF-M, respectively and the presence of many hydrophilic functional groups on the surface of ship residuals indicate that the dominant mechanism of their water uptake is the water dissolution into the soluble coverage and the formation of a thick solution film surrounding the particles.

H₂O

WSF

H₂O H2O

H2O H2O H₂O

Aircraft engine soot as contrail nuclei

O.B. Popovicheva, N.M. Persiantseva, E.E. Lukhovitskaya, N.K. Shonija, N.A. Zubareva, B. Demirdjian, D. Ferry, and J. Suzanne Geophysical Research Letters 31 (11): Art. No. L11104 Jun 5 2004

Heterogeneities in the microstructure and composition of aircraft engine combustor soot: impact on the water uptake.

B. Demirdjian, D. Ferry, J. Suzanne, O.B. Popovicheva, N.M. Persiantsevaand N.K. Shonija Journal of Atmospheric Chemistry, 56 (1) (2007) 83-103

Water interaction with hydrophobic and hydrophilic soot particles

O. B. Popovicheva, N. M. Persiantseva, N. K. Shonija, P. DeMott, K. Koehler, M. Petters, S. Kreidenweis, V. Tishkova, B. Demirdjian, and J. Suzanne

Physical Chemistry Chemical Physics 10 (2008), 2332-2344

Effect of soot on immersion freezing of water and possible atmospheric implications O. Popovicheva, E. Kireeva, N. Persiantseva, T. Khokhlova, N. Shonija, V. Tishkova, and B. Demirdjian Atmospheric Research 90 (2008) 326–337

Characterisation of particulate matter and gaseous emissions from a large ship diesel engine

Jana Moldanová, Erik Fridell, Olga Popovicheva, Benjamin Demirdjian, Victoria Tishkova, Alessandro Faccinettoand CristianFocsa AtmosphericEnvironment43 (2009) 2632-2641

REFERENCES

Fraction of impurities responsible of the high hydrophilicity Fraction of impurities responsible of the high hydrophilicity

nm D  48

MICROSTRUCTURE

CHEMICAL COMPOSITION:

“ONION-LIKE”MICROSTRCUTURE

TURBOSTRATIC STRUCTURE

MICROSTRUCTURE

CHEMICAL COMPOSITION: