Aerosol Science and Technology

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Jet Engine Exhaust Aerosol Characterization

A. Petzold & F. P. Schröder

To cite this article: A. Petzold & F. P. Schröder (1998) Jet Engine Exhaust
Aerosol Characterization, Aerosol Science and Technology, 28:1, 62-76, DOI:
10.1080/02786829808965512

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 ELSEVIER

Jet Engine Exhaust Aerosol Characterization

A. Petzold and F. P. Schvoder
DEUTSCHE FORSCHUNGSANSIALT FUR IUI-I- UND KAUMFAHRT (DI R), INSTITUT FUR PHYSIK DER
ATMO\PHARE, OBERPTAFFENHOFEN, D-82234 WLSSLING, GLRMANY

ABSTRACT. Jet engine exhaust aerosol was characterized with respect to mass
concentration and composition of the carbonaceous aerosol fraction and the par-
ticulate sulfate as a function of engine power setting for fuel with low-sulfur content
(6 ppm) and high-sulfur content (3000 ppm). The ratio of black carbon (BC) to total
carbon (TC) varied from 11% with the engine in idle run to >SO% at take-off thrust.
The corresponding BC emission index was C0.6 g kg-' fuel on a mass scale and
C1.7 x 10'' kg-' fuel on a number scale. The optical specific absorption coefficient
of the BC aerosol was measured to 6 k 1 m2 g-' by filter reflectance analysis (A =
0.8 pm). The carbon aerosol split into a primary soot mode at 0.045 p m diameter
with geometric standard deviation 1.5 and a coagulation mode at 0.18 p m diameter
with geometric standard deviation 1.42. The mass emission index of particulate
sulfate remained almost constant at <0.05 g kg-' throughout the examined engine
power setting between 11% and 71% take-off thrust. The conversion rate from SO,
molecules into particulate SO:- within the young exhaust plume prior to sampling
(plume age <0.1 s) was <0.5% with only a slight dependence on engine power
setting. AEROSOL SCIENCE AND TECHNOLOGY 2852-76 (1998) @ 1998 American
Association for Aerosol Research

INTRODUCTION glomerates with a maximum diameter of

The environmental effects of jet engine ex-
haust emissions from high-flying aircraft on
the state of the atmosphere have gained in-
creasing attention in the discussion of an-
thropogenic climate change and ozone de-
pletion (Schumann, 1994; Weisenstein et al.,
1996). Of particular interest are carbona-
ceous particles and sulfur oxides that are
emitted from aircraft engines in addition to
large amounts of H,O and CO,. In the upper
troposphere and lower stratosphere (10-13
km) carbonaceous particles are trace constit-
uents with mass concentrations of about
0.6 ng m-" their residence time is approxi-
mately several weeks up to a few months
(Pueschel, 1996). The particles form ag-
about 0.3 p m that are composed of smaller
spheres with 0.03 pm in diameter (Sheridan
et al., 1994). Up to 50% of the BC near the
tropopause region can be attributed to air-
craft emissions (Schumann, 1994; Pueschel,
1996). An open but very important question
is to what extent carbonaceous particles are
activated to form cloud condensation nuclei
(CCN). Reported values of the fraction of
droplet-forming nuclei at natural cloud su-
persaturation of 5 1 % vary between less
than 1% (Pitchford et al., 1991; Hudson et
al., 1991) and 40% (Whitefield et al., 1993).
Of major interest are the water vapor nu-
cleation properties of jet exhaust particles
that strongly depend on the content of wa-
Aerosol Science and Technology 28:62-76 (1998)
0 1998 American Association for Aerosol Research
Published by Elsevier Science Inc.
Aerosol Science and Tcchnology
28:1 January 1998
ter-soluble matter. According to the particle
formation mechanism during combustion,
carbonaceous particles consist of black car-
bon (BC) and organic carbon (OC) with
varying split between BC and OC. In gen-
eral, young combustion aerosol contains al-
most no water-soluble matter. Hence, pure
carbonaceous aerosol is hydrophobic, i.e., it
requires high supersaturations to be acti-
vated (Niessner et al., 1990), and it shows
almost no water uptake in a humid atmo-
sphere (Wyslouzil et al., 1994). However, the
treatment of carbon particles with H2S04
improves their hydration properties so that
sulfuric acid treated carbon particles be-
come activated already at very low super-
saturations of less than 0.3% (Lammel and
Novakov, 3 995).
A potential source for chemically acti-
vated BC particles is the formation of BC-
H,SO,-H,O agglomerates inside a young ex-
haust plume of a jet engine (Kdrcher, 1996).
It is suggested that emitted SO, is oxidized
by O H or 0 to SO, that reacts with H,O to
form gaseous H,S04. The formation of SO,
is restricted only to the very young plume
with less than 10 ms in age (Frenzel and
Arnold, 1994; Karcher et al., 1995). The sul-
furic acid undergoes binary nucleation with
water vapor followed by heterogeneous nu-
cleation of the H,S04-H,O mixture onto
carbon particles (Miake-Lye et al., 1994;
Zhao and Turco, 1995). These chemically
activated carbonaceous particles are as-
sumed to be the most likely source of cloud
condensation nuclei (CCN) in contrail for-
mation (e.g., Schumann et al., 1996, Brown
et al., 1996). Up to now it is not clear to what
extent gaseous H2S0, exists in the exhaust
plume. As discussed by Karcher et al. (1995),
Frenzel and Arnold (1994) and Karcher
(1996) gas-to-particle conversion and coag-
ulation lead to the buildup of (H,SO,),
(H,O), clusters with an approximate size of
0.001 pm within a plume age of 0.5 s that
then will grow by H,S04 condensation, co-
agulation, and water uptake to very small
droplets making up an invisible contrail.
Model derived estimates of the conversion
rate of SO, into S O : in young exhaust
plumes (Myake-Lye et al., 1994; Karcher et
Jet Engine Exhaust Aerosol Characterization 63
al., 1995; Brown et al., 1996) as well as ex-
perimental data (Frenzel and Arnold, 1994)
are between 0.5% and 1.4% while in situ
measurements in the lower stratosphere be-
hind a Concordc indicate a conversion rate
of 12-45% (Fahey et al., 1995b).
A second path for S O : formation is the
catalytic oxidation of SO, in water droplets
containing carbon particles (e.g., Dlugi et al.,
1981; Mamane and Gottlieb, 1989). Since
this process requires high relative humidities
(270%) and long reaction times ( 2 1 h) it
seems to be important only for aged exhaust
plumes. Reported conversion rates vary
from 0.140 g SO:- g-' C (Mamane and
Gottlieb, 1989) to 0.6 g S O : g-' C (Dlugi et
al., 1981).
To achieve better understanding of the
processes involved, emission rates for total
carbon (TC), BC and particulate sulfuric
acid will be reported. Additionally, depen-
dencies of OC-BC split and emission rates
on engine power setting and sulfur content
of the burned fuel will be given.
EXPERIMENTAL
Measurements were performed in the ex-
haust plume of a Rolls RoyceISNECMA
M45H Mk501 turbofan engine of the
ATTAS aircraft of DLR (Deutsche For-
schungsanstalt fiir Luft- und Raumfahrt)
during the SULFUR 4 experiment in March
1996. This engine has a bypass ratio of 3:1
and generates about 5 times more carbon
particles than most modern engines. A more
detailed description of the engine parame-
ters is given by Schumann (1995). During
sampling, the engine was operated at power
settings 11%, 30% and 66% with a sulfur-
free fuel (sulfur content 6 ppm) and at
power settings 11%, 2096, 30% and 71%
burning a fuel with high-sulfur content of
3000 ppm. For both fuel sulfur contents the
same low-sulfur fuel was used. The high-
sulfur content of 3000 ppm was achieved by
adding distinct amounts of dibutylsulfide to
the fuel (Busen et al., 1997). Thermody-
namic properties of dibutylsulfide and stan-
dard jet fuel are of comparable order, so that
64 A. Petzold
i'
7
JET ENGINE
/
CONICAL SHROUD
PARTICLE-FREE
COMPRESSED AIR
FIGURE 1. Sketch of the sampling system.
a similar combustion behavior of the low-
and high-sulfur fuel is expected.
Aerosol Sampling
For the collection of turbine exhaust parti-
cles on appropriate filter matrices a setup
comparable to that described by Champagne
(1971) was used. The inlet of the sampling
line was positioned at a distance of 1.5 m
behind the exit of the turbine engine in the
exhaust gas stream of the engine core. The
plume age at the sampling line inlet varied
from 5 ms to 15 ms depending on the power
setting. To achieve an almost isokinetic sam-
pling, the exhaust gas was decelerated by a
conical shroud with an overall opening angle
of 14 degrees that covered the sampling in-
let. The sampling inlet itself was positioned
at a distance of 10 cm behind the tip of the
shroud. Immediately behind the sampling
inlet the exhaust aerosol was diluted by add-
ing particle-free compressed air to the sam-
pled gas. The dilution ratio was set to 1:1 and
checked by measuring the dilution air flow
with a rotameter. The total sampling volume
sucked through the filter was limited to
10.5 L minp' by a critical orifice and moni-
tored with a dry gas meter. The sampling
line had an overall length of 8 m from the
Aerosol Science and Technology
28:1 January 1998
FILTER CRITICAL PUMP VOLUME METER
ORIFICE
inlet to the filter holder and an inner diam-
eter of 4 mm. Thus, it took about 0.6 s to
draw a particle from the tip of the sampling
line to the filter holder. The sampling time
varied between 1 min and 5 min depending
on the corresponding power setting. The fil-
ter holder itself allowed parallel sampling on
two different filter matrices that were used
for optical/thermal carbon and ion chroma-
tography analyses, respectively. A sketch of
the sampling setup is given in Fig. 1.
Chemical Characterization
BC mass deposited on a particle-laden pre-
fired glass fiber filter (MN 85/90 BF, Mach-
erey and Nagel) was determined by a ther-
mal method (Petzold and Niessner, 199%).
To remove the organic carbon fraction from
the sample a combination of solvent extrac-
tion in a 1:1 (v/v) mixture of toluenel2-pro-
panol and heating of the previously ex-
tracted sample under N, to 500°C was
applied. The remaining black carbon was
analyzed as CO, that evolved during sample
combustion at 650°C under 0, by coulomet-
ric titration in a carbon analyzer (Coulomat
702, Stroehlein). The precision of the
method is 8% and 5% of deposited mass for
BC determination and TC determination,
Aerosol Science and Technology
28:l January 1998
respectively. The detection limit corre-
sponds to a carbon load of 9 p per filter
3
sample (filter area approx. 10 cm ). Further
details on the thermal method are given by
Petzold and Niessner (1995a).
Optical analyses of particle-laden glass fi-
ber filters were performed with an aethalo-
meter A E 9 (Magee Scientific) on the same
filters as used for thermal carbon analysis
prior to the extraction/combustion proce-
dure. To convert light attenuation by parti-
cle-laden glass fiber filters into BC mass
loading the value of the specific attenuation
cross-section was set to 19 m2 g-' as recom-
mended by the manufacturer. An accurate
value of the blank filter reference signal was
obtained by measuring the light transmission
of each filter before sampling. After sam-
pling and drying, the filter transmission was
measured again to obtain the corresponding
light attenuation. To improve the accuracy
of those attenuation determinations all filter
measurements were repeated for at least
three times in different positions in the filter
holder. This procedure gave an error in at-
tenuation of about 2% (Petzold and Niess-
ner, 1995a). A more general description of
this filter transmission method is given by
Petzold et al. (1997).
To obtain further information about the
absorptive properties of the sampled BC
particles the reflectance of selected particle-
laden filter samples was measured with an
EEL 43 Smoke Stain Reflectometer (Diffu-
sion Systems Ltd.). The reflectance R (in %)
is related to the BC mass loading S,, and
specific absorption cross section a,,, (BC)
via the relation In R = -2a,,,S,, (Bailey
and Clayton, 1982). In combination with an
independent measurement of S,, via the
thermal method a reflectance measurement
yields an estimate for a,,, (BC) within an
accuracy of about 20% with respect to an
average wavelength of 0.8 p m (Petzold and
Niessner, 1995a; 199%).
S O : was measured by ion chromatogra-
phy using a DIONEX 4000i instrument
equipped with an AS4A anion specific col-
umn and AG4A guard column. Before sam-
pling, the glass fiber filters were washed with
bi-distilled water and fired at 500°C for 4 h to
Jet Engine Exhaust Aerosol Characterization 65
achieve a low and constant SO:- back-
ground signal. This pretreatment is a simpli-
fied version of a procedure reported by Rob-
erts and Friedlander (1976) that should
lower the catalytic conversion of gaseous
SO2 to particulate sulfate on the filter sub-
strate. Sulfate was extracted from the filters
with 30 min ultrasonic extraction in bi-dis-
tilled water. The error in S O : determina-
tion is estimated to 3% (e.g., Harrison and
Perry, 1986).
Size Distribution Measurements
Particle size distributions of jet engine ex-
haust aerosol were measured with two opti-
cal spectrometers and a condensation parti-
cle counter installed on the Falcon research
aircraft of DLR during the SULFUR 4 ex-
periment. A passive cavity aerosol spectro-
meter probe (PCASP 100-X, PMS Inc.) clas-
sifies aerosol in the size range from 0.1 pm to
3 pm in diameter by the integral amount of
scattered laser power. Since a tiny air sample
flow is aerodynamically focused by a com-
paratively large, dry (and warmer) sheath air
flow, any water bound to aerosol particles
will have left the condensed phase before
detection and the aerosol can thus referred
to as "dry" (RH << 5%). A forward scatte-
ring spectrometer probe (FSSP 300, PMS
Inc.) measures the hydrated aerosol in situ in
the size range from nominal1 0.3 to 20 pm
and requires at least 20 m s-'true air speed
to provide data (Strapp et al., 1992). Both
spectrometers were mounted 0.5 m below
the wings of the Falcon and approx. 0.4 m
ahead of the leading edge. Further informa-
tion about the total number concentration
of particles with D > 0.01 p m was ob-
tained by a modifed CPC (TSI model
3010) installed inside the aircraft.
RESULTS AND DISCUSSION
Sampling Losses
Before mass concentrations and derived
emission indices of the measured species are
discussed, we briefly focus on possible losses
and artifact formation during sampling. As
66 A. Petzold
main loss processes particle scavenging due
to water vapor condensation in the sampling
line and diffusion/impaction loss of particles
and molecules to the tube walls are assumed.
The losses due to condensation processes
were excluded by diluting the sample air with
ratio 1:l as described in the experimental
section. Using characteristic engine parame-
ters (emission index of H,O: 1.2 kg kgC1fuel,
fuel flow at 71% power setting: 0.24 kg sC',
volume flow: 38 m3 s-l) given by Schumann
(1995), a water vapor concentration of approx.
8 g mC3inside the plume at the engine exit is
obtained. Diluting the exhaust air 1:l results
in a maximum water vapor mass concentra-
tion of 4 g mC3that is below water saturation
at the filter holder temperature of 10°C.
Hence, no particle scavenging due to water
vapor condensation has to be considered.
The particle losses inside the sampling
line will focus on diffusional losses. Losses in
the mixing zone of sample air and dilution
air are neglected, because the dilution air
was addcd via a coaxial flow under nearly
isokinetic conditions to avoid turbulence.
Electrostatic losses and inertial losses inside
the sampling line were minimized by using
metallic tubes with only smooth curvatures
for sampling.
Starting with the parameters sample flow
Q = 1.75 X m%-', diameter of sam-
pling tube d = 0.004 m and length of sam-
pling tube L = 8 m we obtain a flow velocity
of 14 m sC1 and a Reynolds number Re .=
3100 for the sample flow, i.e., the flow can
assumed to be quasi-laminar. Both diffusion
of molecules as well as diffusion of particles
are treated by the same relations. The pen-
etration P through a circular tube is given by
if p > 0.02 and P < 0.19 and
if p L. 0.02 (Willeke and Baron, 1993). The
parameter p is defined as
Aerosol Science and Technology
28:1 January 1998
particle size or molecule species enter p via
the diffusion coefficient D. The fractional
loss (in %) as a function of the penetration
P is given as 100 (1 - P ) .
The diffusion coefficient of SO, diluted in
air is 1.3 x m2 sC' (Durham et al., 1978),
the diffusion coefficient of H,S04 is esti-
mated to 1.0 X m2 sC1because of the
higher molecular weight. The diffusion coeffi-
cients of particles with diameters 0.01 pm,
0.05 p m and 0.1 pm are 5.2 X loC8m2 sC1,
2.4 X 1 0 - h 2 s-' and 6.8 X 1 0 ~ m2 " sC'
(Willeke and Baron, 1993). Introducing these
values in Eqs. (1) and (2) corresponding frac-
tional losses of 8.9%, 1.2% and 0.5% are ob-
tained. The fractional losses for SO, are less
than 10% with sticking probabilities less than
0.01. Gaseous sulfuric acid, which is a very
reactive species, as well as (H2S04),(H,0),
clusters with a diameter of 0.003 pm would
be adsorbed almost completely at the tube
wall ( P L. 0.05).
Summarizing these estimates, the gas
phase SO, and aerosol particles with D, 2
0.02 p m will be transferred through the
sampling line without substantial losses,
while gaseous H2S04 is lost almost com-
pletely to the tube walls. Artifact formation
of sulfuric acid particles by catalytic oxida-
tion of SO, at sampled carbon particles is
only of minor importance because the time
scale for this process is in the order of hours
(Dlugi et al., 1981). Sulfuric acid formation
by SO, oxidation at the surface of the glass
fibers of the filter matrix is reduced by the
applied filter pretreatment, but nevertheless,
the S O : mass concentrations should be
taken as an upper limit for the "true" mass
concentrations. The transformation of gas-
eous H,SO, to particulate sulfuric acid on
the filter matrix can be excluded.
Mass Concentrations
The main parameters that are derived di-
rectly from the filter analyses are the mass
concentrations of total carbon (TC) and
black carbon (BC) from thermal filter ana-
lysis, black carbon (BC (0~:))obtained with
an aethalometer and SO, from ion chro-
matography. The SO, concentration is de-
Aerosol Science and Technology
28:l January 1998
TABLE 1. Mass concentrations in the core exhaust of a turbofan engine Rolls RoyceISNECMA M45H Mk501;
values are given for total carbon (TC) and black carbon (BC) from thermal filter analysis, black carbon [BC (opt)]
obtained with an aethalometer and SO:- from ion chromatography, SO, mass concentrations were calculated with
the assumption that all sulfur contained in the fuel was oxidized during combustion
Sulfur Content Power Setting
(PP~) (%I TC
duced from the fuel flow and the sulfur con-
tent of the burned fuel with the assumption
that all sulfur is oxidized to SO,. The values
are listed in Table 1. All mass concentrations
are corrected for standard conditions.
The measured BC mass concentration val-
ues are comparable with the carbon mass
concentrations derived from the smoke
number values (SN) of the International
Civil Aviation Organization (ICAO) for the
present engine. The corresponding carbon
mass concentrations are 0.22, 1.33, 6.3 and
9.28 mg m-"or 7, 30, 85 and 100% take-
off thrust (Schumann et al., 1996). SN mea-
surements by Huster (1995) behind the AT-
TAS aircraft gave smoke numbers 2.5, 5.1,
10.2 and 24.1, carbon concentrations of 0.20,
0.50, 1.22, and 3.43 mg m-"ith respect to
power settings 7, 18.5,30 and 57.5%. For the
conversion of SN into carbon mass concen-
trations the relation given by Hurley (1993)
was used.
Conclusions that can be drawn from the
mass concentration data are:
The BC as well as the TC mass concen-
trations are of comparable magnitude at dis-
tinct power settings for fuel with high-sulfur
and low-sulfur content. Hence, BC forma-
tion is almost independent from the fuel
sulfur content.
The BC fraction of TC is strongly affected
by combustion conditions. As can be seen in
Fig. 2 the BC to TC ratio varies from about
10% at 11% power setting to more than 80%
at 70% power setting. This finding corre-
sponds to the well-known fact that the BC
Jet Engine Exhaust Aerosol Characterization 67
Mass Concentration (mg m-3)
BC BC (opt) so2 SO;-
fraction increases with decreasing aidfuel
ratio, while especially at low power setting
the major fraction of carbonaceous aerosol
is emitted as unburned hydrocarbon com-
pounds. The obtained OC-BC split also sug-
gests that the carbonaceous aerosol that is
emitted by a jet engine at cruise power of
50% contains between 20% and 30% or-
ganic matter with respect to total carbon
mass. No explanation can be given for the
finding that the BCITC fraction always ap-
pears to be smaller in the low-sulfur fuel
case compared with the high-sulfur fuel case.
The overall conversion rate of SO, to par-
ticulate H2S04 seems to be almost indepen-
dent from the engine power setting. The
upper limit is 0.8% on a mass scale and 0.5%
on a number scale for plume ages <1 s. This
conversion rate is in good agreement with
estimated values as cited above, but it has to
be mentioned that these measurements are
restricted to particulate sulfuric acid. Fur-
thermore, the measurements cannot resolve
different processes that lead to the forma-
tion of particulate sulfate. Only the catalytic
oxidation of SO, at the surface of BC parti-
cles can be excluded. In Fig. 3 the abundance
ratios of SO:- to SO, and SO:- to BC are
plotted as a function of engine power setting.
Only a slight increase in ratio SO:- to SO,
from 0.4% to 0.5% with increasing power
setting is observed. However, the ratio of
SO:- to BC shows a strong decrease with
increasing power setting. In case sulfate for-
mation via oxidation of SO, on BC particles
has been an important path for sulfate for-
68 A. Petzold Aerosol Science and Technology
28:l January 1998

-0- Low sulfur

-0- High sulfur

Power setting in %
FIGURE 2. Black carbon (BC) fraction of total carbon (TC) as a function of engine power setting; low sulfur and
high sulfur correspond to a fuel sulfur content 6 ppm and 3000 ppm, respectively.

mation in a young exhaust plume, this ratio Mass Emission Indices

is expected to increase with increasing BC
mass concentration, i.e., with increasing The mass emission index of, e.g., BC, which
power setting (Dlugi et al., 1981; Mamane gives the mass of emitted BC per kg of con-
and Gottlieb, 1989). sumed fuel, is determined from the corre-

-0- SO, / BC
-0- SO, / SO,

0 10 20 30 40 50 60 70 80 90 100

Power setting in %
FIGURE 3. Abundance ratios of SO:-/SO, and SO$-IBC plotted as functions of engine power setting for a sulfur
fuel content of 3000 ppm.
Aerosol Science and Technology Jet Engine Exhaust Aerosol Charactcrization 69
28:l January 1998

TABLE 2. Mass emission indices of a turbofan engine Rolls RoyceISNECMA M45H Mk501 for species TC, BC and
SO:-; the values are given in gram per kilogram of consumed fuel
Mass Emission Index
Sulfur Content Power Setting Fuel Flow Core Speed Volume Flow (g kg-')
( P P ~ (%I (kg s-') (m S-') (m3 S-I) TC BC SO:-

sponding mass concentration cBc via the re- The mass emission indices of the measured
lation species as obtained by Eq. (4) with respect to
the mass concentrations from Table 1 are
summarized in Table 2.
In order to illustrate the almost linear
with the effective exit cross section of the correlation between power setting and emis-
engine A, = 0.125 m2, velocity v, at the sion of carbonaceous particles, the BC mass
engine exit and fuel flow m,. Values for the emission index EIBc is plotted as a function
core speed v, are between 80 m s p l and of power setting in Fig. 4. The correlation
357 m s-' for engine power settings 7% and coefficient is r = 0.97 for n = 7 data pairs
8596, respectively (Schumann, 1995). Inter- with a slope m = 0.01 g (kg %)-I. Again,
mediate v, values were obtained by interpo- this plot shows the similarity of burning low-
lation. The fuel flow m, was measured at sulfur fuel and high-sulfur fuel with respect
each power setting during the experiment. to BC emission. For cruise condition of

1.0 . I . I . I . I . I . , . I . I ~ I . -

0.9 -
0.8 -
0.7 -
0.6 - ,o 6 -
0.5 - -
0.4 - -
0 ,*'
0.3 - ,a* -
0.2 - -
,*' 0
Low sulfur -
0.1 - ,,,h 0 High sulfur -
0.0 ' " " " " " " " " " -

0 10 20 30 40 50 60 70 80 90 100

Power setting in %
FIGURE 4. Black carbon mass emission index EZBC (in grams BC per kilograms fuel) plotted as a function of engine
power setting, the dashed line corresponds to the linear regression line with parameters y = -0.05 (20.06) 0.0098 +
(20.001) x and correlation coefficient r = 0.97 for n = 7 data pairs.
70 A. Petzold
Power setting in %
FIGURE 5. Specific absorption coefficient of the black carbon aerosol at different engine power settings; the error
bars correspond to an estimated uncertainty of 20%.
about 50% power, a BC mass emission index
of 0.45 g kg-' can be assumed. In contrast to
the BC emission, the TC mass emission in-
dex varies only by a factor of less than 2
between 11% and 70% power. The mass
emission index of particulate sulfate is found
to be independent from the power setting.
This seems reasonable because the sulfate
formation is only related to the amount of
oxidized sulfur. Obviously, the latter is a
constant value with respect to a given mass
of burned fuel.
Optical Properties
With the procedure as described in the ex-
perimental section, the optical specific ab-
sorption coefficient of the emitted BC par-
ticles was determined from filter reflectance
data combined with thermal carbon mass
loading data. The results are presented in
Fig. 5. We found no significant dependence
of the specific absorption coefficient neither
from power setting nor from fuel sulfur con-
tent. The average value is 6 1 1 m2 &-'. This
specific absorption coefficient is twice as
high as the value for pure graphitic carbon
aerosol (3 m2 g-') obtained with the same
Aerosol Science and Technology
28: 1 January 1998
technique (Petzold and Niessner, 1995a).
The increased absorption efficiency can be
explained with a lower packing density of
combustion aerosol in comparison to pure
graphitic carbon aerosol. However, this
value is slightly lower than the generally
accepte-dl specffic absorption coefficient of
10 m g for vis~blehght, but this discrepancy
may be due to differences in the radiation
spectra between visible light (A = 0.55 pm)
and the incandescence lamp spectrum (A
0.8 pm) used for the reflectance analysis
-
method. The constant a,,,(BC) value is
confirmed by the finding, that the aethalo-
meter derived BC values that depend on the
absorptive properties of the BC particles,
too, are in good agreement with the BC
values from the thermal technique for all
power settings.
Size Distributions
Several particle-size distributions of the jet
engine exhaust aerosol were measured in-
side the exhaust plume of the ATTAS while
the Falcon was placed within about 200 m
behind on the runway. Figure 6 shows the
time series of accumulation mode particle
Aerosol Science and Technology Jet Engine Exhaust Aerosol Characterization 71
28: 1 January 1998

Take-off thrust

12.02 12.03 12.04 12.05 12.06

Decimal time
FIGURE 6. Time series of the total particle concentration behind the ATTAS aircraft at a distance of about 200 m;
indicated are the seauences that were used to determine size distributions of the background aerosol, the idle run
aerosol and the aerosol at take-off thrust.

concentrations as measured by the PCASP tribution. Additionally, the size distribution

(D, > 0.1 pm = N,,,) and the FSSP 300
(D,, > 0.3 pm = N,,,). Between 12.00 and
12.04 decimal time, engines were running at
idle mode. Distinct plumes of exhaust aero-
sol were drifting into the PCASP inlet in-
of the ambient aerosol was derived from the
sequences where no exhaust aerosol reached
the PCASP inlet. In Figs. 7a and 7b the size
distributions are shown for the idle run
mode and for the take-off thrust mode su-

(N,,, -
creasing the back round concentrations
3
2000 c m ) to about 5000-6000
cm-! When the engines of ATTAS were
pushed to take-off thrust (12.043) N l peak
concentrations exceeded 15,000 cm-! After
12.048, the Falcon itself accelerated and
took off 12-14 s behind ATTAS. During this
period the FSSP 300 provided N,,, concen-
trations around 600 cm-3 compared with
N,,, concentrations of about 5000 ~ m - ~ . a not necessarily aircraft-generated coarse
Whenever the ATTAS exhaust plume hit the
Falcon during the whole sequence beginning
at 12.00, the CN counter was saturated indi-
perpositioned on the background aerosol
size distribution. The interpretation of the
size spectra is straightforward. Both the idle
,run and the take-off thrust exhaust aerosol
consist of a log-normally distributed primary
soot mode. At take-off thrust an additional
mode at a larger diameter is observed that
may be formed by coagulation of the pri-
mary soot spheres inside the jet turbine, and
particle mode is also found. Count median
diameter (CMD), geometric standard devi-
ation ( G S D ) , and total number concentra-

prn = Nl,) well above lo5 cm- . I

cating total CN concentrations D, > 0.01 tion ( N ) of the model distributions are sum-
marized in Table 3. The differences in black
To obtain size distributions for different carbon mass concentration c,, with respect
engine thrust levels, the maximum values of to the values given in Table 1 for the ground
indicated idle run sequences were averaged test are due to dilution by ambient air en-
and taken as a representative idle run size trainment.
distribution, and the maximum values of the Figure 8 shows the particle size distribu-
take-off thrust sequence were averaged and tion measured in the exhaust plume of the
taken as a representative take-off thrust dis- ATTAS aircraft during Falcon take-off. The
72 A. Petzold Aerosol Science and Technology
28:l January 1998

Exhaust 0 Exhaust
Backgrounc - - - - - Backgrouns
Model -Model

I I
1021
0.1 1 10
Particle diameter Dp in pm Particle diameter Dp in pm

FIGURE 7a. Particle size distribution of the idle run
mode; shown are measured values (circles), back-
ground size distribution (dashed line) and size distri-
bution of the background aerosol plus primary soot
mode (straight line) with parameters CMD = 0.045
pm, GSD = 1.5 and N = 8 X lo5 ~ m - ~ .
FIGURE 7b. Particle size distribution of the take-off
thrust mode; shown are measured values (circles),
background size distribution (dashed line) and size
distribution of the background aerosol plus primary
soot mode with parameters CMD = 0.045 pm, GSD =
1.5 and N = 8 x lo5 ~ m - coagulated
~ , soot mode with
CMD = 0.18 pm, GSD = 1.42 and N = 2.5 X lo4 cm-"
and coarse particle mode with CMD = 0.56 pm, GSD =
1.65 and N = 1500 cm-3 (straight line).

distribution is comparable to that shown in with D, 1 pm show a liquid aerosol phase.

Fig. 7b as expected. A remarkable feature is
the equivalence of PCASP and FSSP 300
spectra in the size range of the primary and
the coagulated soot mode ( D , < 1 pm),
which indicates that the soot particles are
completely dry. Only coarse mode particles
The possible effects of coagulation growth
and hygroscopic behavior on the size spec-
trum are indicated in the figure. This submi-
cron spectrum may be taken as a represen-
tative size distribution for the dry exhaust
aerosol phase. The coarse mode is entrained

TABLE 3. Parameters CMD (count median diameter), GSD (geometric standard deviation), N (number concen-
tration), and c,, (black carbon mass concentration) of the log-normally distributed primary soot mode, the
coagulation mode and the coarse particle mode; values are given for the idle run exhaust aerosol and the take-off
thrust exhaust aerosol
Idle Run Take-off Thrust
Primary Soot Primary Soot Coagulated Soot Coarse Particle Mode

CMD ( ~ m ) 0.045 0.045 0.180 0.560

GSD 1.5 1.5 1.42 1.65
N (cm ') 8 X 105 8 x lo5 2.5 X lo4 1.5 X lo1
c,, (mg m-'9 0.120 0.120 0.200
Aerosol Science and Technology
28: 1 January 1998
, ,c
0.1 1 10
Particle diameter Dp in pm
FIGURE 8. Particle-size distribution inside the ex-
haust plume of the ATTAS aircraft; indicated are the
region of coagulated soot particles and hygroscopic
behavior of ambient aerosol particles; the straight line
corresponds to the model distribution composed of the
primary soot mode and the coarse particle mode with
same parameters as used in Fig. 7b, which are shown
both as dashed lines.
from ambient air via turbulent mixing during
take-off.
The idle run aerosol is dominated by the
primary soot mode (Fig. 7a), while the take-
off thrust aerosol is raised well above the
background throughout the whole size
range. Furthermore, the take-off size distri-
bution requires additional coagulation and
coarse particle modes to model the experi-
mental result (Fig. 7b). The primary soot
mode is equivalent for both types of aerosol
with its parameters in good agreement with
CMD values from 0.03 pm to 0.06 p m and a
geometric standard deviation of 1.6 as re-
ported by Hagen et al. (1994) for a jet ex-
haust aerosol. The coarse particle fraction of
the take-off thrust aerosol is assumed to be
entrained from ambient air, because the en-
gine exhaust at take-off thrust is a highly
turbulent plume moving along the runway
Jet Engine Exhaust Aerosol Characterization 73
with wind speeds well above 100 m s-l. As
this mode was not measured during flight in
the ATTAS exhaust plume, it will be ne-
glected in further discussions.
Using a density p = 1.5 g cm-"or loosely
packed BC agglomerates the mass concen-
tration c,, is derived from the number con-
centration N according to (Hinds, 1982)
P*
=N ----- [CMD exp(1.5 l n % ~ D ) ] "
6
(5
The mass concentrations obtained from Eq.
(5) for the primary soot mode and the coag-
ulated soot mode are listed in Table 3, too. A
comparison with the measured BC mass
concentrations of 0.25-0.28 mg m-%n the
idle run mode and 5.4-5.6 mg mp3 in the
take-off thrust mode gives dilution ratios of
2 and 20, respectively. Relating this emitted
carbon mass to the TC emissions instead of
BC emissions, gives an almost constant dilu-
tion ratio of 20 independent from the engine
power setting, which is less reasonable than
the BC values. Hence, the PCASP-measured
particles can be viewed as BC particles,
while the organic fraction that is dominating
the carbonaceous idle run aerosol by mass is
below the measuring range of the PCASP.
At maximum power 63% of total BC mass is
shifted from the primary mode to the coag-
ulation mode.
Finally, we attempted to determine the
BC particle emission index El,,,,, which is
the number of emitted particles per kilo-
gram of consumed fuel, from measured mass
concentrations and estimated particle size
distributions. For that purpose, the number
concentration N in Eq. (5) was scaled up
until the calculated mass concentration was
in agreement with the measured BC mass
concentration. Both modes of the take-off
thrust aerosol were scaled up equivalently.
The BC particle emission indices then were
calculated by introducing these number con-
centrations into Eq. (4). We obtained num-
ber concentrations of 1.8 x lo6 cm-%nd
1.5 X lo7 and emission indices Elp,,,
of 4 X 1014kg-' and 1.7 X 1015 kg-' in the
idle run case and the take-off thrust case,
74 A. Petzold
respectively. The particle emission indices
are in excellent agreement with data de-
duced from CN measurements behind the
ATTAS at cruise (2 x 1015kg-', Schumann
et al., 1996). Similar values were found for
the ER-2 stratospheric aircraft (Fahey et al.,
1995a), but the particle emission index is one
order of magnitude smaller than the emis-
sion index for nonvolatile particles of a high-
speed civil transport aircraft (Concorde) as
reported by Fahey et al. (1995b). The com-
parison with the Concorde emission indices
(EIP,,, < 9 X 1016 kg-'), which correspond
to an aircraft operating with Mach 2 in the
lower stratosphere at 16 km altitude, gives
rise to the interpretation that most of the
emitted nonvolatile particles of a jet engine
are small-sized BC particles.
SUMMARY AND CONCLUSIONS
The exhaust aerosol of a jet engine was char-
acterized using a set of techniques to mea-
sure mass concentrations of carbonaceous
matter and particulate sulfate, respectively,
and the particle size distribution. The ob-
served size distributions could be parameter-
ized by a primary BC mode around 0.045 pm
and a coagulated mode around 0.18 Fm. The
corresponding BC emission indices are
<0.6 g kg-' on a mass scale and <1.7 X 1015
kgp' on a number scale. These findings are
in agreement with reported exhaust aerosol
size distributions and emission indices. The
latter mode that occurred only at the high
engine power setting contained more than
60% of total BC mass. Additionally, the BC
aerosol inside the young exhaust plume was
found to be almost completely dry, which
agrees with the plume conditions of high
temperature and low relative humidity.
The conversion rate from SO, molecules
into particulate SO:- inside the young ex-
haust of <0.5% with only a slight depen-
dence on engine power setting is in agree-
ment with theoretical values based on the
conversion of SO, via O H oxidation and a
reaction of the formed SO, with H,O to
sulfuric acid. A formation of particulate sul-
furic acid via the catalytic oxidation of SO,
on the surface of the BC particles can be
Aerosol Science and Technology
28:1 January 1998
excluded, because no correlation between
sulfate and BC was observed.
The reported results allow a sufficient
characterization of the carbonaceous frac-
tion of a jet engine exhaust aerosol. How-
ever, the existence of gaseous H2S04 in the
young exhaust plume is still under discus-
sion. Our experiments cannot address this
question because our measurements were
restricted to particulate sulfate.
The authors are grateful to U. Schumann from DLR at
Oberpfajjenhofen for initiating the SULFUR 4 experiment
and to R. Busen, also from DLR, for the organization of
the experiment. We wish to thank R. Niesrner from the
Technical University of M~michfor providing the thermal
carbon analysis system to us, R. Ape1 for the sulfate mea-
surements, and S. Mahler for her assistance in the carbon
measurements. Both are also from the Technical Univer-
sity of Munich. The FSSP 300 and the PCASP were
provided by S. Bortmann from the University of Mainz
and R. Dlugifrom the University of Munich, who are abo
gratefully acknowledged.
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