Aerosol Science 35 (2004) 281299

www.elsevier.com/locate/jaerosci
A compact multistage (cascade) impactor for the
characterization of atmospheric aerosols
Philip Demokritou

, Seung Joo Lee, Stephen T. Ferguson,

Petros Koutrakis
Environmental Science and Engineering Program, Department of Environmental Health,
School of Public Health, Harvard University, 401 Park Drive, P.O. BOX 15677,
Landmark Center-West, Boston, MA 02215, USA
Received 18 February 2003; accepted 22 September 2003
Abstract
This paper presents the development, laboratory characterization, and eld evaluation of a compact multi-
stage cascade impactor (CCI). The CCI operates at a ow rate of 30 LPM and consists of eight impaction
stages equipped with rectangular slit-shaped acceleration nozzles. A 47 mm backup Teon membrane lter
is used downstream of the eighth stage to collect particles smaller than 0.16 m. In each stage, particles
are retained by impaction onto the inert polyurethane foam (PUF) substrate. The major feature of this novel
sampler is its ability to both fractionate by size and collect relatively large amounts of particles (mg quan-
tities) onto an inert polyurethane foam impaction substrates. Even though the impaction substrates are not
coated with adhesives such as grease or mineral oil, particle bounce and re-entrainment losses were found to
be insignicant. Impaction characteristics (cutpoint and sharpness of collection eciency curve) of the PUF
substrates are maintained for mass loadings of at least 25 mg, which is much higher than for other commonly
used rigid, at impaction substrates. The system was calibrated in laboratory experiments using polydisperse
aerosols. The 50% cutpoints of the eight stages were 9.9, 5.3, 3.3, 2.5, 1.7, 1.0, 0.47 and 0.16 m (aerody-
namic diameter), with pressure drops of 0.02, 0.02, 0.04, 0.06, 0.08, 0.27, 1.57 and 5.73 kPa. These pressure
drops are considerably lower than those obtained using at rigid impaction substrates with comparable cut-
points. Particle losses for each stage were less than 10% for particles smaller than 7 m and less than 20%
for particles larger than 7 m. The CCI was also compared with the collocated micro-orice impactor (MOI)
in laboratory-controlled experiments using articially generated polydisperse aerosol. These laboratory tests
showed that the mass concentrations measured by the MOI are considerably lower than those measured by
the CCI (the average ratio of total mass concentration of MOI to CCI was 0.86), with the size distribution
measured by the CCI closer to that measured using the real time particle sizing instruments (SMPS, APS).
A eld comparison of CCI, the Harvard impactor (HI) and the federal reference method (FRM) for ne

Corresponding author. Tel.: +1-617-3848847.

E-mail address: pdemokri@hsph.harvard.edu (P. Demokritou).
0021-8502/$ - see front matter ? 2003 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jaerosci.2003.09.003
282 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
particles showed a good agreement between the CCI and the reference samplers for particles smaller than
2.5 m.
? 2003 Elsevier Ltd. All rights reserved.
Keywords: Cascade impactor; Particle sampling; Collection eciency
1. Introduction
There is a great interest in investigating the toxicity of atmospheric particles through in vitro
cellular studies (Imrich, Ning, Koziel, Coull, & Kobzik, 1999; Soukup, Ghio, & Becker, 2000).
To adequately conduct these studies, it is necessary to collect relatively large amounts of ambient
particles (several mg). In addition, a major objective of particle toxicity studies is to investigate the
relative toxicity of the dierent particle size fractions. Previously used particle samplers have two
major shortcomings: rst, the collection capacity of the impaction substrate is limited, and; second,
they have extensive particle bounce-o and re-entrainment. In order to minimize particle bounce-o
and re-entrainment, impaction substrates are usually coated with adhesives such as mineral oil or
grease, both of which provide a signicantly limited loading capacity (John, Fritter, & Winklmayr,
1991; John & Sethi, 1993; Sehmel, 1980; Wall, John, Wang, & Coren, 1990). For reasonably small
amounts of collected particles, it was shown that the collection eciency of an impactor could
depend on the amount of particles collected on the impaction substrate (Pak, Liu, & Rubow, 1992).
Recently, we developed a new impaction substrate that does not require the use of adhesives
such as grease or mineral oil to minimize particle bounce-o and re-entrainment losses (US patent
#6, 435, 043 B1, 2002). This impaction substrate consists of polyurethane foam (PUF, density =
20 kg}m
3
, Merryweather foam, OH) and can be used to collect large quantities of particles (mg
amounts) while maintaining its impaction characteristics (cutpoint and sharpness of collection e-
ciency curve). Polyurethane foam is a porous polymeric material with stable physical characteris-
tics, low chemical background (when cleaned properly) and high collection eciency characteristics
(Kavouras, Ferguson, Wolfson, & Koutrakis, 2000; Salonen et al., 2000). The use of polyurethane
foam substrates improves the performance of inertial impactors, as compared to both coated and
uncoated at plate substrates (Demokritou, Kavouras, Ferguson, & Koutrakis, 2002a,b; Kavouras
et al., 2000; Kavouras & Koutrakis, 2001; Salonen et al., 2000). Since for the same nozzle geom-
etry and owrate, lower cutpoints can be achieved as compared to those for at plate substrates,
the pressure drop is substantially reduced for the same size cutpoint (Demokritou et al., 2002a,b;
Kavouras et al., 2000; Kavouras & Koutrakis, 2001). Recently, we have used the PUF substrate in
the development of a high volume cascade impactor (Demokritou et al., 2002a,b) and the high vol-
ume low cutpoint impactor (Kavouras et al., 2000). These two methods have been used extensively
to characterize the physicochemical and toxicological properties of atmospheric aerosols.
In this paper, we present the development and evaluation of the compact cascade impactor (CCI)
that utilizes the PUF foam as the collection medium. This system consists of eight impaction stages,
equipped with rectangular nozzles. The major feature of the CCI is its ability to fractionate aerosols
by size and collect large amounts of particles onto small, inert impaction substrates without the use
of adhesives.
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 283
2. Methods
2.1. Design considerations
According to impaction theory, the dimensionless Stokes number, Stk, is the governing parameter
for impaction and is dened as follows:
Stk =
j
p
d
2
p
UC
c
9jW
, (1)
where j is the dynamic viscosity of the air, d
p
is the diameter of the particle, j
p
is the particle
density, W is the nozzle diameter, U is the jet velocity and C
c
is the Cunningham slip correction
factor. The slip correction factor is given by (Hinds, 1999)
C
c
= 1 +
Kn
2
(2.34 + 1.05e
0.195Kn
), (2)
where Kn is the dimensionless Knudsen number, 2z}d
p
, dened by the ratio of two times the mean
air molecule free path (z) to the particle diameter (d
p
).
2.2. Description of the compact cascade impactor (CCI)
A fully assembled compact cascade impactor (CCI) and its internal parts are shown in Fig. 1. The
sampling device consists of eight impactor stages and an after lter. The CCI is compact (50 cm H
and 11 cm O.D.), and is relatively lightweight (3.5 kg). Each stage consists of a slit-shaped accel-
eration nozzle and a rectangular polyurethane foam (PUF) impaction substrate (density =20 kg}m
3
,
Merryweather Foam, OH). The PUF substrates are easily inserted and removed from a substrate
base (Fig. 1), and securely transported to a laboratory for gravimetric or chemical analysis. The
acceleration nozzle width and length dimensions are shown in Table 1. The optimal thickness of the
polyurethane foam for all stages is 0.64 cm, which assures that particles do not penetrate through
the PUF to the substrate holder.
Ultrane particles (less than 0.16 m) are collected on a 47 mm diameter 2 m pore Teon mem-
brane lters (Cat. No. R2PJ047, Pall Life Sciences, Ann Arbor, MI). This lter material was previ-
ously characterized in our lab and has both a high collection eciency and a relatively low-pressure
drop (Demokritou et al., 2002a,b). Other lter materials such as polypropylene ber (Monadnock,
Grade 5300) can also be used to collect the ultrane particles.
2.3. Laboratory performance characterization of CCI
The experimental setup used for the laboratory performance characterization of the system is
shown schematically in Fig. 2. The apparatus consists of two major components: (1) the particle
generation system, and (2) the particle sampling and monitoring system. Due to the wide range of
CCI cutpoints, two dierent techniques were employed to generate and measure the polydisperse
particles for the calibration of the various stages.
284 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
Fig. 1. The compact cascade impactor (CCI).
2.3.1. Aerosol generators
(1) For the 0.011.0 jm size range: the polydisperse aerosol generator for the 0.011.0 m size
range is shown in Fig. 2. An aqueous solution of sodium chloride (NaCl) was atomized using
a collision-type atomizer (TSI model 3076). All the generated particles were drawn through the
dilution chamber (volume of 1.15 10
2
m
3
) with dry, particle-free room air. After dilution, the
mixed stream was drawn though the diusion dryer (TSI, model 3062) and then passed through a
Kr-85 neutralizer (TSI model 3012) to stabilize the particle electrostatic charge.
(2) For the 1.020.0 jm size range: the aerosol generator for the 1.020.0 m size range is
also shown in Fig. 2. It uses an aqueous suspension of either hollow glass spheres (nominal size
220 m, density = 1.10 g}cm
3
Polysciences, PA) or solid glass spheres (nominal size
310 m, density = 2.48 g}cm
3
Polysciences, PA). A suspension of approximately 1.0 g of glass
beads per 200 ml of distilled water was continuously mixed with a magnetic stirrer, and aerosolized
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 285
Table 1
Physical characteristics, ow parameters, and experimental results of CCI
Stage no. 1 2 3 4 5 6 7 8
Physical characteristics
Acceleration nozzle W (cm) 0.432 0.236 0.160 0.137 0.094 0.058 0.058 0.028
L (cm) 7.19 7.01 6.32 5.92 5.59 5.00 1.78 1.91
S}W 1.0 1.0 1.0 1.0 1.0 1.0 1.0 2.0
Substrate Width length 1.8 8.1 1.8 8.1 1.0 6.4 1.0 6.4 0.64 6.4 0.64 6.4 0.64 6.4 0.64 6.4
(cm)
Material PUF PUF PUF PUF PUF PUF PUF PUF
Flow parameters
Re 926 950 1053 1125 1191 1330 3744 3495
U (m/s) 1.6 3.0 4.9 6.2 9.5 17.1 48.1 93.9
Experimental results
d
50
(m) 9.9 5.3 3.3 2.5 1.7 1.0 0.47 0.16

Stk 0.47 0.47 0.46 0.43 0.44 0.47 0.39 0.32

o 1.38 1.33 1.32 1.38 1.33 1.43 1.81 1.74
P (kPa) 0.02 0.02 0.04 0.06 0.08 0.27 1.57 5.73
Note. W, nozzle width; L, nozzle length; S, substrate-to-nozzle distance; Re, Reynolds number; U, nozzle air velocity;
d
50
, 50% cutpoint;

Stk, square root of Stokes number; o, collection eciency curve sharpness; P, pressure drop.
using a nebulizer (Retec Model X-70/N, with air pressure at 7 psi) and then dried and diluted using
dry, particle-free room air.
2.3.2. Particle sampling and monitoring system
The output of the aerosol generator passed into the top of a cylindrical anodized aluminum dilution
tube (120 cm H5.08 cm O.D.). Supplemental air was drawn in through a HEPA lter at the top of
the dilution tube. To assure aerosol mixing inside the tube, a round plate was placed inside the tube
downstream of the input ows. Each stage of the CCI was evaluated separately. Each impaction stage
was mounted inside the dilution tube, one at the time, as shown in Fig. 2. Particle concentrations were
measured for one minute durations using isokinetic sampling probes, alternating between upstream
and downstream of the sampler. The alternating measurements were repeated at least ve times to
ensure adequate precision. The upstream sampling port was placed approximately eight-duct diameters
downstream from the duct entrance. The downstream sampling port was similarly placed on a second
duct connected to the outlet of the impaction system. The reproducibility of the measurements was
5%. An aerodynamic particle sizer (APS, TSI Model 3310) and a scanning mobility particle sizer
(SMPS, TSI Model 3080) were used to measure particles with diameter from 0.5 to 20 m and
from 0.01 to 1.0 m, respectively. Particle losses for each impaction stage were measured using the
tested impaction stage without the impaction substrate in place.
For the SMPS data, each particle size interval was converted from mobility equivalent diameter
to aerodynamic diameter. Assuming that the mobility equivalent diameter is equal to the equivalent
286 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
Silica Gel
HEPA
Filter
2 LPM
Mixing Chamber
TSI 3012
Kr-85 Neutralizer
TSI 3062
Diffusion Dryer
NaCl Solution
TSI 3076
Constant Output
Atomizer
Silica
Gel
HEPA
Filter
35 psi
7 psi
HEPA Filter
Mixing Chamber
HEPA
Filter
Silica
Gel
Excess
fluid
Nebulizer
Bubbling
Air
Glass bead
suspension
PUMP
PUMP
PUMP
PUMP
PUMP
PUMP
Supplemental
Filtered Air
PARTICLE SAMPLING & MONITORING
TEST AEROSOL GENERATOR FOR SIZE
RANGE 1 - 20 m
TEST AEROSOL GENERATOR FOR SIZE
RANGE 0 - 1 m
Pressure
Gauge
29.7 or 25.0 LPM
HEPA
Filter
Flowmeter
PUMP
Pressure
Gauge
SMPS / APS
Isokinetic Sampler
Isokinetic Sampler
Impactor
stage
0.3 or 5.0 LPM
Magnetic
Stirrer
HEPA
Filter
Fig. 2. Experimental setup for laboratory characterization of CCI.
volume diameter (Kasper, 1982), the conversion was made using (Peters, Chein, & Lundgren, 1993)

C
a
d
a
=

j
p
C
m
j
o
,
d
m
, (3)
where d
a
is aerodynamic diameter, d
m
is the mobility equivalent diameter, C
a
is the slip correction
factor for the aerodynamic diameter, C
m
is the slip correction factor for the mobility equivalent
diameter, , is the dynamic shape factor, j
p
is the density of the particle, and j
0
is the unit density
(1 g}cm
3
). For sodium chloride particles, the dynamic shape factor and particle density were assumed
to be , = 1.08 (that of a cube) and 2.2 g}cm
3
, respectively.
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 287
The collection eciency for a given particle size, E(d
a
), for each impaction stage, was calculated
using
E(d
a
) =
C(d
a
)
1(d
a
)
=
1(d
a
) P(d
a
)
1(d
a
)
, (4)
where 1(d
a
), C(d
a
) and P(d
a
) are the total, collected and penetrated particles of aerodynamic
diameter of d
a
, respectively. The collection eciency data were tted using the Boltzmann sigmoidal
algorithm (Origin, MicroCal Software Inc.) using
E(d
a
) =
A
1
A
2
1 + e
(d
a
x
0
)}dx
+ A
2
, (5)
where x
0
is the median aerodynamic diameter; dx is the width of the tting; and A
1
and A
2
, are the
coecients determined by the algorithm. The sharpness (o) of the collection eciency curve was
calculated using
o =

d
84.1
d
15.9
, (6)
where d
84.1
and d
15.9
are the sizes of particles having collection eciencies of 84.1% and 15.9%,
respectively (Hinds, 1999).
2.4. Particle loading capacity experiment
In conventional impactors, a known limitation is the collection eciency change as a function of
the deposited on the impaction substrate particles. This eect may introduce a signicant sampling
artifact and thereby cause an unacceptable reduction in the useful duration of sampling. Previous
investigations of the eect of particle loading on the commonly used at surface impaction substrates
showed that signicant changes occur for both particle bounce and cuto diameter, even for particle
loading of less than 1.0 mg (Kenny, Gussmann, & Meyer, 2000; Misra, Singh, Shen, Sioutas, &
Hall, 2002; Tsai & Cheng, 1995; Turner & Hering, 1987).
Experiments were performed to investigate the eect of substrate particle loading on the collection
eciency curve. Stage no. 4 (50% cutpoint: 2.5 m) was selected to investigate the loading eect on
PUF. As the loading was built up over time on the substrate, consecutive particle number concentra-
tions were measured up- and down-stream of the sampler (see Fig. 2). Particle collection eciency
was calculated based on Eq. (4) as a function of loaded mass on the PUF substrate. Loaded mass,
M, on the substrate was calculated using
M =
m

)
n

i
N
i, )
e
i, )
j
p
d
3
p
i
6
, (7)
where, i is the ith number of n channels in APS, ) is the )th minute, N
i)
is the upstream par-
ticle number, e
i)
is the collection eciency, j
p
is the particle density, and d
p
is the particle
diameter.
288 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
TSI 3400A Fludized Bed
Aerosol Generator
SMPS / APS
TEST AEROSOL GENERATOR FOR SIZE
RANGE 1 - 20 m
PUMP Silica
HEPA
35 psi
30.0 LPM
140.0 LPM
30.0 LPM
HEPA
CCI
PUMP
TSI 3062
Diffusion Dryer
TEST AEROSOL GENERATOR FOR SIZE
RANGE 0-1m
NaCl Solution
TSI 3076
Constant Output
Atomizer
Dry & filtered air
35 psi
Mixing Chamber
Dry& filtered air
TSI 3012
Kr-85 Neutralizer
60.0 LPM
Mixing Duct
Supplemental
Filtered Air
SAMPLING SYSTEM
MOI
PUMP
PUMP
Fig. 3. Laboratory intercomparison experimental setup.
2.5. Laboratory intercomparison experiments
Laboratory experiments were conducted to compare the size distribution measured by both the
microorice impactor (MOI, MSP Corporation, Minneapolis, MN) and by the CCI, with that obtained
using real time instrument measurements (SMPS, APS). The experimental setup for these experiments
is shown in Fig. 3. In order to simulate the bi-modal size distribution of atmospheric aerosols,
two separate aerosol generators were used in parallel to generate polydisperse aerosols in the 0
20 m size range. Fine Test Dust (FTD, Powder Technology Inc., Burnsville, MN) and NaCl were
used as the test aerosols. FTD was dried over 24 h prior its use in a temperature of 50

C and
aerosolized using a Fluidized Bed Aerosol Generator (TSI Model 3400A). An aqueous solution
of sodium chloride (NaCl) was atomized using a Collision type atomizer (TSI model 3076) as
outlined above, in the impactor characterization experiments. The mixture of aerosolized FTD and
NaCl was then passed through the Kr-85 Neutralizer to reduce the particle charge to close to the
Boltzmann equilibrium distribution. The aerosol was then introduced into a circular aluminum tube
(ID=5.08 cm). Isokinetic probes were placed at a distance of more than 10 times of tube diameter
to sample aerosol for both the cascade impactors and the real time instruments (SMPS/APS).
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 289
MOI operates at 30 LPM and was used to classify particles in the following size intervals:
60.175, 0.1750.56, 0.561.0, 1.01.8, 1.83.2, 3.25.6, 5.610 and 10 m, using 37 mm Teon
membrane lters (Cat. No. R2PJ037, Pall Life Sciences, Ann Arbor, MI) as impaction substrates.
Sample duration for both cascade impactors was 90 min. Tests were conducted using both a rela-
tively high particle concentration of about 5.0 mg}m
3
and a relatively low concentration of about
0.4 mg}m
3
. At the end of each run, PUF substrates, the 47 mm Teon after-lter of CCI, and
37 mm Teon lers of MOI were equilibrated over a 48-h period in a temperature and relative
humidity-controlled room (40 5% RH and 21 2.8

C). Just prior to gravimetric analysis both

the lters and the PUF substrates were exposed to
210
Po ionizing units (Staticmaster Model 2U500,
NRD Inc., Grand Island, NY) for more than 10 s, to minimize eects of electrostatic charge. For all
samples, 100% replicate weighing was performed both before and after sampling, with a third weigh-
ing done when the rst two was not within 5 g. This procedure was implemented to improve
the precision of the gravimetric analysis and to exclude outliers (Allen, Oh, Koutrakis, & Sioutas,
1999). Average particle concentrations were also calculated based on the real time data obtained by
the collocated APS and SMPS.
2.6. Field study
For the intercomparison study to measure the particulate ne mass (PM
2.5
), two conventional
Harvard PM
2.5
impactors (HI; Marple, Rubow, Turner, & Spengler, 1987), and a PM
2.5
Federal
Reference Method impactor (FRM, Rupprecht and Patashnick, Albany, NY) were collocated with
the CCI system on the roof of Harvard Countway Library in Boston, MA. Samples were collected
during the month of September 2002, with durations of 48 h. Initial and nal sampler ows for the
samplers were measured with calibrated rotameters (Matheson, East Rutherford, NJ).
The PM
2.5
HI collects particles on 37 mm Teon membrane lters (Pall Life Sciences, Ann Arbor,
MI) at 10 LPM, while the FRM uses a 47 mm lter operating at 16.7 LPM. Final weighing was
done within 10 days after sampling, following EPA guidelines, as described above.
3. Results and discussion
3.1. Impactor characterization experiments
The collection eciency curves for each of the eight cascade impactor stages are shown in
Fig. 4. The experimentally calculated cutpoints (d
50
, m), the collection eciency sharpness (o)
and pressure drop (P, kPa) are also presented in Table 1.
As expected, the experimentally determined cutpoints and

Stk values of the porous impaction
substrates are smaller than the theoretically calculated value for a at rigid surface impaction sub-
strate, assuming a

Stk value at 0.7. This cutpoint decrease was experimentally conrmed for both
rectangular and round nozzles and was presumed to be due to the penetration of some air stream-
lines into the porous polyurethane foam surface (Kavouras et al., 2000; Kavouras & Koutrakis,
2001). Huang and Tsai (2003) also showed that this is due to the penetration of air into PUF
causing a higher inertial force for particles near the surface of the porous PUF than that of the at
substrate. The same results were reported in theoretical/experimental investigations (Huang & Tsai,
290 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
Aerodynamic particle diameter (m)
0.1
1
10
C
o
l
l
e
c
t
i
o
n

e
f
f
i
c
i
e
n
c
y
,

%
0
10
20
30
40
50
60
70
80
90
100
5 2 6 8 7 4 3 1
Fig. 4. Collection eciencies as a function of aerodynamic diameter for each stage of CCI.
2003; Huang, Tsai, & Shih, 2001). This shows that for the same nozzle geometry and owrate,
lower cutpoints can be achieved as compared to at rigid substrates, and therefore, the pressure drop
is substantially reduced for the same cutpoint (Demokritou et al., 2002a,b; Kavouras et al., 2000;
Kavouras & Koutrakis, 2001).
Table 1 summarizes the characterization of critical parameters for each stage of the CCI. These
include the cutpoint, the

Stk, the collection eciency curve sharpness (o), and the pressure drop
across the stage. For all stages, the o values are adequate to assure good separation of particles larger
than the cutpoint from the airstream (Fig. 4). Even for the lowest cutpoint (stage 8), the pressure
drop is quite low (5.73 kPa), and is signicantly lower than that of impactors that use at rigid
impaction substrates (for the same cutpoint), and thus minimizes losses of semivolatile components
from collected atmospheric particles (Kelly et al., 1994).
Fig. 5 shows the combined particle losses for all eight stages (based on measurements for each
individual stage) as a function of the particle aerodynamic diameter. Inertial particle losses within the
CCI may be caused by the turbulent ow in the acceleration nozzle region, at ow turns, and at the
ow exit/entrance between stages. Particle losses inside each stage were determined by measuring
particles up- and down-stream each stage, with the substrate removed. It is important to note that the
collection eciencies for each stage (see Fig. 4) include particles collected on both the impaction
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 291
Aerodynamic particle diameter (m)
0.1 1 10
P
a
r
t
i
c
l
e

L
o
s
s
,

%
0
10
20
30
40
50
60
70
80
90
100
3 4 5 6 7 8 1
Stage Number (cutpoint)
2
Fig. 5. Interstage particle losses as a function of aerodynamic diameter.
substrate and particles lost on stage walls and acceleration nozzle. Coarse particle (2.510 m) losses
increased from 5% for 4 m particles, up to 20% for particles with diameter larger than 8 m. Fine
particle (2.5 m) losses are minimal (less than 5%). Particle losses in the last stage (0.16 m)
were higher (about 10%), due to the increased diusional deposition of these small particles. Similar
results were previously reported for other cascade impactors (Demokritou et al., 2002a,b; Kavouras
et al., 2000; Marple, Rubow, & Behm, 1991).
3.2. Particle loading experiments
Fig. 6 summarizes the experimental results of particle loading eect on the impaction characteristics
of PUF. Fig. 6(a) shows the change of cut-o diameter (d
50
), as a function of loaded mass on PUF
(for stage 4, with a cutpoint of 2.5 m). The cutpoint increased from 2.5 to 2.6 and 2.7 m, for
10.9 and 24 mg of loaded mass, respectively. These mass loadings correspond to 121 and 264 h,
respectively, of sampler operation at an average ambient PM
2.5
concentration of 50 g}m
3
(or 48 h
at 126 and 276 g}m
3
, respectively). This should be considered a negligible eect on the cutpoint,
compared to the eect when using an oiled at substrate, for which the d
50
decreased from 2.45
to 2.25 m (about 8.2% decrease from the initial cutpoint) for a particle loading of only 1.5 mg
(Kenny et al., 2000).
Fig. 6(b) presents the collection eciency as a function of particle mass loading for particle
sizes of 9.7 and 1.7 m, which represents particles signicantly larger and signicantly smaller than
the cutpoint (d
50
= 2.5 m), respectively. The collection eciencies for the 9.7 m particle remain
unchanged and close to 100% for loading up to about 25 mg. This is an indication that there is
negligible particle bounce and re-entrainment, which is usually more pronounced for large particle
292 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
Loaded mass, M (mg)
0 5 10 15 20 25
d
5
0
(

m
)
1.50
1.75
2.00
2.25
2.50
2.75
3.00
3.25
3.50
Change of d
50
Loaded mass, M (mg)
0 5 10 15 20 25
C
o
l
l
e
c
t
i
o
n

e
f
f
i
c
i
e
n
c
y

(
%
)
0
10
20
30
40
50
60
70
80
90
100
da = 9.7 m
da = 1.7 m
(a)
(b)

Fig. 6. Particle loading test for an impaction stage of 30 LPM CCI (d

50
=2.5 m). (a) Change of 50% cut-o aerodynamic
diameter vs. loaded mass. (b) Collection eciency vs. loaded mass for d
a
= 1.7 and 9.7 m, respectively.
sizes. This conrms that the PUF substrate maintains its ability to minimize particle bounce even
with relatively high loading conditions. It is worthwhile to point out that also for a greased coated
impaction substrate, particle bounce became signicant for a particle mass loading of only about
1 mg, due to a change in the impaction surface characteristics (Tsai & Cheng, 1995). Similarly,
for the particle size smaller than the cutpoint (1.7 m), the collection eciency was relatively low
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 293
Table 2
Laboratory comparison of the particulate mass collected with the MOI, the CCI and SMPS/APS
Test MOI stage size range (m) and collected mass (mg) Total
collected
0.175 0.1750.56 0.561.0 1.01.8 1.83.2 3.25.6 5.610 10 mass (mg)
High loading 0.564 0.757 1.023 2.571 2.871 1.366 0.168 0.031 9.35
Low loading 0.067 0.119 0.134 0.245 0.311 0.118 0.017 0.001 1.013
Test CCI stage size range (m) and collected mass (mg) Total
collected
0.16 0.16 0.47 0.471.0 1.01.7 1.72.5 2.5 3.3 3.35.3 5.39.9 9.9 mass (mg)
High loading 0.452 0.491 0.795 1.228 2.132 2.03 2.533 1.859 0.352 11.871
Low loading 0.061 0.068 0.090 0.117 0.178 0.149 0.325 0.098 0.000 1.085
Test SMPS/APS size range (m) and collected mass (mg) Total
collected
0.16 0.160.47 0.471.0 1.0 1.7 1.7 2.5 2.53.3 3.35.3 5.39.9 9.9 mass (mg)
Low loading 0.014 0.073 0.076 0.097 0.174 0.206 0.242 0.080 0.001 0.964
(approximately 20%) and also remained unchanged with loading, an indication that there is no
signicant distortion of the collection eciency curve in general.
This superior performance of this porous substrate (PUF) in terms of loading capacity is most
likely due to the lack of formation of a hummock-like deposit during particle loading on the
surface, which is a distinctive feature for rigid, at impaction substrates. In this case, the particles
are deposited inside the pores of the foam, resulting in a much larger holding capacity.
3.3. Comparison of CCI and MOI and real time methods
Table 2 summarizes the results from the laboratory comparison of the MOI, the CCI and the
real time instruments (SMPS/APS) for both relatively high (about 10 mg) and relatively low (about
1 mg) total collected mass. Fig. 7 shows the mass size distributions measured by all three methods,
for the low total concentration conditions. It is obvious that the size distribution obtained from
the CCI measurements agrees well with that of the real time instrumentation (SMPS/APS), while
the MOI measurements do not show as a good agreement. The MOI measurements indicate lower
coarse particle concentrations, and higher ne particle concentrations than the other two methods. A
previous study showed that particle bounce of coarse particles occurs in the MOI stages when using
Teon membrane lters as impaction substrates (Marple et al., 1991). The results observed here are
consistent with bounce-o the coarse particles from the upper MOI stages, which are then collected
downstream on the ne particle stages. Similar ndings were found for the high concentration test,
an indication that particle bounce of coarse particles can occur with the MOI, for both high and low
ambient total particle concentrations.
294 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
Aerodynamic Diameter (Dp), m
0.1 1 10

M
a
s
s

C
o
n
c
e
n
t
r
a
t
i
o
n
/

l
o
g
(
D
p
)
,

g
/
m
3
0.0
5.0
10.0
15.0
20.0
25.0
Compact Cascade Impactor
MOI
SMPS/APS data
Fig. 7. Laboratory intercomparison of the particulate mass concentration measured with the MOI, the CCI, and the
SMPS/APS at low loading particle concentration.
The ratio of MOI to CCI mean total mass collected was 0.79 and 0.93 for the high and low-
concentration tests, respectively. One possible reason for these results is that multiple nozzles of
the MOI impaction stages are expected to have higher wall losses by diusion than the single slit
nozzles of the CCI stages. It is likely that the presumably higher amount of particle bounce for
the higher concentration test was one reason why there was a smaller ratio of MOI to CCI to-
tal mass for this experiment. Visual observation also indicated that there was signicant particle
deposition on the walls and the multiple nozzles of the MOI. It is also possible that use of an un-
coated substrate (Teon membrane lter) for the MOI contributed to the dierences between the two
samplers. This would be in agreement with the ndings of higher wall and nozzle losses, when un-
coated impaction substrates were used, as reported by Sioutas, Chang, Kim, Koutrakis, and Ferguson
(1999).
3.4. Field study results
PUF is a porous material, and is known to absorb varying amounts of water vapor from the air,
with increasing absorption for increasing relative humidity. In order to investigate the weight change
of the PUF as a function of the relative humidity in the RH- and temperature-controlled balance
room, ve laboratory blank substrates (for each of the three substrate sizes used by the CCI) were
weighed daily for 1 week. It was shown that a mean of 0.17% mass dierence occurred for the
largest (5%) dierence in relative humidity (RH). For a 48-h sampling period, this corresponds to
4.1, 1.8 and 1.0 g}m
3
, for nominal PUF masses of 104, 46, and 25 mg, respectively. To correct
eld test substrates for the eects of relative humidity, laboratory blanks were used. The dierence
in mass for each eld test substrate, before and after sampling, was adjusted to take into account
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 295
Table 3
Mean concentration, precision, limit of detection (LOD), and coecient of variation (CV) for CCI
Stage No. of sample (n) Mean conc. (g}m
3
) Precision (g}m
3
) LOD (g}m
3
) CV
1 18 5.72 0.59 1.62 0.10
2 18 5.67 0.60 1.62 0.11
3 18 3.41 0.29 1.10 0.09
4 18 1.92 0.21 1.10 0.11
5 18 1.16 0.18 0.49 0.15
6 18 1.26 0.22 0.49 0.18
7 18 2.54 0.33 0.49 0.13
8 18 2.96 0.71 0.49 0.24
changes in the corresponding blanks. No humidity eects were observed for the Teon lters used
for the impaction stages of the MOI and the back-up lter of the CCI.
The limit of detection (LOD), precision, and coecient of variation (CV) were also calculated for
the PUF substrates of each stage. LOD was calculated based on three times the standard deviation
of mass value for the eld blanks. Precision was obtained as the root mean square (RMS) dierence
for the paired values of CCI, divided by

2. CV was calculated as the precision divided by the
mean concentration. The LOD, precision, CV values of every stage are shown in Table 3. The mean
ambient concentrations of each stage in Boston were all higher than the LOD values.
The particle mass concentration, as a function of the aerodynamic diameter for the CCI, for two
representative sampling periods, were plotted in Fig. 8. The size distributions are both bimodal which
is typical for the Boston area (Long, 2000). Figs. 9(a) and (b) show good agreement between the
PM
2.5
mass measurements for the CCI vs. the HI and the FRM, respectively. PM
2.5
concentrations
for the CCI were calculated using the sum of the mass concentrations for the 5th, 6th, 7th, and 8th
stages, and the backup lter.
4. Summary and conclusion
A 30 LPM compact eight stage-cascade impactor (CCI) was developed and evaluated. This sys-
tem measures particle sizes between 10 and 0.16 m, with a backup lter to collect the remaining
ultrane particles, and has a total pressure drop of about 8.0 kPa. This relatively low-pressure drop
signicantly reduces the potential for volatilization losses of semi-volatile particle components. The
polyurethane foam used for the impaction substrates results in insignicant particle bounce-o and
re-entrainment, without using adhesives such as grease or mineral oil as coatings. Interstage losses
of ultrane and ne particles were less than 10% and were less than 20 for coarse particles. The
system adequately maintained its impaction characteristics for a loading of up to 25 mg, which is
signicantly better than the performance of other cascade impactors that use at, rigid substrates.
The compact cascade impactor was also evaluated in a laboratory and eld study and compared
with the microorice impactor (MOI), Harvard impactor (HI) and the Federal reference method
(FRM) for ne particles. The average CCI collected mass was found to be higher than that of
the MOI. The dierence is most likely due to the particle bounce-o from the uncoated impaction
296 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
Aerodynamic Diameter (Dp), m
0.1 1 10

M
a
s
s

C
o
n
c
e
n
t
r
a
t
i
o
n
/

l
o
g
(
D
p
)
,

g
/
m
3
0
5
10
15
20
25
Sep. 23 - 25, 2002
Aerodynamic Diameter (Dp), m
0.1 1 10

M
a
s
s

C
o
n
c
e
n
t
r
a
t
i
o
n
/

l
o
g
(
D
p
)
,

g
/
m
3
0
5
10
15
20
25
Sep. 25 - 27, 2002
Fig. 8. Mass size distribution measured by CCI in Boston.
substrates and the increased wall and nozzle particle losses for the MOI. The size distribution
obtained by CCI agrees well with that of the real time instrumentation (SMPS/APS). The eld study
results show good agreement between the CCI and the two reference methods (HI and FRM) for
PM
2.5
mass concentration.
P. Demokritou et al. / Aerosol Science 35 (2004) 281299 297
HI PM
2.5
Concentration (g/m
3
)
0 2 4 6 8 10 12 14 16 18 20 22
C
C
I

P
M
2
.
5

C
o
n
c
e
n
t
r
a
t
i
o
n

(

g
/
m
3
)
0
2
4
6
8
10
12
14
16
18
20
22
Data
1 : 1
Regression
CCI=1.05*HI-1.48
r
2
=0.92
FRM PM
2.5
Concentration (g/m
3
)
0 2 4 6 8 10 12 14 16 18 20 22
C
C
I

P
M
2
.
5

C
o
n
c
e
n
t
r
a
t
i
o
n

(

g
/
m
3
)
0
2
4
6
8
10
12
14
16
18
20
22
Data
1 : 1
Regression
CCI=1.17*FRM-0.08
r
2
=0.97
(a)
(b)
Harvard Impactor vs. CCI
FRM vs. CCI
Fig. 9. Intercomparison between CCI, HI, and FRM for PM
2.5
mass concentrations during eld study in Boston.
Acknowledgements
The laboratory performance evaluation of the sampler was supported by the EPA/Harvard Particle
Health Eects Center (EPA Grant No. R827 353-01-0) and the NIEHS Harvard Center (NIEHS
Grant No. ES00002).
298 P. Demokritou et al. / Aerosol Science 35 (2004) 281299
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