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    Aerosol Science 35 (2004) 281299

    www.elsevier.com/locate/jaerosci

    A compact multistage (cascade) impactor for thecharacterization 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 novelsampler 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: [email protected] (P. Demokritou).

    0021-8502/$ - see front matter? 2003 Elsevier Ltd. All rights reserved.doi:10.1016/j.jaerosci.2003.09.003

    mailto:[email protected]:[email protected]
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    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 therelative 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=m3, 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.

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    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=pd

    2pUCc

    9W; (1)

    where is the dynamic viscosity of the air, dp is the diameter of the particle, p is the particle

    density, W is the nozzle diameter, U is the jet velocity and Cc is the Cunningham slip correction

    factor. The slip correction factor is given by (Hinds, 1999)

    Cc = 1 + Kn2

    (2:34 + 1:05e0:195Kn); (2)

    where Kn is the dimensionless Knudsen number, 2=dp, dened by the ratio of two times the mean

    air molecule free path () to the particle diameter (dp).

    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=m3,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.

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    Fig. 1. The compact cascade impactor (CCI).

    2.3.1. Aerosol generators

    (1) For the 0.011.0 m 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 usinga collision-type atomizer (TSI model 3076). All the generated particles were drawn through the

    dilution chamber (volume of 1:15 102 m3) with dry, particle-free room air. After dilution, themixed 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 m size range: the aerosol generator for the 1.0 20:0 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=cm3 Polysciences, PA) or solid glass spheres (nominal size

    310 m; density = 2:48 g=cm3 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

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    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

    d50 (m) 9.9 5.3 3.3 2.5 1.7 1.0 0.47 0.16Stk 0.47 0.47 0.46 0.43 0.44 0.47 0.39 0.32

    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;

    d50, 50% cutpoint;

    Stk, square root of Stokes number; , 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 usingdry, 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 ofthe 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 toensure 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

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    Silica Gel

    HEPAFilter

    2 LPM

    Mixing Chamber TSI 3012Kr-85 Neutralizer

    TSI 3062Diffusion Dryer

    NaCl Solution

    TSI 3076Constant OutputAtomizer

    SilicaGel

    HEPAFilter

    35 psi

    7 psi

    HEPA Filter

    Mixing Chamber

    HEPAFilter

    SilicaGel

    Excess

    fluid

    Nebulizer

    BubblingAir

    Glass beadsuspension

    PUMP

    PUMP

    PUMP

    PUMP

    PUMP

    PUMP

    SupplementalFiltered Air

    PARTICLE SAMPLING & MONITORING

    TEST AEROSOL GENERATOR FOR SIZERANGE 1 - 20 m

    TEST AEROSOL GENERATOR FOR SIZERANGE 0 - 1 m

    PressureGauge

    29.7 or 25.0 LPMHEPAFilter

    Flowmeter

    PUMP

    Pressure

    Gauge

    SMPS / APS

    Isokinetic Sampler

    Isokinetic Sampler

    Impactorstage

    0.3 or 5.0 LPM

    MagneticStirrer

    HEPAFilter

    Fig. 2. Experimental setup for laboratory characterization of CCI.

    volume diameter (Kasper, 1982), the conversion was made using (Peters, Chein, & Lundgren, 1993)

    Cada =

    pCm

    odm; (3)

    where da is aerodynamic diameter, dm is the mobility equivalent diameter, Ca is the slip correction

    factor for the aerodynamic diameter, Cm is the slip correction factor for the mobility equivalent

    diameter, is the dynamic shape factor, p is the density of the particle, and 0 is the unit density

    (1 g=cm3). 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=cm3, respectively.

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    The collection eciency for a given particle size, E(da), for each impaction stage, was calculated

    using

    E(da) = C(da)T(da)

    = T(da)P(da)T(da)

    ; (4)

    where T(da); C(da) and P(da) are the total, collected and penetrated particles of aerodynamic

    diameter of da, respectively. The collection eciency data were tted using the Boltzmann sigmoidal

    algorithm (Origin, MicroCal Software Inc.) using

    E(da) =A1 A2

    1 + e(dax0)=dx

    + A2; (5)

    where x0 is the median aerodynamic diameter; dx is the width of the tting; and A1 and A2, are the

    coecients determined by the algorithm. The sharpness () of the collection eciency curve was

    calculated using

    =

    d84:1

    d15:9; (6)

    where d84:1 and d15:9 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 eciencywas 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 =

    mj

    ni

    Ni; j ei; j pd3pi

    6; (7)

    where, i is the ith number of n channels in APS, j is the jth minute, Nij is the upstream par-

    ticle number, eij is the collection eciency, p is the particle density, and dp is the particle

    diameter.

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    TSI 3400A Fludized Bed

    Aerosol GeneratorSMPS / APS

    TEST AEROSOL GENERATOR FOR SIZERANGE 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 SIZERANGE 0-1m

    NaCl Solution

    TSI 3076Constant OutputAtomizerDry & filtered air

    35 psi

    Mixing ChamberDry& filtered airTSI 3012Kr-85 Neutralizer

    60.0 LPM

    Mixing Duct

    SupplementalFiltered 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 020 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 50C 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).

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    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=m3 and a relatively low concentration of about

    0:4 mg=m3. 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 2:8C). Just prior to gravimetric analysis boththe lters and the PUF substrates were exposed to 210Po 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 improvethe 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 bythe collocated APS and SMPS.

    2.6. Field study

    For the intercomparison study to measure the particulate ne mass (PM2:5), two conventional

    Harvard PM2:5 impactors (HI; Marple, Rubow, Turner, & Spengler, 1987), and a PM2:5 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 PM2:5 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 (d50; m), the collection eciency sharpness ()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,

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    Aerodynamic particle diameter (m)

    0.1 1 10

    Collec

    tionefficiency,

    %

    0

    10

    20

    30

    40

    50

    60

    70

    80

    90

    100

    5 268 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 (), and the pressure drop

    across the stage. For all stages, the 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 pressuredrop 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

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    Aerodynamic particle diameter (m)

    0.1 1 10

    Part

    icleLoss,

    %

    0

    10

    20

    30

    40

    50

    60

    70

    80

    90

    100

    345678 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. Similarresults 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 (d50), 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=m3

    (or 48 hat 126 and 276 g=m3, respectively). This should be considered a negligible eect on the cutpoint,

    compared to the eect when using an oiled at substrate, for which the d50 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 (d50 = 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

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    Loaded mass, M (mg)

    0 5 10 15 20 25

    d50

    (m)

    1.50

    1.75

    2.00

    2.25

    2.50

    2.75

    3.00

    3.25

    3.50

    Change of d50

    Loaded mass, M (mg)

    0 5 10 15 20 25

    Collectioneffic

    iency(%)

    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 ( d50 =2:5 m). (a) Change of 50% cut-o aerodynamic

    diameter vs. loaded mass. (b) Collection eciency vs. loaded mass for da = 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

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    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 0.175 0.56 0.56 1.0 1.0 1.8 1.83.2 3.25.6 5.6 10 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 mostlikely 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 fromthe 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.

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    Aerodynamic Diameter (Dp), m

    0.1 1 10

    Mass

    Concen

    tra

    tion

    /log

    (Dp

    ),

    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 forthe 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=m3, 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

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    Table 3

    Mean concentration, precision, limit of detection (LOD), and coecient of variation (CV) for CCI

    Stage No. of sample (n) Mean conc. (g=m3) Precision (g=m3) LOD (g=m3) 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 usedfor 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

    PM2:5 mass measurements for the CCI vs. the HI and the FRM, respectively. PM2:5 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. Thepolyurethane 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

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    Aerodynamic Diameter (Dp), m

    0.1 1 10

    MassConcentration/log(Dp),g

    /m3

    0

    5

    10

    15

    20

    25

    Sep. 23 - 25, 2002

    Aerodynamic Diameter (Dp), m

    0.1 1 10

    MassConcentration/lo

    g(Dp),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

    PM2:5 mass concentration.

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    HI PM 2.5 Concentration (g/m3)

    0 2 4 6 8 10 12 14 16 18 20 22

    CCIPM

    2.5

    Concen

    tra

    tion

    (g

    /m3)

    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 PM2.5 Concentration (g/m

    3)

    0 2 4 6 8 10 12 14 16 18 20 22

    CCIPM

    2.5

    Concen

    tra

    tion

    (g

    /m3)

    0

    2

    4

    6

    8

    10

    12

    14

    16

    18

    20

    22

    Data

    1 : 1

    Regression

    CCI=1.17*FRM-0.08

    r2=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).

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