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Coarse PMCoarse PMMethods Evaluation StudyMethods Evaluation Study
Study Design and Preliminary ResultsStudy Design and Preliminary Results
Thomas Ellestad, Robert Vanderpool, Thomas Ellestad, Robert Vanderpool, Paul Solomon, and Mary HarmonPaul Solomon, and Mary Harmon
USEPA/ORD/NERLUSEPA/ORD/NERL
Sanjay Natarajan, Chris Noble, and Bob MurdochSanjay Natarajan, Chris Noble, and Bob MurdochResearch Triangle InstituteResearch Triangle Institute
[email protected]@epa.gov919919--541541--78777877
BackgroundBackground
§§ 1997 air regulations established NAAQS for 1997 air regulations established NAAQS for PM2.5 and PM10 as separate metricsPM2.5 and PM10 as separate metrics
§§ U.S. courts have reviewed subsequent U.S. courts have reviewed subsequent litigation and ruled that the PM10 metric is a litigation and ruled that the PM10 metric is a “poorly matched indicator” because it “poorly matched indicator” because it includes the PM2.5 fractionincludes the PM2.5 fraction
§§ EPA has since been considering the possibility EPA has since been considering the possibility of vacating the PM10 regulation and of vacating the PM10 regulation and developing a separate standard for PMcdeveloping a separate standard for PMc
Study ObjectivesStudy Objectives
§§ EvaluateEvaluate the field performance of the field performance of leading leading methods for monitoring the coarse fraction of methods for monitoring the coarse fraction of PM10 (PMc = PM10 PM10 (PMc = PM10 –– PM2.5)PM2.5)
§§ Evaluate samplers which are either already Evaluate samplers which are either already commercially available or in their final stages of commercially available or in their final stages of developmentdevelopment
§§ Include both filterInclude both filter--based (timebased (time--integrated) and integrated) and semisemi--continuous measurement methodscontinuous measurement methods
PM2.5 and PM10 FRM SamplersPM2.5 and PM10 FRM Samplers§§ Standard lowStandard low--vol PM10 inlets vol PM10 inlets
aspirating at 16.7 lpm aspirating at 16.7 lpm (actual conditions)(actual conditions)
§§ PM2.5 aerosol fractionation PM2.5 aerosol fractionation using aWINS equipped with using aWINS equipped with DOS impaction oil DOS impaction oil
§§ Filters were conditioned at Filters were conditioned at 22C and 35% RH, analyzed 22C and 35% RH, analyzed gravimetrically. Postgravimetrically. Post--sampling filters archived at sampling filters archived at --30C for subsequent chemical 30C for subsequent chemical analysisanalysis
§§ 3 FRM pairs from BGI, 3 FRM pairs from BGI, R&P, and ThermoR&P, and Thermo--Andersen Andersen equipped with teflon filters equipped with teflon filters (4(4thth FRM pair equipped with FRM pair equipped with quartz filters)quartz filters)
PM10
PM10(WINS Removed)
PM2.5(with WINS)
PMc = PM10 – PM2.5
R&P PartisolR&P Partisol--Plus 2025 DichotPlus 2025 Dichot
§§ Standard PM10 inlet Standard PM10 inlet aspirating at 16.7 lpm aspirating at 16.7 lpm (actual)(actual)
§§ Aerosol fractionation by Aerosol fractionation by custom virtual impactor custom virtual impactor (15 lpm and 1.67 lpm)(15 lpm and 1.67 lpm)
§§ PM2.5 and PMc mass PM2.5 and PMc mass collected on 47 teflon filters collected on 47 teflon filters for gravimetric analysisfor gravimetric analysis
§§ Sequential sampler with Sequential sampler with multimulti--day capabilityday capability
§§ 4 units used in our study 4 units used in our study (3 teflon and 1 quartz)(3 teflon and 1 quartz)
R&P Coarse Particle TEOMR&P Coarse Particle TEOM
§§ Modified PM10 inlet Modified PM10 inlet aspirating at 50 lpm (actual)aspirating at 50 lpm (actual)
§§ PM10 aerosol is fractionated PM10 aerosol is fractionated by a custom virtual impactor by a custom virtual impactor (2 lpm coarse flow and 48 lpm (2 lpm coarse flow and 48 lpm fine flow)fine flow)
§§ PMc fraction is heated to 50 C PMc fraction is heated to 50 C to remove particle bound to remove particle bound waterwater
§§ Coarse aerosol is collected Coarse aerosol is collected and quantified by a standard and quantified by a standard TEOM sensorTEOM sensor
§§ 3 units used in our study3 units used in our study
Tisch SPMTisch SPM--613D Dichot Beta Gauge613D Dichot Beta Gauge
§§ Standard PM10 inlet Standard PM10 inlet aspirating at 16.7 lpm (~std)aspirating at 16.7 lpm (~std)
§§ Aerosol heated >25CAerosol heated >25C§§ Aerosol fractionation by Aerosol fractionation by
custom virtual impactor custom virtual impactor §§ PM2.5 and PMc mass PM2.5 and PMc mass
collected on polyflon tape collected on polyflon tape rollroll
§§ PM2.5 and PMc mass PM2.5 and PMc mass quantified hourly using quantified hourly using separate beta sources and separate beta sources and detectorsdetectors
§§ 3 units used in our study3 units used in our study
TSI Model 3321 Aerodynamic Particle SizerTSI Model 3321 Aerodynamic Particle Sizer
§§ Standard PM10 inlet aspirating Standard PM10 inlet aspirating at 16.7 lpm (actual)at 16.7 lpm (actual)
§§ Isokinetic fraction of PM10 Isokinetic fraction of PM10 aerosol removed at 5 lpm and aerosol removed at 5 lpm and enters the APS inletenters the APS inlet
§§ APS sizes individual particles APS sizes individual particles aerodynamically using time of aerodynamically using time of flight approachflight approach
§§ Single particle volume converted Single particle volume converted to mass using mean density to mass using mean density provided by userprovided by user
§§ Total aerosol mass is sum of Total aerosol mass is sum of individual particle massindividual particle mass
§§ APS provide only PMc; not APS provide only PMc; not applicable for PM2.5 or PM10applicable for PM2.5 or PM10
§§ Only sampler in study which Only sampler in study which provides detailed size distribution provides detailed size distribution informationinformation
§§ 2 units used in our study2 units used in our study
Sampler Performance IssuesSampler Performance Issues
§§ Relative bias versus collocated FRMs Relative bias versus collocated FRMs
§§ Precision (2 or 3 samplers of each type)Precision (2 or 3 samplers of each type)
§§ Field reliabilityField reliability
§§ Evaluation under a wide range of Evaluation under a wide range of weather conditions and aerosol typesweather conditions and aerosol types
QA/QC InitiativesQA/QC Initiatives§§ QAPP was reviewed and approved by EPAQAPP was reviewed and approved by EPA§§ Study design and operation passed EPA’s systems Study design and operation passed EPA’s systems
auditaudit§§ SOPs were reviewed by the sampler manufacturersSOPs were reviewed by the sampler manufacturers§§ Sampler manufacturers were allowed to verify the Sampler manufacturers were allowed to verify the
working condition of their respective samplers prior to working condition of their respective samplers prior to sampling at each sitesampling at each site§§ Sampling and fractionation components cleaned prior Sampling and fractionation components cleaned prior
to each studyto each study§§ NISTNIST--traceable sampler calibration equipment was traceable sampler calibration equipment was
used for all sampler calibrations and auditsused for all sampler calibrations and audits§§ Three performance audits and three field blank tests Three performance audits and three field blank tests
were conducted at each site were conducted at each site §§ Replicate weighings were conducted at the site as well Replicate weighings were conducted at the site as well
as at EPA’s RTP weighing facilityas at EPA’s RTP weighing facility
Study DetailsStudy Details
§§ Using 22 hour, daily sampling periods for comparisons Using 22 hour, daily sampling periods for comparisons (11 am to 9 am local time) (11 am to 9 am local time)
§§ Chemical analysis (XRF, IC, thermal optical) of Chemical analysis (XRF, IC, thermal optical) of archived filters will provide particle composition, archived filters will provide particle composition, which may explain observed sampler performancewhich may explain observed sampler performance
§§ Full data set from all three sites will be ready by Feb Full data set from all three sites will be ready by Feb 2004. Detailed results from Gary, IN will be presented 2004. Detailed results from Gary, IN will be presented at the October AAAR meetingat the October AAAR meeting
Study SitesStudy Sites
§§ RTP, NC (10 days of shakedown tests, Jan. 2003)RTP, NC (10 days of shakedown tests, Jan. 2003)
§§ Gary, IN (30 days of tests under cold, snow/rain, Gary, IN (30 days of tests under cold, snow/rain,
variable PM2.5/PM10 ratios, Marchvariable PM2.5/PM10 ratios, March--April, 2003)April, 2003)
§§ Phoenix, AZ (30 days of tests under hot, dusty Phoenix, AZ (30 days of tests under hot, dusty
conditions, consistently low PM2.5/PM10 ratios, conditions, consistently low PM2.5/PM10 ratios,
MayMay--June, 2003)June, 2003)
§§ Riverside, CA (30 days of tests under warm Riverside, CA (30 days of tests under warm
conditions, higher PM2.5/PM10 ratios than Phoenix, conditions, higher PM2.5/PM10 ratios than Phoenix,
JulyJuly--August, 2003)August, 2003)
GARY, IN SIZE DISTRIBUTION DATAMarch - April, 2003
0.00
0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
0.90
1.00
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32
Sample Day
PM
2.5/
PM
10 C
once
ntra
tion
Rat
io
GARY, IN FRM DATA
PM2.5/PM10 Range = 0.32 to 0.83; Mean = 0.55
PMc FRM MEASUREMENTS - GARY vs RTP WEIGHINGGary, IN (March - April, 2003)
0.0
10.0
20.0
30.0
40.0
50.0
60.0
0 5 10 15 20 25 30 35
SAMPLE DAY
PM
c C
on
c. (m
icro
gra
ms/
m3 )
GARY WEIGHING
RTP WEIGHING
RTP/Gary = 1.00
INTERMANUFACTURER PM2.5 FRM MEASUREMENTS (RTP WEIGHING)
Gary, IN (March - April, 2003)
0.0
10.0
20.0
30.0
40.0
50.0
60.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
SAMPLE DAY
PM
2.5
Co
nc.
(m
icro
gra
ms/
m3 )
ANDR&PBGI
INTERMANUFACTURER CV = 1.5%
Max PM2.5 = 46.9 ì g/m3
Min PM2.5 = 10.3 ì g/m3
Mean PM2.5 = 22.8 ì g/m3
INTERMANUFACTURER PM10 FRM MEASUREMENTS(RTP WEIGHING)
Gary, IN (March - April, 2003)
0.0
10.0
20.0
30.0
40.0
50.0
60.0
70.0
80.0
90.0
100.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
SAMPLE DAY
PM
10 C
on
c. (
mic
rog
ram
s/m
3 )
ANDR&PBGI
INTERMANUFACTURER CV = 2.4%
Max PM10 = 84.9 ì g/m3
Min PM10 = 22.6 ì g/m3
Mean PM10 = 42.6 ì g/m3
INTERMANUFACTURER PMc FRM MEASUREMENTS (RTP WEIGHING)
Gary, IN (March - April, 2003)
0.0
10.0
20.0
30.0
40.0
50.0
60.0
70.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
SAMPLE DAY
PM
c C
onc.
(m
icro
gram
s/m
3 )
ANDR&PBGI
INTERMANUFACTURER CV = 5.7%
Max PMc = 58.1 ì g/m3
Min PMc = 4.5 ì g/m3
Mean PMc = 19.9 ì g/m3
DICHOT AND FRM TIMELINE (PM2.5)GARY, IN (MARCH - APRIL, 2003)
0.0
5.0
10.0
15.0
20.0
25.0
30.0
35.0
40.0
45.0
50.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
2.5 C
onc.
(mic
rogr
ams/
m3)
PM2.5 FRMR&P DICHOTS
DICHOT/FRM = 0.99
Dichot versus FRM PM2.5 ConcentrationsGary, IN (March - April, 2003)
0.0
5.0
10.0
15.0
20.0
25.0
30.0
35.0
40.0
45.0
50.0
0.0 5.0 10.0 15.0 20.0 25.0 30.0 35.0 40.0 45.0 50.0
FRM PM2.5 Concentrations (micrograms/m3)
Dic
hot P
M2.
5 C
once
ntra
tions
(mic
rogr
ams/
m3)
Dichot = 0.99*FRM + 0.0R Square = 0.998
DICHOT AND FRM TIMELINE (PMc)Gary, IN (March - April, 2003)
0.0
10.0
20.0
30.0
40.0
50.0
60.0
70.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
c C
on
c.
(mic
rog
ram
s/m
3)
FRM PMc (PM10-PM2.5)R&P DICHOTS
Dichot/FRM = 0.89
Dichot = 0.87*FRM + 0.4R square = 0.969
DICHOT AND FRM TIMELINE (PM10)Gary, IN (March - April, 2003)
0
10
20
30
40
50
60
70
80
90
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
10 C
on
c. (m
icro
gra
ms/
m3 ) PM10 FRM
R&P DICHOTS
Dichot/FRM = 0.94Dichot = 0.95*FRM - 0.5R square = 0.981
TISCH SPM-613D AND FRM TIMELINE (PM2.5)Gary, IN (March - April, 2003)
0
10
20
30
40
50
60
70
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
2.5
Co
nc.
(mic
rog
ram
s/m
3 )
PM2.5 FRMTISCH SPM-613D
TISCH CV = 7.1%
TISCH/FRM = 1.26
Tisch = 1.17*FRM + 1.6R square = 0.948
TISCH SPM-613D AND FRM TIMELINE (PMc)Gary, IN (March - April, 2003)
0
10
20
30
40
50
60
70
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
c C
on
c. (m
icro
gra
ms/
m3 )
FRM PMc (PM10-PM2.5)
TISCH SPM-613D
TISCH/FRM = 0.91
TISCH = 0.89*FRM + 0.3R square = 0.979
TISCH CV = 10.5%
R&P COARSE TEOM AND FRM TIMELINE (PMc)Gary, IN (March - April, 2003)
0
10
20
30
40
50
60
70
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
c C
on
c. (
mic
rog
ram
s/m
3)
PMc (PM10-PM2.5)
R&P CONTINUOUS COARSE
TEOM PMc/FRM = 0.69
TEOM PMc CV = 4.4%
TEOM = 0.68* FRM + 0.18R square = 0.982
TSI APS vs FRM PMc ConcentrationsGary, IN (March - April)
0.0
10.0
20.0
30.0
40.0
50.0
60.0
70.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
SAMPLE DAY
PM
c C
on
c. (
mic
rog
ram
s/m
3 )
APS 1 PMc
APS 2 PMc
Mean FRM PMc
APS/FRM = 0.42
APS CV = 16.8%
APS = 0.48*FRM -1.4R square = 0.795
Phoenix versus RTP FRM WeighingMay - June 2003
0.0
50.0
100.0
150.0
200.0
250.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30
Sampling Day
Mas
s C
once
ntra
tion
(mic
rogr
ams
per
cubi
c m
eter
)
PM2.5 (RTP)
PM10 (RTP)
PMc (RTP)
PM2.5 (Site)
PM10 (Site)
PMc (Site)
PM10
PMc
PM2.5
Inter-manufacturerer PM2.5 CV = 3.4%Inter-manufacturerer PMc CV = 3.3%Inter-manufacturerer PM10 CV = 3.6%
PM2.5/PM10 Range = 0.10 to 0.28: Mean = 0.22
Dichot PM2.5 versus FRM PM2.5Phoenix, AZ
May - June, 2003
0.0
5.0
10.0
15.0
20.0
25.0
30.0
0.0 5.0 10.0 15.0 20.0 25.0
FRM PM2.5 (micrograms per cubic meter)
Dic
ho
t P
M2.
5 (m
icro
gra
ms
per
cu
bic
met
er)
Dichot = 1.24 * FRM - 1.6 R Square = 0.97
Mean Dichot/FRM = 1.09
DICHOT AND FRM TIMELINE (PMc)Phoenix, AZ (May - June, 2003)
0.0
50.0
100.0
150.0
200.0
250.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
c C
on
c.
(mic
rog
ram
s/m
3 ) PMc (PM10-PM2.5)R&P DICHOTS
Mean Dichot/FRM = 0.80
Dichot = 0.70*FRM + 5.0R square = 0.98
DICHOT AND FRM TIMELINE (PM10)Phoenix, AZ (May - June, 2003)
0.0
50.0
100.0
150.0
200.0
250.0
0 2 4 6 8 10 12 14 16 18 20 22 24 26 28 30 32
Sample Day
PM
10 C
on
c.
(mic
rog
ram
s/m
3 ) PM10 FRMR&P DICHOTS
Mean Dichot/FRM = 0.84
Dichot = 0.75*FRM + 5.9R square = 0.98
Tisch & FRM PM2.5 ConcentrationsPhoenix AZ: May - Jun, 2003
0
10
20
30
40
50
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30
Sample Day
PM
2.5
con
cen
trat
ion
s (u
g/m
3)
Tisch PM2.5-1
Tisch PM2.5-2
Tisch PM2.5-3
Mean FRM-PM2.5
Average Tisch CV = 5.9 %
Mean Tisch/FRM = 1.70
Tisch = 2.03*FRM - 3.4R square = 0.947
Tisch, & FRM PMc ConcentrationsPhoenix AZ: May - Jun, 2003
0
20
40
60
80
100
120
140
160
180
200
220
1 3 5 7 9 11 13 15 17 19 21 23 25 27 29
Sample Day
PM
c co
nce
ntr
atio
ns
(ug
/m3)
Tisch PMc-1
Tisch PMc-2
Tisch PMc-3
Mean FRM-PMc
Average Tisch PMc CV = 9.5 %
Mean Tisch/FRM = 1.04
Tisch = 0.92*FRM + 6.0R square = 0.996
TEOM, & FRM PMc ConcentrationsPhoenix AZ: May - Jun, 2003
0
20
40
60
80
100
120
140
160
180
200
220
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30
Sample Day
PM
c co
nce
ntr
atio
ns
(ug
/m3) TEOM PMc1
TEOM PMc2TEOM PMc3FRM-PMc
Average TEOM PMc CV = 6.6 %
Average TEOM/FRM Ratio = 1.05
TEOM = 0.79*FRM +12.8R square = 0.951
APS, & FRM PMc ConcentrationsPhoenix AZ: May - Jun, 2003
0
20
40
60
80
100
120
140
160
180
200
220
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30
Sample Day
PM
c co
nce
ntr
atio
ns
(ug
/m3)
APS 1-PMc
APS 2-PMc
FRM PMcAverage APS PMc CV (Days 1-15) = 2.2 %
Average APS/FRM = 0.55
APS = 0.56*FRM -0.2R square = 0.992
PM Size Distributions (TSI APS)Gary,IN and Phoenix,AZ
0.0
0.5
1.0
1.5
2.0
2.5
3.0
3.5
4.0
4.5
0 1 10 100
Log Dp
Del
ta M
ass/
Del
ta L
og D
p
Gary
Phoenix
Summary of ResultsSummary of Results(independent of site)(independent of site)
§§ FRMs show strong interFRMs show strong inter--manufacturer precision manufacturer precision (CV<4% for all three metrics) with no tendency for (CV<4% for all three metrics) with no tendency for producing negative PMc values producing negative PMc values §§ FilterFilter--based dichots show strong precision (CV<4% based dichots show strong precision (CV<4%
for all metrics)for all metrics)§§ Site weighing results agree closely with RTP resultsSite weighing results agree closely with RTP results§§ Precision of the semiPrecision of the semi--continuous samplers is continuous samplers is
considered to be acceptableconsidered to be acceptable§§ Correlation (RCorrelation (R22) of all continuous samplers is ) of all continuous samplers is
typically strong versus the collocated FRMstypically strong versus the collocated FRMs
0.550.42APS/FRM PMcTSI APS
1.040.91Tisch/FRM PMc
1.161.09Tisch/FRM PM10
1.701.26Tisch/FRM PM2.5TISCH
1.050.69TEOM PMc/FRM TEOM PMc
0.790.90Dichot/FRM PMc
0.840.94Dichot/FRM PM10
1.091.00Dichot/FRM PM2.5DICHOTS
0.180.55PM2.5/PM10 Ratio
0.10 - 0.280.32 - 0.83PM2.5/PM10 Range
55.619.9PMc Mean ( ìg/m3)SITE AEROSOL
PHOENIX, AZGARY, IN
SUMMARY OF SITE RESULTSSUMMARY OF SITE RESULTS
Future WorkFuture Work
§§ Complete RTP gravimetric analysis of Riverside, Complete RTP gravimetric analysis of Riverside, CA filters (>1500 filter weighings per site)CA filters (>1500 filter weighings per site)
§§ Conduct chemical analysis of archived site Conduct chemical analysis of archived site filters; potentially use results as “explainers” of filters; potentially use results as “explainers” of sampler performancesampler performance
§§ Possibly conduct comprehensive field tests at an Possibly conduct comprehensive field tests at an additional field siteadditional field site
§§ Possibly perform laboratory tests with samplers Possibly perform laboratory tests with samplers to better understand aerosol fractionation and/or to better understand aerosol fractionation and/or particle loss issuesparticle loss issues
AcknowledgementsAcknowledgements
§§ RupprechtRupprecht & Patashnick, Inc.& Patashnick, Inc.§§ Tisch Environmental, Inc.Tisch Environmental, Inc.
§§ TSI, Inc.TSI, Inc.
§§ Indiana Department of Environmental Indiana Department of Environmental Management (Gary)Management (Gary)
§§ Maricopa County Environmental Services Maricopa County Environmental Services Department (Phoenix)Department (Phoenix)§§ University of California Ag Ops (Riverside)University of California Ag Ops (Riverside)
DisclaimerDisclaimer
§§ The United States Environmental Protection The United States Environmental Protection Agency through its Office of Research and Agency through its Office of Research and Development funded and managed the Development funded and managed the research described here under Contract 68research described here under Contract 68--DD--0000--206. It has been subjected to Agency 206. It has been subjected to Agency review and approved for publication.review and approved for publication.