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Organic aerosols in relation to small- scale wood combustion, forest fires and traffic

R. Hillamo, S. Saarikoski, H. Timonen, K. Saarnio, A.

Frey, M. Aurela

Finnish Meteorological Institute, Helsinki, Finland

L. Järvi, M. Kulmala

University of Helsinki, Helsinki, Finland

(2)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 2

Measurements

Site

SMEAR III (60°20'N, 24°97’E), urban background

• Local sources: traffic, biomass combustion

• Long-range transport ~50% of PM2.5, frequent wild fire plumes

Period shown here

• June 2006–February 2007

SMEAR III belongs to the European ACCENT network – access to field and laboratory infrastructures

Helsinki

(3)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 3

Identification of sources –different approaches

Time resolution 24-48 h

• Needs long-term measurements + large sets of chemical components → seasonal (annual) cycles

Time resolution < 3 h (for several components)

• Diurnal variations, good timing for specific episodes (pollution or clean)

• Excellent data for modellers,epidemiological studies and for statistical methods (e.g. PMF)

Same observations at several sites

• Helsinki (urban)

• Hyytiälä (rural forest)

(4)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 4

Methods

Sampling (24 h)

• PM 1 filter sampling (80 lpm, 47 mm filter)

• Analytical techniques: IC, TOC, LC/MS, TOT (Sunset lab) Online/real-time (1 s – 3 h)

• PILS-IC for ions (15 min)

• PILS-Total organic carbon analyzer for WSOC (5 min)

• Semicontinuous EC/OC (Sunset Lab, 1-3 h)

• Aethalometer (black carbon, 5 min)

• PSAP (aerosol absorption, 1 s)

• Twin-TEOM (PM 1 , PM 1-10 , 30 min)

• DMPS, APS (particle number size distribution, 10 min)

• O 3 , NOx, CO

• Meteorology

Site comparison (Helsinki/urban – Hyytiälä/rural, distance 200 km)

(5)

Black carbon (soot) data from Helsinki 1996-2005

Virkkula et al. (2007) A Simple Procedure for Correcting Loading Effects of Aethalometer Data, J. Air & Waste Manage. Assoc.

57:1214–1222

• Correction of BC data (Virkkula et al., 2007)

• Selection of periods to be

compared (1996-1997, 2000-

2001, 2004-2005)

(6)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 6

Black carbon (PM 2.5 ) in Helsinki 1996-2005:

concentrations (μg/m 3 ) during comparable periods

Järvi et al. (2007) Atmos. Chem. Phys. Discuss., 7, 14265–14294

(7)

Traffic intensity vs. BC concentrations

Järvi et al. (2007) Atmos. Chem. Phys. Discuss., 7, 14265–14294

(8)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 8

PM 2.5 from wood combustion and wild fires

0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7

6.2.06 13.2.06 20.2.06 27.2.06 6.3.06 13.3.06 20.3.06 27.3.06 3.4.06 10.4.06 17.4.06 24.4.06 1.5.06 8.5.06 15.5.06 22.5.06 29.5.06 5.6.06 12.6.06 19.6.06 26.6.06 3.7.06 10.7.06 17.7.06 24.7.06 31.7.06 7.8.06 14.8.06 21.8.06 28.8.06 4.9.06 11.9.06 18.9.06 25.9.06 2.10.06 9.10.06 16.10.06 23.10.06 30.10.06 6.11.06 13.11.06 20.11.06 27.11.06 4.12.06 11.12.06 18.12.06 25.12.06 1.1.07 8.1.07 15.1.07 22.1.07 29.1.07 5.2.07 12.2.07 19.2.07 26.2.07

Da te

levoglucosan µg/m3

0 2 4 6 8 10 12 14 16 18

OC µg/m3

MA OC 0.0

0.1 0.2 0.3 0.4 0.5 0.6 0.7

6.2.06 13.2.06 20.2.06 27.2.06 6.3.06 13.3.06 20.3.06 27.3.06 3.4.06 10.4.06 17.4.06 24.4.06 1.5.06 8.5.06 15.5.06 22.5.06 29.5.06 5.6.06 12.6.06 19.6.06 26.6.06 3.7.06 10.7.06 17.7.06 24.7.06 31.7.06 7.8.06 14.8.06 21.8.06 28.8.06 4.9.06 11.9.06 18.9.06 25.9.06 2.10.06 9.10.06 16.10.06 23.10.06 30.10.06 6.11.06 13.11.06 20.11.06 27.11.06 4.12.06 11.12.06 18.12.06 25.12.06 1.1.07 8.1.07 15.1.07 22.1.07 29.1.07 5.2.07 12.2.07 19.2.07 26.2.07

Da te

levoglucosan µg/m3

0 10 20 30 40 50 60

PM2.5 µg/m3

MA PM2.5

MA= monosaccharide anhydrates= sum (levoglucosan+mannosan+galactosan)

(9)

Wood combustion

Online measurements of PM 1 chemistry

- time resolution 15 min-3h - 9 months campaign

NO, NO2 ppb 0 50 100 150 200

CO ppm

0 200 400 600 800 1000 1200 1400 NO

CO NO2

Saturday 10 Feb

Local time

03 06 09 12 15 18 21 03 06 09 12 15 18 21

00 00 00

OC, EC µg m-3

0 2 4 6 8 10 12 14

K µg m-3

0.0 0.3 0.6 0.9 1.2 1.5

OC EC K

µg m-3

0 1 2 3 4 5 6

SO4 NH4 NO3

µg m-3

0.0 0.2 0.4 0.6 0.8 1.0

Cl Na

Local time

03 06 09 12 15 18 21 03 06 09 12 15 18 21

00 00 00

Temperature °C

-20 -15 -10 -5 0

wind speed m s-1

0 1 2 3 4 5

T wind speed

Sunday 11 Feb a)

b)

c)

d)

e)

Saarikoski S. et al., 2008, Atmospheric

Chemistry and Physics, submitted

(10)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 10

Wild fire spring 2006: mass closure study

a) Mass closure

µg/ m

3

0 10 20 30 40 50 60

Elemental carbon Mass PM

2.5

Organic compounds Ions

Sulfate

EC PM

2.5

POM Other ions SO

4

b) Carbonaceous

26 .3 . 28 .3 .

30.3. 1.4. 3.4. 5.4 . 7.4 .

9.4. 11.4. 13.4. 15 .4.

17 .4.

19 .4.

21 .4.

23.4. 25 .4.

27 .4.

29 .4. 1.5. 3.5. 5.5. 7.5.

9.5 .

µg/ m

3

0 5 10 15 20

Elemental carbon

Water-insoluble organic carbon Water-soluble organic carbon

Saarikoski et al. (2007). Chemical composition of aerosols during a major biomass burning episode over

northern Europe in spring 2006: Experimental and modelling assessments. Atmos. Environ. 41:3577-3589 .

(11)

Episode in spring 2006. Episode in August 2006.

From filter sampling

Date 15-Apr 22-Apr 29-Apr 06-May 13-May

mass concent rat ion, µg m

-3

0 10 20 30 40 50

60 Spring 2006

01-Aug 08-Aug 15-Aug 22-Aug 29-Aug

mass concent rat ion, µg m

-3

0 10 20 30 40 50 60 EC

WISPOM WSPOM Other ions Sulphate PM

2.5

August 2006

(12)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 12

August episode with 3-hour time-resolution

From on-line measurements

August 2006

Date

08-Aug 12-Aug 16-Aug 20-Aug 24-Aug

mas s c onc entrati on, µg m -3

0 20 40 60 80 100

EC

POM

Other ions

Sulphate

PM 2.5

(13)

Wildfire: August 15, 2006

D a [µm]

0.01 0.1 1 10

dm/dlogD a [µg/m 3 ]

0 20 40 60 80 100 120

A: 00-03 B: 03-06 C: 06-09 D: 09-12 E: 12-15 F: 15-18

A B

C D

E F

*

A: 0 0- 03

B: 0 3-0 6

C: 0 6- 09

D: 0 9-1 2

E: 1 2-1 5

F: 1 5- 18

mass co ncen tra tion , µg m

-3

0 10 20 30 40 50 60

*) POM and EC not available

other ions Ammonium Sulphate POM EC

PM

2.5

mass

3-hour mass size distributions (A-F) during the progress of the plume on August 15, 2006.

(F represents a non-plume situation.)

The PM 2.5 mass and chemical composition of PM 1 on August 15, 2006 with 3-hour time-

resolution.

(14)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 14

Biomass burning tracers

K/Levoglucosan K/Oxalate Oxalate/Levoglucosan

Spring episode 1.04 0.85 1.28

August episode 1.02 0.31 5.13

Plumes of August episode

0.32 0.32 1.03

”Non-plume”-samples 1.71 0.29 9.22

• Spring episode: April 24 – May 7, 2006

• August episode: August 1 – August 28, 2006

• Plume samples have been chosen according to the high content of levoglucosan

Spring flaming, August plumes smoldering fires

(15)

Levoglucosan/potassium ratio

Ja n

Feb Ma r

Ap r

Ma y

Jun Jul

Aug

Se p

Oc t

No v

Dec Jan

le vo gl uc os an/ pot as si um r at io

0 1 2 3 4

Levoglucosan better qualitative tracer than K +

(16)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 16

Long-term measurements: two sites

PM 1 filter sampling (Feb 07-Feb 08)

Organic carbon

µg /m

3

0 1 2 3 4 5 6 7

Hyytiälä Helsinki

Elemental carbon

Mar-2007 Apr-2007 May-2007 Jun-2007 Jul-2007 Aug-2007

µg/m

3

0

1

2

3

(17)

Levoglucosan

Temperature °C

-30 -20 -10 0 10 20 30

Levoglucosan/POM

0.0001 0.001 0.01 0.1

Oxalate

Temperature °C

-30 -20 -10 0 10 20 30

Oxalate/POM

0.0001 0.001 0.01 0.1

OC

Temperature °C

-30 -20 -10 0 10 20 30

C oncen tration µg /m

3

0.01 0.1 1 10 100

Summer Fall Winter

Biomass burning Episode

Contribution of POM to PM 2.5

Temperature °C

-30 -20 -10 0 10 20 30

Co ntribu tion to PM

2.5

0.01 0.1 1 10

Summer Fall Winter

Biomass burning Episode

Seasonal variation in Helsinki:

Organic carbon

Biomass burning

episode

(18)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 18

PM 1 organic carbon in Helsinki

Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Jan

C ontribution to OC

0.0 0.2 0.4 0.6 0.8 1.0

Traffic

Biomass Combustion Unknown

Fe b Ma r

Ap r Ma y

Ju n Ju l Au g

Sep Oc t No v

De c Ja n

Fe b

contribution t o OC

0.00 0.01 0.02 0.03 0.04

Oxalate

-Traffic (primary) based on EC/OC ratio

-Biomass combustion based

on levoglucosan to OC ratio

- Unknown is obviously SOA

(19)

Sources of PM 1 (PMF)

Factor 2

OC EC WSOC levog NH4 K SO4 Ox O3 NO NO2

relative contribution

0.0 0.2 0.4 0.6 0.8 1.0

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Jan

relative contribution

0 2 4 6 8 10

Factor 3

OC EC WSOC levog NH4 K SO4 Ox O3 NO NO2

relative contribution

0.0 0.2 0.4 0.6 0.8 1.0

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Jan

relative contribution

0 1 2 3 4 5

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Jan

relative contribution

0 1 2 3 4

Factor 4

OC EC WSOC levog NH4 K SO4 Ox O3 NO NO2

relative contribution

0.0 0.2 0.4 0.6 0.8 1.0

Factor 1

OC EC WSOC levog NH4 K SO4 Ox O3 NO NO2

relative contribution

0.0 0.2 0.4 0.6 0.8 1.0

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Jan

relative contribution

0 1 2 3 4 5

SOA

Biomass combustion

LRT

Traffic

Saarikoski S. et al., 2008, Atmospheric

Chemistry and Physics, submitted

(20)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 20

Concentrations from different sources

b) Water-soluble organic carbon

Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Jan

co nc en tr at ion µ g m

-3

0 1 2 3 4

a) Organic carbon

co ncentrati on µg m

-3

0 1 2 3 4 5 6 7

Traffic SOA

Biomass combustion Long-range transport

• PM 1 (<1µm)

24 h sampling,

chemical analysis

in laboratory

(21)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 21

Seasonal source contributions in Helsinki

The source contributions for OC and WSOC in winter (Dec–Feb), spring (Mar–May), summer (Jun–Aug) and fall (Sep–Nov) (average ±SD). Sources and their contributions were identified by PMF.

Winter Spring Summer Fall

% of OC Secondary organic

aerosol 16 ± 11 34 ± 17 64 ± 12 32 ± 18

Biomass combustion 41 ± 15 12 ± 8.9 3.4 ± 6.0 20 ± 14 Long-range transport 17 ± 13 29 ± 10 19 ± 11 21 ± 14

Traffic 26 ± 12 25 ± 13 15 ± 13 27 ± 15

% of WSOC

Secondary organic

aerosol 28 ± 18 49 ± 19 78 ± 8.8 47 ± 21

Biomass combustion 38 ± 16 11 ± 8.1 2.3 ± 4.1 18 ± 15 Long-range transport 18 ± 14 27 ± 11 13 ± 8.4 20 ± 13

Traffic 16 ± 8.5 14 ± 9.0 6.6 ± 6.7 15 ± 11

Saarikoski S. et al., 2008, Atmospheric Chemistry and Physics, submitted

(22)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 22

24-hour sample

24-hour PM

1

filter sample

22/08 09:00 Date 23/08 09:00

mass concen tr a tion, µg/m

3

0 10 20 30 40

PM1-2.5 Potassium Ammonium Nitrate Sulphate Oxalate WSPOM WISPOM EC

24-hour PM

2.5

sample

22/08 09:00 Date 23/08 09:00

ma ss co ncen tr atio n, µg /m 3

0 10 20 30 40

PM

2.5

(23)

On-line measurement

On-line measurements

Date

22/08 09:00 22/08 15:00 22/08 21:00 23/08 03:00 23/08 09:00

m as s c on cent ra tion , µ g /m

3

0 10 20 30 40

PM1-2.5 Potassium Ammonium Sodium Chloride Nitrate Sulphate Oxalate POM EC

On-line PM

2.5

22/08 09:00 22/08 15:00 22/08 21:00 23/08 03:00 23/08 09:00 Date

mass con ce nt rat ion, µg /m

3

0 10 20 30 40

PM

2.5

(24)

March 19, 2008

R. Hillamo, Cost 633, Brussels, March 13, 2007 24

Conclusions

• To assess PM sources, a large array of chemical

components and physical parameters should be measured on long-term basis

Atmospheric particulate matter system highly unlinear

→ decreasing one component may increase concentrations of other components

• Data from advanced PM measurements (in a few locations in Europe) is needed in planning the cost-effective

abatement strategy for Europe (health effects or climate change concerns)

New challenges for the PM studies due to combustion of

biofuels and other efforts needed to reduce CO 2 emissions

Referencer

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