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2015 international Training Course in Atmospheric ChemistryCartagena, Colombia, July, 2015
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Atmospheric Aerosols
Size distribution - composition part III
International Atmospheric Chemistry - July 2015
2015 international Training Course in Atmospheric Chemistry
Cartagena, Colombia, July, 2015
TYPICAL U.S. AEROSOL SIZE DISTRIBUTIONS
Fresh
urban
Aged
urban rural
remote Warneck [1999]
Size Distribution
0
500
1000
1500
0 1 2 3
Dimetro (mm)
dN
/dD
(m
m-1cm
-3)
0
500
1000
1500
0,1 1 10
Dimetro (mm)
dN
/dD
(m
m-1cm
-3)
Size Distributions
0
500
1000
1500
2000
2500
0,1 1 10
Dimetro (mm)
dN
/d??? (**
*)
dN/dD dN/dlnD dN/dlogD
(cm-3
)
(mm-1
cm-3
)
(cm-3
)
Diferences among distributions
0
4000
8000
12000
16000
20000
0 0.2 0.4 0.6 0.8 1
D (mm)
dN/dlog
D (cm
-3 )
martimo
continental
rural
urbano
Difference in the distributions
0
4000
8000
12000
16000
20000
0.001 0.01 0.1 1
D (mm)
dN/dlog
D (cm
-3 )
martimo
continental
rural
urbano
Differences in the distributions
0
40
80
120
160
200
0.001 0.01 0.1 1 10
D (mm)
dN/dlog
D (cm
-3 )
martimo
continental
rural
urbano
0.01
0.1
1
10
100
1000
10000
100000
0.001 0.01 0.1 1 10
D (mm)
dN/dlog
D (cm
-3 )
martimo
continental
rural
urbano
02
4
6
8
10
0.001 0.01 0.1 1 10
D (mm)
dN-d
M/d
logD
Nmero
Massa
URBAN AND BIOMASS BURNING
0
5000
10000
15000
20000
25000
1 10 100 1000
DIMETRO (nm)
dN
/dD
(cm
-3)
SP min
SP mx
AM min
AM mx
00.03
0.06
0.09
0.12
0.15
1.00 10.00 100.00 1000.00
DIMETRO (nm)
CO
NC
EN
TR
A
O
(??) NMEROREA
VOLUME
Size Distributions for Diesel particles.
0
0.05
0.1
0.15
0.2
0.25
1 10 100 1,000 10,000
Diameter (nm)
Nor
mal
ized
Con
cent
ratio
n (1
/Cto
tal)d
C/d
logD
p
Number Surface Mass
Fine Particles
Dp < 2.5 mm
Ultrafine Particles
Dp < 100 nm
Nanoparticles
Dp < 50 nm
Nuclei Mode - Usually
forms from volatile
precursors as exhaust
dilutes and cools
Accumulation Mode - Usually
consists of carbonaceous
agglomerates and adsorbed
material
Coarse Mode - Usually
consists of reentrained
particles, crankcase
fumes
PM10
Dp < 10 mmIn some cases this
mode may consist of
very small particles
below the range of
conventional
instruments, Dp < 10
nm
Kittelson et al, 2002
DIURNAL CICLE
0
5000
10000
15000
20000
4 8 12 16 20 24
HORA LOCAL
dN
/dlo
gD
30
100
300
0
5000
10000
15000
20000
14 18 22 2 6 10
HORA LOCAL
dN
/dlo
gD 30
100
300
So Paulo
Rondnia
Variao temporal da concentrao do nmero de partculas, em funo do dimetro.
Albuquerque T., 2007
Distribuio de Tamanho Centro So Paulo
01
2
3
4
5
6
7
8
9Conce
ntra
o m
dia
(g.m
-3)
Estgios 5,68 5,43 5,57 5,26 4,30 4,74 5,22 8,78 5,24 2,42 5,75 3,66 3,11 2,75
BC 0,02 0,02 0,03 0,05 0,04 0,11 0,18 1,47 0,73 0,49 2,19 0,05 0,02 0,02
I 1A 2A 3A 4A 5A 6A 7A 8A 9A 10A A B C
Mass size distributions for aerosol collected at So Paulo
Black Carbon distribution
Main distribution at nucleation
interval
Mass size distribution.
Five modes can be see:
ultrafine; nucleation,
accumulation, fine and
coarse
Almeida et al., 2014
Number Size Distribution De 10 a 660 nm.
Mass Size Distribution
Atmospheric Sciences Department - USP
Number Size Distributions
Cumulative Fraction
International Atmospheric Chemistry - July 2015
International Atmospheric Chemistry - July 2015
International Atmospheric Chemistry - July 2015
Composition
NARSTO, 2004
Annual mean PM2.5 concentrations (NARSTO, 2004)
Current air quality standard is 15 mg m-3
THE IMPORTANCE OF ORGANIC AEROSOL
[Zhang et al., 2007] Sulfate Organics
Organic material contributes 20-50% of the total fine aerosol mass at continental mid-latitudes [Saxena and Hildemann, 1996; Putaud et al., 2004] and as much as 90% in the tropical forested areas [Andreae and Crutzen, 1997; Talbot et al., 1988; 1990;
Artaxo et al., 1988; 1990; Roberts et al., 2001]
NH4+ NO3-
110
100
1000
10000
1977 1981 1983 1986 1989 1994 1997 1998 1999 2003 2005 2008 2009 2012
Co
nce
ntr
ao
ng
/m3
Temporal Variation of PM2.5 concentration in So Paulo
MP2.5
Si
S
K
Ca
V
Fe
Ni
Zn
S
Pb
References since 1978 (Orsini et al.), etc.
Important public policies:
- Sulfur reduction in fuel and banning
of Pb
- Change the fuel in boilers
- Proconve (Program for Controlling
Vehicular emission)
Monthly variations in selected air pollutants in So Paulo. Solid regression lines show monthly mean concentrations used in
this paper. Error bars summarize the relative uncertainties in pollutant concentration measurements. Data are from the So
Paulo Environmental Company CETESB, 20002013 (http://www.cetesb.sp.gov.br/ar/qualidade-do-ar/32-qualar) Perez et al., 2015, JGR
Concentration OC/EC & PM2.5
Winter 2012
Projeto NUANCE
y = 2.1236x - 0.6739
R = 0.6735
0
10
20
30
40
50
60
0 5 10 15 20 25
OC/PM2.5= 0.44 EC/PM2.5=0.13
Hetem, mestrado
Results show an increase in aerosol hygroscopicity in the
afternoon as a result of
aerosol photochemical processing, leading to an
enhancement of both organic and
inorganic secondary aerosols in the atmosphere, as well
as an increase in aerosol
average diameter.
Atmos. Chem. Phys. Discuss., 13, 3235332389, 2013 www.atmos-chem-phys-discuss.net/13/32353/2013/
doi:10.5194/acpd-13-32353-2013
CCN number distribution
AOD mean AOD maximum AOD minimum
Aqua Satellite
0,316 0,215
0,927 0,201
0,049 0,005
Terra Satellite 0,187 0,174 0,915 0,024 0,005 0,005
AOD July-September, 2012
LIDAR Retroscatering, September 12, 2012
Figura 2 Medidas do perfil vertical da atmosfera da RMSP para o dia 12 de Setembro
de 2012, durante a campanha de medidas do projeto NUANCES-SP.
a) b)
c)
d)
Vertical Profile Setembro 12, 2012
Lopes, 2013
Lidar Measurements and AOD
Atmospheric Sciences Department - USP
1.0
10.0
100.0
1000.0
10000.0
Co
nce
ntr
a
o e
m n
g/m
3
g/m3
0.001
0.01
0.1
1
10
100
Pa
rtic
ipa
o
em
% d
e M
P2
.5
Tra
ce-e
lem
ent
con
cen
trat
ion
SECONDARY ORGANIC AEROSOL (SOA)
PRIMARY BIOLOGICAL AEROSOL PARTICLES (PBAP)
International Atmospheric Chemistry - July 2015
Emission Inventory of Organic Aerosols
Botton-up approach
BSOA (biogenic SOA) 12-70 TgC/year
POA 35 TgC/year (9 anthropogenic) (25 biomass burning)
ASOA 2- 12 TgC/year
Total 50-90 TgC/year
The formation, properties and impact of secondary organic aerosol: current and
emerging issues
Atmos. Chem. Phys., 9, 51555236, 2009 www.atmos-chem-phys.net/9/5155/2009/
Isoprene (C5H8)
Monoterpenes(C10H16)
Sesquiterpenes (C15H24)
WHICH VOCs ARE IMPORTANT SOA PRECURSORS?
Anthropogenic SOA-precursors = aromatics
(emissions are 10x smaller)
Three factors:
1. Atmospheric Abundance
2. Chemical reactivity
3. The vapour pressure (or volatility)
of its products
International Atmospheric Chemistry - July 2015
Estimativa da formao de Aerossis Orgnicos
Secundrios a partir dos dados medidos nos
experimentos de tneis. Em azul para o ano de 2004 e
em vermelho para o ano de 2011
PRIMARY BIOLOGICAL AEROSOL PARTICLES (PBAP)
POLLEN
BACTERIA VIRUSES
FUNGUS
ALGAE PLANT
DEBRIS
Jaenicke [2005] suggests may be as large a source as dust/sea salt (1000s Tg/yr)
May act as CCN and IN [Diehl et al., 2001; Bauer et al., 2003; Christiner et al., 2008]
Burkard
7-day Recording Sampler
Pollen Spores in So Paulo
Lamina
(Drum) Fita
Lminas ROGERS et al., 2001 Msc. Ana Paula Mendes
Ascomicetos
Basidiomicetos Basidisporo
Ascsporo
Myxomicetos
Deuteromicetos Mitsporos
Metodology:
HAINES et al., 2000; Imagens: VALERO, 2013; GUIMARES, 2008; ONTARIO CROPIPM, 2009; ROCA, 2015
results: spores
;
;
A Pithomyces chartarum; K: Diatrypaceae Grande;
B: Venturia sp.; L: Ascsporo de 2 clulas sem cor;
C: Torula sp.; M: Paraphaeosphaeria Michotii
D: Basidisporo colorido indet.;
N: Basidisporos hialino grande;
E: Spegazzinia sp.; O: Aspergillus/Penicillium like
F: Myxomyceto; P: Cladosporium sp.;
G: Gliomastix sp.; Q: Ascsporo de 4 clulas sem cor;
H: Ascsporo de 4 clulas com cor;
R: Drechslera-like;
I: Ganoderma sp.; S: Xylariaceae;
J: Epicoccum nigrum; T: Periconia sp.
Secondary organic aerosol (SOA)
droplets that were formed by atmospheric
oxidation
and gas-to-particle conversion of biogenic
volatile organic compounds) and in which no
other chemical components were detectable; (ii)
SOA-inorganic particles composed of secondary
organic material mixed with sulfates and/or
chlorides
from regional or marine sources ; (iii)
primary biological aerosol (PBA) particles, such
as plant fragments or fungal spores;
(iv) mineral dust particles consisting mostly of
clay minerals from the Sahara desert; or
(v) pyrogenic carbon particles that exhibited
characteristic
agglomerate structures and originated
from regional or African sources of biomass
burning
or fossil fuel combustion (6). Fluorescent biological aerosol (FBA) particles, which can be
regarded as a lower-limit proxy for PBA particles
Some examples aerosol
characterization
Metropolitan Area of So Paulo - MASP
Metropolitan Area of So Paulo
Area: 8051 km2
Urb: 1500 km2
Pop: 23 million people
Vehicles: > 6 million
Distance from the sea-shore: 70 km
Lat=-23.6o
Lon=- 46.7o
Vehicles: > 7 million
MASP= So Paulo city + 38 cities
19 million inhabitants 7,2 million vehicles 2000 significative industrial plants 8000 km2
Atmospheric Sciences Department - USP
Metropolitan Region of So
Paulo
Population:~ 20 million inhabitants.
Area: 8511 km2
Vehicular fleet: 7 million
85% light-duty fleet
55% gasohol
4% ethanol hidrated
38% flex
2% diesel
3% diesel
12% motorcycles
Atmospheric Sciences Department - USP
Important questions
Expansion of urban areas and population growth
Silva Dias et al., (2011)
Very dense urban area
Contrast between urban and suburban areas
Atmospheric Sciences Department - USP
Official Data Emission Inventory in the Metropolitan Area of So Paulo for Regulated
Pollutants
Source: CETESB Atmospheric Sciences Department - USP
Some studies in Brazil
Which are the sources of particles (PM2.5)
Importance of vehicular contribution for PM2.5
Health Impact of vehicular emission
Motivation: the health impacts of atmospheric aerosols
Inhalation of particles: asthma, increase of respiratory symptoms, pulmonary and cardio-vascular diseases.
The increase in PM concentration is associated to an increase in mortality
http://aerosol.ees.ufl.edu/atmos_aerosol/section07-2.html
Relative risk adjusted to total mortality and PM2.5 concentrations in six cities.
During two periods: 1 from 1974 to 1989 and 2 from 1990 to 1998.
P=Portage, T=Topeka, W=Watertown, L=St. Louis, H=Harriman, S= Steubenville.
Recife
Belo Horizonte
Rio de Janeiro So Paulo Curitiba
Porto Alegre
Metropolitan Area Population (million) Area (thousand km2)
So Paulo 19.9 7.9
Rio de Janeiro 11.8 5.6
Belo Horizonte 5.0 0.9
Porto Alegre 9.8 4.1
Curitiba 3.2 15.4
Recife 3.8 2.8
MP2.5
PM2.5 Std Dev Black Carbon Std Dev BC/PM2.5
So Paulo 30 13 10 6 0.33
Rio de Janeiro 19 11 3 2 0.17
Belo Horizonte 17 7 5 3 0.28
Porto Alegre 16 12 4 4 0.22
Curitiba 17 8 4 3 0.27
Recife 12 3 2 1 0.17
PM2.5 Average mass concentration July 2007 October 2008 Concentrations in g/m3
Andrade et al., 2011
0.0
0.1
1.0
10.0
Co
nce
ntr
atio
n (
ug
/m3)
Ions
Curitiba Rio Janeiro Recife So Paulo Belo Horizonte Porto Alegre
Ions composition
Mass Balance
The inorganic compounds were considered in the oxidazied form:
Al2O3, SiO2, K2O, CaO3, TiO, VO, MnO2, Fe2O3, NiO,
Cu2O, ZnO, Se, Br, Sr, Zr, Pb
+ ions
+BC
Crustal
So Paulo
Crustal Ions BC ND
So Paulo
Rio de Janeiro
Crustal
Ions
BC
ND
Rio de Janeiro Belo Horizonte
Crustal
Ions
BC
ND
Belo Horizonte
Porto Alegre
Crustal
Ions
BC
ND
Porto Alegre Curitiba
Crustal
Ions
BC
ND
Curitiba
Recife
Crustal
Ions
BC
ND
Recife
Multivariate Methods
Principal Component Analysis
Receptor Modeling
Meteorological data Air quality
Source profile
Risk Analysis
Muchas Gracias!