1. Source contributions to ambient levels of NO2 & PM in Spain (main focus BCN):
Sources and strategies to take into account for the improvement of air quality
X. Querol, A. Alastuey, T. Moreno, M. Viana, J. Pey, M. Pandolfi,
M.C. Minguillón, N. Pérez, F. Amato, M. Cusack, C. Reche, N. Moreno, J. Targa*
Institute for Environmental Assessment and Water Research, IDAEA, CSIC
Spanish Research Council, Barcelona, Spain
xavier.querol@idaea.csic.es
* 4sfera Innova, Girona, Spain
Barcelona, June 17 2010

2. OUTLINE
Air Quality: NO2 & PM in Spain
The problem and the main sources of NO2
The problem and the main sources of PM
Main strategies to reduce ambient NO2 & PM
Conclusions
EVALUATION OF AIR QUALITY (PM & NO2) IN THE
METROPOLITAN AREA OF BARCELONA
AIR QUALITY IMPROVEMENT GUIDELINES FOR SPAIN

3. ENVIRONMENTAL STRANDARDS FOR AIR QUALITY: EC
293 ° , 101,3 kPa
K
Directive 2008/50/CE except PM and metals, Evriron. Cond.
Hourly 350 µg/m3 SO2 24 times per year
Daily 125 µg/m 3 SO 3 times per year
2
Annual prot. ecos. 20 µg/m3 SO2 not exceeding annual and mean 1 Oct-31 Mar
Hourly 200 µg/m 3 NO 18 times per year
2
Annual 40 µg/m3 NO2 not exceeding
Annual prot. vegetation 30 µg/m3 NOx (reported as NO2) not exceeding
Annual 30 (5) µg/m 3 Benzene not exceeding
Mean 8-h max. in a day 10 mg/m3 CO not exceeding
Annual 500 ng/m 3 Pb not exceeding
Annual 40 µg/m3 PM10 not exceeding
Daily 50 µg/m3 PM10 n<35 per year
Anual (25 y 20 (18) µg/m3 PM ) not exceeding
2.5
2010-2020 (reducing 20% PM2.5 triennial for mean of urban background)
2004/107/CE
Annual 6 ng/m3 As not exceeding
Annual 20 ng/m3 Ni not exceeding
Annual 5 ng/m3 Cd not exceeding
Annual 1 ng/m3 α
Benzo[α]pirene not exceeding
Critical parameters (exceedances)

4. NO2 LEVELS SPAIN 2006-2008
120
120.0
Rurales y urbanas, 2006
Industriales, 2006
Estaciones de tráfico 51%
sub-urbanas y urbanas
80 80.0
NO2 (µg/m )
NO2 (µg/m )
3
3
15% Urbanas
Urbanas de fondo 4% Sub-urbanas
Rurales y regionales 8%
Rurales y regionales Sub-urbanas próximas a ciudades 6%
próximas a ciudades
40 40.0
Remotas
0 0.0
281 estaciones de vigilancia y control calidad del aire (España 2006), 23% superan el VLA 191 estaciones de vigilancia y control calidad del aire (España 2006), 4% superan el VLA
120
120
Rurales y urbanas, 2007
Industriales, 2007
51%
80 Estaciones de tráfico
rurales, sub-urbanas y urbanas 80
NO2 (µg/m )
NO2 (µg/m )
3
3
Sub-urbanas y urbanas de fondo Urbanas
Sub-urbanas
3% 12% Rurales y regionales 10%
próximas a ciudades 5%
40 40
Rurales y regionales
próximas a ciudades
Remotas
0 0
286 estaciones de vigilancia y control calidad del aire (España 2007), 22% superan el VLA 197 estaciones de vigilancia y control calidad del aire (España 2007), 4% superan el VLA
120
120
Rurales y urbanas, 2008
Industriales, 2008
41%
Estaciones de tráfico
rurales, sub-urbanas y urbanas
80 80
NO2 (µg/m )
NO2 (µg/m )
3
3
Urbanas de fondo Urbanas
Sub-urbanas
6% 8% Rurales y regionales 3%
próximas a ciudades 3%
Sub-urbanas
40 40
Rurales y regionales
próximas a ciudades
Remotas
0 0
299 estaciones de vigilancia y control calidad del aire (España 2008), 16% superan el VLA 197 estaciones de vigilancia y control calidad del aire (España 2008), 2% superan el VLA

5. NO2 MAY-JUNE 2008 (120 PASSIVE DOSIMETRES)
Levels

6. NO2 MAY-JUNE 2008
Fabra - Barceloneta
G.

7. Lo
nd
re
s
0
500
1000
1500
2000
2500
R 20
om 0 1
a
M 02
20
ad
ri d
2379
Be 20
05
rlí
n
20
M
i lá 0 6
n
M 2
1398
1226
u n 002
ic
h
797
20
Vi
en 05
Ba
rc a
el 20
o 04
Bu na
da 20
pe 0
st 6
20
617
Pr 05
ag
Va a 2
le 0
n c 04
Fr ia
an 20
06
Es kfu
to rt
20
359
co
Ám lm 05
o
st 20
er 06
da
m
Bo 20
lo 06
ni
H a
Turismos (x1000)
el 20
si 05
nk
i2
C 00
op Os 4
en lo
ha 2 0
gu 05
Very high density of vehicles (#/km2)
e
20
05
139
Ba
rc
el
o
na 0
1
2
3
4
5
6
7
20
M
ilá 06
Va n 2
le 0
nc 0 2
6.1
ia
M 2
ad 00
WHY SO HIGH NO2?
ri d 6
M
2.6
20
C un 05
op ic
en h
2.3
ha 20
gu 05
e
20
Vi 05
en
Lo a
nd 200
re 4
s
R 20
om 01
a
Be 2 0 0
rlí 2
Bo n 2
lo 00
Es n 6
to ia 2
1.4
co 00
lm 5
Fr o
an 200
kf 6
Turismos/Km 2 (x1000)
ur
t2
Pr 00
a
Bu ga 5
da 20
pe 04
st
H 20
el
Ám si n 05
ki
st
er 20 0
da 4
m
20
O 06
sl
o
20
05
http://w3.bcn.es/fitxers/mobilitat/dadesbasiques2006.222.pdf
1.0 0.4

8. NO & NO2 TRENDS 1990-2009
NOx NO NO2 %NO2/NOx % diessel fleet Prov. BCN
180 70
160
Martorell 60
140
50
120
100 40
3
µg/m
%
80 30
60 Essen-Ost: Courtesy: Prof. Dr. P. Bruckmann
20
40
10
20
0 0
1991 1992 1993 1994 1995 1996 1997 1998 1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009

9. Institute for Internal Combustion Engines and Thermodynamics
Courtesy: Prof. Dr. S. Hausberger
Measurements: type approval vs. real world for PC
1.6 1.6
NO
Diesel NEDC NO Diesel CADC (hot start)
1.4 NO2
1.4
NO2
1.2 1.2 (2015!!!!!!)
NOx [g/km]
NOx [g/km]
1.0 1.0
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0.0 0.0
EU 0 EU 1 EU 2 EU 3 EU 4 EU 5 EU 0 EU 1 EU 2 EU 3 EU 4 EU 5 EU 6
NO2 fleet emission factors in urban traffic (share in mileage for AUT)
0 .2 5 2 .5
P a s s e n g e r c a r s g a s o lin e
NO2
Passenger cars NO2 [g/km]
P a s s e n g e r c a r s d ie s e l
0 .2 HD V 2 Total effect of NOx and NO2 fleet emission
HDV NO2 [g/km] reduction may not be sufficient to reach
0 .1 5 1 .5
NO2 air quality targets near roads with high
0 .1 1 traffic volumes until 2015:
0 .0 5 0 .5
NON TECHNOLOGICAL MEASURES
0 0
1990 1995 2000 2005 2010 2015 2020 ARE URGENTLY NEEDED
I
Y ear
S. Hausberger: Brussels, 14. April 2010 9

10. PM10 IN SPAIN 2006-2008
80 80
Rurales y urbanas, 2006 Industriales, 2006 Urbanas Industriales
Sub-urbanas industriales
Sub-urbanas de tráfico 40%
Urbanas de tráfico 42%
60 35% 60
Regionales-industriales
Sub-urbanas de fondo 29%
Urbanas de fondo y próximas a ciudades-industriales
Rurales regionales 9%
27%
PM 10 (µg/m )
PM 10 (µg/m )
3
3
y próximas a ciudades
5% 6%
40 40
4%
Remotas
20 20
0 0
268 estaciones de vigilancia y control calidad del aire (España 2006), 25% superan VLA 177 estaciones de vigilancia y control calidad del aire (España 2006), 24% superan el VLA
80 80
Rurales y urbanas, 2007 Industriales, 2007 Urbanas Industriales
Sub-urbanas industriales
Sub-urbanas de tráfico
26%
60 Sub-urbanas de fondo 60
29% Regionales-industriales 21% 43%
16% Urbanas de fondo y próximas a ciudades-industriales
Rurales regionales Urbanas de tráfico
30%
PM 10 (µg/m )
PM 10 (µg/m )
3
y próximas a ciudades
3
2%
40 40
Remotas
20 20
0 0
294 estaciones de vigilancia y control calidad del aire (España 2007), 20% superan VLA 175 estaciones de vigilancia y control calidad del aire (España 2007), 19% superan el VLA
80 80
Rurales y urbanas, 2008 Industriales, 2008 Urbanas Industriales
Sub-urbanas industriales
15%
60 Sub-urbanas de tráfico 60
Regionales-industriales 13% 10%
Sub-urbanas de fondo
Urbanas de fondo y próximas a ciudades-industriales
Rurales regionales 10% Urbanas de tráfico
11%
PM 10 (µg/m )
PM 10 (µg/m )
3
y próximas a ciudades 21%
3
13%
40 40
Remotas
20 20
0 0
293 estaciones de vigilancia y control calidad del aire (España 2008), 11% superan VLA 188 estaciones de vigilancia y control calidad del aire (España 2008), 10% superan el VLA

11. SPECIFIC INDUSTRIAL AREAS WITH PM EXCEEDANCES
www.ecologistasextremadura.org

12. PM: A COMMON ORIGIN OF PROBLEMS FOR EU?
Madrid / Barcelona
Amsterdam
60
45
Direct from local
PM10 (µg/m3)
PM10 (µg/m3)
50 traffic from this Direct from local
45 40
street (T) traffic from this
40 street (T) 35
Urban background 30
15 Urban urbano (FU)
Fondo background
Regional background
Fondo regional (FR) (RB) Regional background (RB) 10
8
Continental background
Fondo continental (FC) (CB) Continental background (CB)

13. No local C sources
<3
3-5
5-7
7-10
10-15
15-18
10-12 traffic and some industrial
5-10 urban background
3- 4 in rural, regional back.
Maximal dispersion, Trade winds
OM+EC (µg/m3) PM10
Seasonal trend
JFMAMJJASOND

14. Claudia Mohr et al., 2010, EGU
Montserrat
16%
BBOA
16%
68% HOA
OOA
29% 7%
OOA BBOA
OOA levels close
Origin???
64%
HOA
Barcelona
14

15. Low re-suspension
<3
3-5
5-7
7-10
10-15
15-18 Influence from Traffic
>18 Influence from Traffic
African contribution
Mineral matter (µg/m3) PM10
Seasonal trend
JFMAMJJASOND

16. unnacounted
metals PM10/PM2.5 Kerbside station
OC+EC
µg/m3
marine
mineral Urban background
NH4+
NO3- Helsinki (1) Helsinki (1)
Rural background 14/8 µg/m3 25/12 µg/m3
nmSO42-
Sweden (3)
The Netherlands 10 µg/m3
UK (7) (6)
35/24 Berlin (5)
UK (7) 25/20 30/20 40/26 µg/m3
25/16 22/14 Berlin (5)
29/22 µg/m3
Krakow (2)
100 µg/m3
Bemantes
Spain (12) Gent (8)
24/19
Urban dust a major problem
19/14 µg/m3
Llodio in S. Europe
33/24 µg/m3 Basel (9)
28/- µg/m3 Wien (4) Illmitz (4)
53/38 µg/m3 24/20 µg/m3
1. Pakkanen et al., (2001)
Las Palmas Milano (10) 2. Marelli et al., 2006; Putaud et al., 2006
48/18 µg/m3 --/47 3. EC, 2004
4. EC, 2004
5. Abraham et al., 2001
6. Visser et al., 2001
Barcelona 48/- 7. EC, 2004
Alcobendas 28/-
47/28 µg/m3 8. Viana et al., 2006a
29/17 µg/m3
Roma (11) 37/- 9. Röösli et al., 2001
10. Rodriguez et al., 2007
Huelva
11. Perrino and Allegrini, 2006
36/19 µg/m3
12. Querol et al., 2004

17. Preliminary results
Barri Gòtic and traffic sites
8 and 4 µg/m3 NH3
NaNO3
Ca(NO3)2
NH4NO3
Major specie (excluding Canary Isl.)
EMEP
Thermal instability of NH4NO3
NO3- (µg/m3) PM10
along the year
<1
1-2 Seasonal trend
2-3
3-4
4-5
JFMAMJJASOND
>5

18. AIR QUALITY: THE PROBLEM OF DUST RE-SUSPENSION
Amato et al., 2009. Atmos. Environ.
Max. PM10 Traffic: 43%
Shipping: 3%
Industrial, 1.0,
Intrusión
2%
Fuel oil, 1.5, 3% Sahariana, 1.5,
Marino, 3.5, 8% 3%
Motores, 9.0, Fuente: Tesis doctoral
20% F. Amato CSIC-IJA
Sulfatos, 7.9,
Road dust, 6.7,
18%
15%
Dem.-res. (reg.): 20%
Mineral, 8.8, 20% Nitratos , 4.9,
11%
Max. PM2.5 Traffic: 46% Max. PM1 Traffic: 50%
Shipping: 4%
Industrial, 0.9,
Intrusión
Shipping: 5% Industrial, 0.5,
3% 3%
Sahariana, 0.9, Intrusión
Fuel oil, 0.9, 5%
Fuel oil, 1.3, 4% Sahariana, 0.3,
3%
Marino, 0.9, 3% Marino, 0.1, 1% 2%
Motores, 8.0,
27% Motores, 6.3,
35%
Sulfatos, 7.8, Sulfatos, 6.1,
27% Road dust, 2.2, 34%
8% Road dust, 0.3,
Mineral, 2.9, 10% Nitratos , 4.3, Mineral, 0.2, 1% Nitratos , 3.0, 2%
15% 17%
Demolition-resuspension (reg.): 10% Demolition-resuspension (reg.): 1%

19. ROAD SWEEPING AND WASHING: 3 experiments
2 in Barcelona, 1 in Madrid
F. Amato PhD, 2010
Me
rid
ia n
aA
v.
Glories
0 15 30
60 45
345
v.
50
330 60
40
315 75
A
30
300 20 90
10
ia
285 0 105
270 120
255
240 150
135 nc
le
225 165
210 195
180
Va
.
l Av
a
on
ag
Di

20. ROAD SWEEPING AND WASHING: 3 experiments
Rainfall ~ 1 L/m2
Duration of cleaning effect F. Amato PhD, 2010
Road cleaning
Dust load mg/m2
Deposition > Emission
Rainfall > 3 L/m2
Deposition = Emission
Abating deposition
dDL
= Dep − f ( DL )
dt
Time of recovery
Time Time of recovery
Deposition abated
EMISSION RATE DUST LOAD
mixed fleet <10µm
(mg veh-1 km-1) (mg m-2)
Abatement of other emissions (e.g. exhaust,
Barcelona 82** 8.9* demolition/construction) and washing streets in
large areas will abate deposition
Zürich 27*** 0.7
* Amato et al., (2009) ATM ENV
** Amato et al., (2010) STOTEN
***Bukowiecki et al. (2010) ATM ENV

21. BARCELONA, PM10, PM2.5 & PM1 TRENDS
Mean traffic flow in the acces roads to Barcelona
1.240.000
60
1.220.000
Total without NAF
50 1.200.000
(mean for working days)
1.180.000
40
PM10 (µg/m )
3
1.160.000
30 1.140.000
1.000.000 1.120.000
20
1.100.000
-8% 2007-2009
10 980.000 1.080.000 Ajuntament de Barcelona
1.060.000
0 1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009
30 1999 2000 960.000 2003
2001 2002 2004 2005 2006 2007 2008 2009 380000
360000
N vehicles/year
25 940.000 340000 AENA
Traffic: Barcelona airport
20 320000
PM2.5 (µg/m3)
920.000
300000
15
280000
900.000
10 260000
880.000
240000 -21% 2007-2009
5 Ajuntament de Barcelona
220000
0 860.000 200000
1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009
1999 2000 Vehicle2002 2003
2001 fleet/25000 2004 2005 Diesel
% 2006 2007 2008 2009 55
25 1
14.000
% Diesel and N of vehicle fleet*
840.000 13.500
45
-17% 2006 2007
2007-2009
1
20 1999 2000 2001 2002 2003 2004 2005 2008 2009
Tarffic: Barcelona harbours
13.000
1
35
Port de Barcelona
PM1 (µg/m3)
12.500
15
1
25 12.000
10 11.500
0
15
11.000
5 0
5 10.500
10.000
0 0
1 2 3 4 5 6 7 8 9 1 0 1 1
-5 1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009
1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009

22. BARCELONA, PM10, source apportionmentvtrends
PM 10 Aged marine aerosols
35
2003 2004 2005 2006 2007 2008 2009
30
25
µg m-3
20
15
10
5 0.70
0
PM10Primary road traffic 0.60
35
2003 2004 2005 2006 2007 2008 2009
30
0.50 Data
25
Sen's estimate
µg m-3
20
0.40
15
99 % conf. min
10
0.30 99 % conf. max
Cd
5
0 95 % conf. min
0.20
95 % conf. max
90
PM10 Mineral matter 0.10 Residual
80 2003 2004 2005 2006 2007 2008 2009
70 0.00
60
2002 2003 2004 2005 2006 2007 2008 2009 2010
µg m-3
50
40
-0.10
30
20 -0.20
10
0 Year
PM10 Ammonium nitrate
60
2003 2004 2005 2006 2007 2008 2009
50
40
µg m-3
30
20
10.00
10
0
PM 10 Fuel oil + ammonium sulphate 8.00
35
30
2003 2004 2005 2006 2007 2008 2009 Data
25
6.00 Sen's estimate
µg m-3
20
99 % conf. min
15
99 % conf. max
Sb
10
4.00
5 95 % conf. min
0 95 % conf. max
25
PM 10 Industrial emissions 2.00 Residual
2003 2004 2005 2006 2007 2008 2009
20
15 0.00
µg m-3
10 2002 2003 2004 2005 2006 2007 2008 2009 2010
5 -2.00
0 Year

23. CONCLUSIONS
• Limit and target values of NO2, PM10 & PM2.5 are exceeded, specially in areas with high
road traffic loads. A few specific industrial hotspots register also exceedances.
• The climate and urban architecture of Spanish cities favor accumulation of pollutants and
consequently special measures are needed.
NO2
• Drastic measures are needed to solve the problem. High traffic density, very high
dieselization (a high proportion are new!!), high NO2 emissions of new diesel cars are
causing this problem.
• Non technological road traffic measures (reducing the number of cars in the city
centre) are required for NO2.
PM10
• Mineral matter (road and construction dust), carbonaceous PM (exhaust) and nitrate
(exhaust reacting with ammonia) are the target components to abate.
• Drastic and non technological traffic measures are also required for PM.
• In addition to Euro standards and SCRT in buses (TMB), control of construction
emissions (works and transport of powdered material), urban ammonia, and road dust
cleaning over large areas, are the most needed PM abatement measures.
• There are still uncertainties on the origin of secondary organic aerosol (a large fraction of
the carbonaceous material).
Thank you very much for your attention !
xavier.querol@idaea.csic.es