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Atmos. Chem. Phys.

, 11, 6207–6227, 2011
www.atmos-chem-phys.net/11/6207/2011/ Atmospheric
doi:10.5194/acp-11-6207-2011 Chemistry
© Author(s) 2011. CC Attribution 3.0 License. and Physics

New considerations for PM, Black Carbon and particle
number concentration for air quality monitoring across
different European cities
C. Reche1,2 , X. Querol1 , A. Alastuey1 , M. Viana1 , J. Pey1 , T. Moreno1 , S. Rodrı́guez3 , Y. González3 ,
R. Fernández-Camacho4 , A. M. Sánchez de la Campa4 , J. de la Rosa4 , M. Dall’Osto1 , A. S. H. Prévôt5 , C. Hueglin6 ,
R. M. Harrison7 , and P. Quincey8
1 Institutefor Environmental Assessment and Water Research (IDÆA-CSIC), Barcelona, Spain
2 Institutde Ciència i Tecnologia Ambientals (ICTA), Universidad Autónoma de Barcelona, Barcelona, Spain
3 Izaña Atmospheric Research Centre, AEMET, Associate Unit CSIC “Studies on Atmospheric Pollution”, Santa Cruz de

Tenerife, Canary Islands, Spain
4 University of Huelva, Associate Unit CSIC “Atmospheric Pollution”, Huelva, Spain
5 Laboratory of Atmospheric Chemistry, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland
6 Laboratory for Air Pollution and Environmental Technology, Swiss Federal Laboratories for Materials Science and

Technology (EMPA), Dübendorf, Switzerland
7 School of Geography, Earth and Environmental Sciences, University of Birmingham, Birmingham, UK
8 Analytical Science Team, National Physical Laboratory, Hampton Road, Teddington, Middlesex TW11 0LW, UK

Received: 17 February 2011 – Published in Atmos. Chem. Phys. Discuss.: 14 March 2011
Revised: 8 June 2011 – Accepted: 21 June 2011 – Published: 1 July 2011

Abstract. In many large cities of Europe standard air quality fic emissions on urban aerosols. However, BC levels vary
limit values of particulate matter (PM) are exceeded. Emis- proportionally with those of traffic related gaseous pollu-
sions from road traffic and biomass burning are frequently tants, such as CO, NO2 and NO. Due to this high correla-
reported to be the major causes. As a consequence of these tion, one may suppose that monitoring the levels of these
exceedances a large number of air quality plans, most of them gaseous pollutants would be enough to extrapolate exposure
focusing on traffic emissions reductions, have been imple- to traffic-derived BC levels. However, the BC/CO, BC/NO2
mented in the last decade. In spite of this implementation, and BC/NO ratios vary widely among the cities studied, as
a number of cities did not record a decrease of PM levels. a function of distance to traffic emissions, vehicle fleet com-
Thus, is the efficiency of air quality plans overestimated? Do position and the influence of other emission sources such as
the road traffic emissions contribute less than expected to am- biomass burning. Thus, levels of BC should be measured at
bient air PM levels in urban areas? Or do we need a more air quality monitoring sites.
specific metric to evaluate the impact of the above emissions During morning traffic rush hours, a narrow variation in
on the levels of urban aerosols? the N/BC ratio was evidenced, but a wide variation of this ra-
This study shows the results of the interpretation of the tio was determined for the noon period. Although in central
2009 variability of levels of PM, Black Carbon (BC), aerosol and northern Europe N and BC levels tend to vary simulta-
number concentration (N) and a number of gaseous pollu- neously, not only during the traffic rush hours but also during
tants in seven selected urban areas covering road traffic, ur- the whole day, in urban background stations in southern Eu-
ban background, urban-industrial, and urban-shipping envi- rope maximum N levels coinciding with minimum BC lev-
ronments from southern, central and northern Europe. els are recorded at midday in all seasons. These N maxima
The results showed that variations of PM and N levels do recorded in southern European urban background environ-
not always reflect the variation of the impact of road traf- ments are attributed to midday nucleation episodes occurring
when gaseous pollutants are diluted and maximum insola-
tion and O3 levels occur. The occurrence of SO2 peaks may
Correspondence to: C. Reche also contribute to the occurrence of midday nucleation bursts
(cristina.reche@idaea.csic.es) in specific industrial or shipping-influenced areas, although

Published by Copernicus Publications on behalf of the European Geosciences Union.

6208 C. Reche et al.: Considerations for PM, Black Carbon and particle number concentration

at several central European sites similar levels of SO2 are contribute less than expected to ambient air PM levels in ur-
recorded without yielding nucleation episodes. ban areas? Or do we need a more specific metric to evalu-
Accordingly, it is clearly evidenced that N variability in ate the impact of the above emissions on the levels of urban
different European urban environments is not equally influ- aerosols?
enced by the same emission sources and atmospheric pro- A number of studies have reported a strong association be-
cesses. We conclude that N variability does not always re- tween BC and road traffic (Hamilton and Mansfield, 1991;
flect the impact of road traffic on air quality, whereas BC is Watson et al., 1994; Pakkanen et al., 2000) and biomass burn-
a more consistent tracer of such an influence. However, N ing (Sandradewi et al., 2008) emissions. While BC aerosols
should be measured since ultrafine particles (<100 nm) may are not the only cause of adverse health effects due to parti-
have large impacts on human health. cles, they are a major factor, specially the ultrafine BC. In-
The combination of PM10 and BC monitoring in urban deed, the recent WHO report concludes that “combustion-
areas potentially constitutes a useful approach for air qual- derived aerosols are particularly significant in terms of their
ity monitoring. BC is mostly governed by vehicle exhaust health effects” (WHO, 2003).
emissions, while PM10 concentrations at these sites are also On the other hand, number concentrations in urban ar-
governed by non-exhaust particulate emissions resuspended eas are also highly influenced by primary vehicle exhaust
by traffic, by midday atmospheric dilution and by other non- emissions (Morawska et al, 2002; Bukowiecki et al., 2003;
traffic emissions. Hueglin et al., 2006; Rodriguez and Cuevas, 2007, Pérez
et al., 2010). These emissions show bimodal size distribu-
tion, with a nucleation mode below 30 nm and a carbona-
ceous mode peaking between 50–130 nm (Morawska et al.,
1 Introduction 1998, Casati et al., 2007). Therefore, a number of studies
pointed out that exposure to road traffic emissions may be
Health impact of ultrafine particles (UFP) has motivated a properly evaluated by combining ambient air measurements
great deal of ambient aerosol research in recent years. Sev- of Black Carbon (BC) with N concentrations (Fischer et al.,
eral studies suggest that UFP disproportionately induce ox- 2000; Harrison et al., 2004; Janssen et al., 1997; Smargiassi
idative stress in cells and are more toxic compared to larger et al., 2005; Rodriguez and Cuevas, 2007), since nowadays
particles of similar composition (Li et al., 2003; Nel et al., these parameters seem not to be properly controlled by air
2005). Research studies have indicated that fine particles quality limit values.
may be more toxic because a large proportion of these par- Although most of UFP in urban atmospheres are related
ticles are derived from traffic-related, industrial, and do- to vehicle exhaust emissions, its origin may be both primary
mestic emissions which contain abundant transition met- and secondary (Wehner et al., 2002; Dunn et al., 2004; Van
als (Anderson et al., 2001; Klemm et al., 2000; Schwartz et Dingenen et al., 2004). Gaseous pollutants from vehicle ex-
al., 2002; von Klot et al., 2002). Furthermore, UFP have also haust may yield a high aerosol production depending on the
been suggested to be more toxic because of the large surface ambient air conditions. For example, Casati et al. (2007) ob-
area available for biologic interactions with lung cells (Chio served that low ambient temperature and high relative hu-
et al., 2008). Epidemiological studies (Akinson et al., 2010; midity favour secondary formation processes, while Shi and
Stolzel et al., 2007) have shown a clear association of urban Harrison (1999) associated these processes with high dilution
nanoparticle exposures with adverse cardiovascular health after the emission. Furthermore, Wehner et al. (2009) re-
outcomes. ported evidence on the fact that under high engine load con-
Because of the low influence of UFP on PM mass con- ditions a favourable setting for secondary particle formation
centration (the current metric used in European air quality is given within short distance of the exhaust plume. Such
legislation), the number concentration (N) can be a better de- conditions (e.g., acceleration) are typical of urban driving.
scriptor of the variability of UFP. In fact, the combination These particles in the vehicle exhaust mainly comprise or-
of number and size distribution of N may elucidate on the ganic compounds and sulphuric acid and are frequently one
primary or secondary production of these UFP. of the most important fractions in terms of number concen-
In many large cities of Europe standard air quality limit tration (Kittelson et al., 1998).
values of PM are exceeded. Emissions from road traffic New secondary particle formation in ambient air is mostly
and biomass burning are frequently reported to be the ma- attributed to nucleation and cluster/particle growth by con-
jor causes of such exceedances (EEA, 2010). As a conse- densation of photo-oxidised vapours (Morawska et al., 2008;
quence of these exceedances a large number of air quality Dunn et al., 2004) occurring some time after the emis-
plans, most of them focusing on traffic emissions, have been sion (hours to days). The outcome of UFP depends widely
implemented in the last decade. In spite of this implemen- on the pollutants concentrations in the air, thus when the ur-
tation, a number of cities did not record a decrease of PM ban atmosphere is highly polluted, the semi-volatile species
levels. Thus, the question remains: is the efficiency of air condense onto pre-existing particles (Wichmann et al., 2000;
quality plans overestimated? Do the road traffic emissions Zhang et al., 2004; Imhof et al., 2006); however, when low

Atmos. Chem. Phys., 11, 6207–6227, 2011 www.atmos-chem-phys.net/11/6207/2011/

Pérez et al.C. – A southern-European urban background site ife and Huelva (Pey et al. industrial and shipping emissions.. 26 Once created. BCN) characterized by a very dense Fernández-Camacho et al. studies have confirmed that the growth rate depends 2 Monitoring sites on temperature and concentration of available condensable vapors (Kulmala et al.: Considerations for PM. Boy et patterns were selected for the study. 2008. the sig. Both factors favor nucleation processes. ur.. 2009.. 2008.. enhancing the nucleation 21 22 processes. In other cases such as Beijing. Reche et al. 2010. Seven monitoring sites situated in six major European gested that H2 SO4 condensation typically accounts for about cities (Fig. but the especial focus on the process of formation of secondary UFP significant increase in wind speed can be responsible for a with high influence on the variability of N. 1. Cheung et 30 31 Figure 1 al. ing sites also cover a relatively wide range of road traffic den- ciding with sea breezes blowing inland have recently been sity. Cheung et al. urban architecture and fleet composition (Table 2): observed in the urban background of coastal cities in south- western Europe. The combination of the oxidation products of SO2 23 and VOCs are ideal for efficient nucleation (Metzger et al. the semi-volatile species may re. with this process. the develop. Rönkkö et al. Fernández. 2006). as well road traffic network. 6207–6227. 1997.. daily formation of – A north-European urban background site (North Kens- nucleation mode particles was coincident with the arrival of ington. but also by the influence of as in Brisbane. 2002. whereas VOCs account for more than 70 % of the cities/sites intended to cover different climatic zones across material for the particle growth.net/11/6207/2011/ Atmos. Moore et al. Black Carbon and particle number concentration 6209 PM pollution levels occur. The follow- tions. BC. Park et al. Pey tween urban sites under a variety of emission sources and et al. 2007). ability of levels of N. Elevated so. 2004). Location of the six cities selected in the present study. pled with growth. In some cases it has been sug. 2011 . 2010. In case of coastal 16 17 cities. – Two urban traffic sites situated directly at the kerbside erning differences in the secondary formation of particles be. industrial and urban-shipping-influenced sites). At coastal urban sites.. 18 nificant SO2 emissions from shipping may be transported to. Europe (central. 10 11 lar radiation intensities not only provide enough energy for 12 gaseous precursors to nucleate.. as well as The daily cycle of N evidences significant differences urban environments (urban background and traffic. 24 25 2010).. 1 2 sult in large numbers of nucleation-derived aerosols (Hämeri 3 et al. 2005. Cheung et al. Gao et al. Thus. 2005. Chem.... high dilution of the condensable gases involved in growth. and (2) nucleation cou. Santa Cruz de Tener.. 11. 2007.. urban- when comparing cities with distinct meteorological condi. Phys. central-Europe). 2009) and further climate/geographic conditions... such as Barcelona. 2010). 2009. 13 14 cesses as a result of the growing of the mixing layer and the 15 activation of mountain and sea breezes. 2010): (1) burst of nucleation particles without subse- quent growth into larger particles. 1996. The selection of the al. 2007. 9 Camacho et al. the main goal research is needed to elucidate the occurrence of this process of this paper is to study the causes responsible for the vari- in urban environments. 2009. Daily N cycles showing new particle formation coin. As previously reported.. such as Barcelona and Santa Cruz de Tenerife. In this context... nucleated particles may undergo different 27 28 processes in the atmosphere (Boy and Kulmala. 2008. but favour the dilution pro. 2009..atmos-chem-phys. The increase in knowledge of UFP has not been accompa- nied by more in-depth research about the main factors gov. tial area 7 km to the west of central London. Rodrı́guez et al... PM and gaseous pollutants at a ment of sea breezes (enriched in SOx ) simultaneously with selection of air quality monitoring sites representative of dif- the highest solar radiation could be probably related with ferent climate zones and urban environments in Europe. Australia (Mejia et al. UK. www. 7 8 Moore et al. 1) with different climatic and meteorological 10–30 % of the observed growth (Weber et al. Fig.. Park et al. of very busy roads: Bern (Switzerland. Gao et al. Factors governing the evolution of nu- cleated particles without subsequent growth are not well- documented (Johnson et al. 4 5 ban areas with high solar radiation intensities are favourable 6 scenarios for nucleation processes (Johnson et al. western and southern Europe). 2010). NK) in the grounds of a school in a residen- cleaner air masses (Zong-bo et al. 2008. (Barcelona.. Qian 29 et al. 2009. 19 20 wards the city with the sea breeze. Pey et al. 2010)... 2007... 2005).

selected: namism around Barcelona account for the highest road traf- fic density of Europe (6100 cars km−2 . being influ. Basin. with a mean traffic density of 132 000 vehicles/day. This is sited in the grounds of Sion Manning School mulated precipitation is 500 mm.s. London has a population of 7. This site is classified as a roadside site.). As de Tenerife. of one of the largest arterial roads of the city. 2004).7 million inhabitants. The instruments are in a cabin The transport and dispersion of atmospheric pollutants and sampling inlets are less than 5 m from the road. Measurements were carried out at an urban background 00◦ 120 4800 W. breezes (originating from the 120–180◦ sector) are at their strongest around midday. North Kensington.l. tial area. making it the largest in the European Union (Wikipedia. Local within BCN are controlled mainly by fluctuating coastal PM10 emissions are strongly dominated by the heavy-duty winds which typically blow in from the sea during the day vehicles that represent less than 10 % of the traffic (Charron and. HU) highly influenced by the emissions from a large in. Reche et al. The NK site is located about 4 km to the west of enced by vehicular emissions from one of the city’s main MR site. The traffic density in London in 2009 was 1317 reg- – A subtropical island urban background site (Santa Cruz istered vehicles km−2 of which 1134 km−2 were cars. when the boundary layer height 2. Atmos. 68 m a.1 Barcelona. over 80 000 vehicles/day pass the site on six lanes with fre- breaks reach the Barcelona area in the order of 7–10 events quent congestion.s. 2005). Barcelona has one of the main harbours in the rounding area is a street canyon frequented by pedestrians Mediterranean Basin. The daily pattern of the boundary layer height shows maximum Barcelona is located in north eastern Spain (41◦ 230 05◦ N. but it is located in a city with very high road traffic.). As shown in Table 1. 2011 www. London is characterized by a lower pro- lane road running along the shore. shown in Table 1.6210 C.1 London.atmos-chem-phys. 27 m a. whilst the Greater dustrial estate including copper metallurgy. 27 m a.2. motorbikes. The sur- Furthermore. mobility. with influence of the portion of diesel cars. Marylebone. North Kensington (51◦ 310 1600 N. 2010). mean solar radiation is 70 W m−2 . 11. from the land during the night.8). a wide range of inten. The surrounding buildings form an asymmetric street area. which are very often transported of days with concentrations above the limit value was ex- across the city by sea breeze. surrounded by a mainly residen- monitoring site located in southwest Barcelona. and influenced by the emissions – A central-European urban background site (Lugano. in St Charles Square. contributing to decrease atmo- 02◦ 070 09◦ E. Chem. Traffic flows of In addition to the local PM emissions. with a major frequency in the summer and winter– site due to the presence of traffic lights 50 m to the west and spring periods (Rodrı́guez et al. an intersection to the east. and a large side of a major arterial route in London that is heavily proportion of the use of private cars for the daily mobility. Finally. canyon (height-to-width ratio of about 0.). Switzerland.l.s. with the highest number of cruise ships because of tourist attractions and shops.9 mil- ical and fertilizing plants.3 and 13. in the western Mediterranean spheric pollutants concentration. and traffic avenues. The urban architecture and dy. Phys. from 12:00 to 15:00 UTC.2 London. NK maximizes (Pérez et al. less strongly. The annual accu. LUG) situated in a park in the south of the Alps. High PM10 con- for tourists in Spain. petrochem.. 2.net/11/6207/2011/ .2. Spain.. northern-Europe). with For the present study two air quality monitoring sites were about 1. located at approximately a distance of 300 m Marylebone road in London (UK. The sea and Harrison.: Considerations for PM. Barcelona is characterized by a high proportion The London–MR monitoring site is located on the kerb- of diesel cars. London metropolitan area has between 12. heavy duty vehicles. being a significant focus of emissions centrations are measured at MR and the permitted number of atmospheric pollutants. with dense traffic) with values ranging from 5 to 760 W m−2 at midday.. 2001). 00◦ 90 5500W. 2. heavy duty vehicles. The average annual solar (urban background) radiation is 180 W m−2 and at midday values range between 400 and 950 W m−2 within a whole year. three natural gas power stations and The MR supersite belongs to the London Air Quality Net- two city waste incinerators are also based in the metropolitan work.2 London (urban background and traffic sites) – A southern-European urban background site (Huelva. SCO) on the western side of a 4. BCN (urban background site in a city On an annual basis. motorbikes. It is the tenth most populous city in Europe. lion. and emissions from a nearby large harbour and an industrial. Black Carbon and particle number concentration with a traffic density of 25 000 vehicles/day. much more than in 2. Saharan dust out. ceeded in 2005.6 million. 6207–6227. the site is an urban background one. also low proportion of the use of private cars for the daily petrochemical estate. sive industrial activities. Thus. with a traffic density of 80 000 vehicles/day. Braking is frequent near the measurement per year. MR (urban traffic site) most European cities with 1000–1500 cars km−2 ). trafficked (51◦ 310 96◦ N.l.

ch. 11.dgt. Bern is of Bern including neighbouring communities has a pop. UK) 00◦ 090 5500 W 51◦ 310 9600 N 27 Urban traffic Huelva (ES) 05◦ 560 2400 W 03◦ 150 2100 N 10 Urban industrial Santa Cruz de Tenerife (ES) 16◦ 180 3300 W 28◦ 290 2000 N 52 Urban background 2. UK: http://www. Report. 08◦ 570 2600 E. The monitoring site is located in a busy southern foothills of the Alps (46◦ 000 4000 N.bfs.3 Bern. c Department of Transport. The city lies at the edge of Lake Lugano at the 1700 mm per year. 28b 41c 18e 12f 1g ? Pedestrian 32b 21c 47e 40f 52g ? Fleet Motorbike 29b 4c 18e 16f 7g 6g Passenger and LDV 63b 93c 77e 81f 87g 87g Bus 2b 1c 1e 1f 0. Cruz % Diesel fleet 45a ? 17d 17d 55a 24a % New cars diesel 70a 33c 30d 27d ? ? Commuting Private car 40b 37c 35e 48f 45g ? Public T. 281 m a.C. d Swiss Federal Statistical Office: http://www.bve.). 6207–6227. duty vehicles.l. Bern (urban traffic site) The economy of Bern is dominated by public authorities and small and medium sized enterprises from different sectors.ch. high proportion of motorbikes.be. Chem. Main information about the monitoring sites selected for the study. Features of fleets and commuting of the 6 selected cities.s.s.) Station type Barcelona (ES) 02◦ 070 3300 E 41◦ 230 5500 N 80 Urban background Lugano (CH) 08◦ 570 2600 E 46◦ 000 4000 N 281 Urban background North Kensington (London.l. Spain: http://apl. UK) 00◦ 120 4800 W 51◦ 310 1600 N 27 Urban background Bern (CH) 07◦ 260 2700 E 46◦ 570 0400 N 536 Urban traffic Marylebone Road (London. Bern: http://www.net/11/6207/2011/ Atmos.s. Altitude Longitude Latitude (m a.uk. f www.html. however. As shown in Table 1. 2.) and is surrounded by three mountains with www.es/IEST2.4 Lugano.admin.4g HDV 3b 1c 1e 1f 3g 4g Other 2b 1c 3e 2f 1g 2g a Dirección General de Tráfico.l. Table 2.atmos-chem-phys. Barcelona London Bern Lugano Huelva Sta. The urban area emissions or air pollutants. Bern is the capital of Switzer. Black Carbon and particle number concentration 6211 Table 1. g Oral communications from local councils. land and the Canton of Bern.: Considerations for PM..tiresia. b Baldasano et al. The city is located north of the Alps in the Swiss plateau (46◦ 570 0300 N. LUG (urban background site) 536 m a.125 million and the There are. The accumulated precipitation in the city is about munity.gov. Attending to the typical meteorological fea- ture.ch/bve/de/index/mobilitaet/mobilitaet verkehr/mobilitaet/grundlagen mobilitaet. no major industries with especially high fourth most populous city in Switzerland. characterized by a low proportion of diesel cars and heavy ulation of 0. the mean annual solar radiation is 130 W m−2 and it Lugano is a city with 55 000 inhabitants and a total of ranges from 15 W m−2 in winter to 840 W m−2 in summer 145 000 people living in Lugano and the neighbouring com- at noon. (2007). Phys. e Ecoplan (2007) Auswertung Mikrozensus 2005 für den Kanton Bern. street canyon in central Bern (20 000–30 000 vehicles/day). 07◦ 260 2700 E.dft.2g 0. 2011 . Reche et al.35 million. Bern is a city with a population of 0.

2008). The Punta del Sebo Industrial The urban scale transport of air pollutants in Santa Cruz de Estate includes the second smelter factory in Europe. The driguez et al. Measurements were carried out at an urban background There are no major important industrial sources of air pollu. 2011 www. with a maximum of 1200 W m−2 at midday in curs in a petroleum refinery. 6207–6227.. Shipping emis. SO2 . Black Carbon and particle number concentration elevations of around 1000 m a. Inland breeze blowing starts at 08:00 UTC acid. NOx . and also by city of Huelva. buildings protect the site and industrial emissions) from direct road traffic emissions towards all other wind di- Santa Cruz de Tenerife is a city with around 0. Phosphoric acid production plants are also installed light (3–4 m s−1 ) and a slight seaward (eastward) airflow at in this industrial estate. It is located 2.: Considerations for PM. and is characterised by an abrupt shift in wind direction (Ro- sions may be expected from these industrial activities. 11. This sea breeze favors the centrations can be partly derived from the instrumentation. Phys... monitoring station belongs to the air quality network of the Precipitations are frequent. 2007). 2004). As shown in Table 1.. The measurement site in Lugano represents an urban back- ground situation. Rodrı́guez et al. 16◦ 180 3300 W. SO2 ) affecting the enced by vehicle exhaust and harbour emissions.. About 50 m to the east is background site under the influence of shipping a busy urban road (CorsoElvezia). phosphoric night (1 m s−1 ). 52 m a. HU (urban background site influenced by at the bottom of the southern slope of the Anaga ridge and industrial emissions) the eastern slope of the NE to SW ridge crossing the Is- land. The closest roads 3800 mm per year. about 54 natural Saharan dust events occur tions such as North African dust outbreaks. in ozone concentrations (Millán et al. nual average.s. coinciding with the maximum height of the mixing hydrocarbons. aged 2009 data were collected for each parameter and moni- graphic settings. This emissions from the Lombardy region. Chem. As.g. vatory. 6◦ 570 0◦ W. Ni and V. Zn and Sn emissions are well docu. with an accumulated value of Autonomous Government of Andalusia. Reche et al. In addition to the typical urban emissions (with a haust emissions (with a low proportion of diesel cars). lie about 500 and 1000 m to the west and the east of the mea- erage.223 rections.atmos-chem-phys. emis- high proportion of diesel cars). Lugano northeast corner of the city of Huelva. million population located in the Canary Islands – Spain (28◦ 290 200 N.l. and heavy duty vehicles and a high proportion of motorbikes.net/11/6207/2011/ . H2 SO4 . the emissions from a petrochemical estate. southern airflows linked to ther. This is a coastal urban background site mainly influ- port of aerosols and their precursors (e. Mean solar radiation is 150 W m−2 on av. at midday this parameter is between 3 and 900 W m−2 .15 The main sources of pollutants in the city are: vehicle ex- million. 7 km from Punta del lies close to the Italian border and is strongly influenced by Sebo and 14 km from Nuevo Puerto industrial areas. reaching average values of 1200 W m−2 on Data on the instrumentation deployed at the different sites is an hourly basis at midday.s. Solar radiation is 250 W m−2 on an- most important air pollutant emissions in Nuevo Puerto oc. Pb. layer. 2007. 2007). local emissions. This area is characterized by a dry weather. This breeze SO2 . Measurements were performed in the Santa Cruz Obser- In all these cases sea-to-land winds result in the inland trans. At night. sulphuric acid and sodium silicate atmospheric emis. resulting in emissions of volatile summer. where two large industrial es. However.l. 2. sions occur also in the important industrial harbor of Huelva.). The dispersion and transport of summarized in Table 3. SCO (urban versity of Lugano in the city center. near the harbor of Huelva. For the present study hourly aver- air pollutants in this area are highly influenced by the topo. with 3 Instrumentation a yearly accumulated rainfall of 450 mm.l) and has a population of around 0. the wind mostly blows from the toring site. Sb. The solar radiation is very elevated. NH3 . The site is located on campus of the Uni. annual frequency of this natural phenomenon is calculated to be 19 % of days in southern Spain (Sánchez de la Campa et al. The PM10 >100 µg m−3 (Viana et al. often resulting in generalized increase in mass levels of particulate matter.. is characterised by inland (westward) airflows during day- mented. The boundary Lugano is characterized by a low proportion of diesel cars layer height maximizes from 12:00–15:00 UTC. winds (NNE) that blow over the ocean (Guerra et al. on the tants within the close vicinity of Lugano. 2002). surement site.. which produce a along the year (Alonso-Pérez et al.6 Santa Cruz de Tenerife. aerosol precursors are emit.6212 C. entry of industrial plumes and is associated with an increase The latter were measured with a total of three models of Atmos. This topographic setting protects the city from the trade Huelva is located south western Spain (37◦ 150 0◦ N. both and Cuevas. 54 m a. In addition to the The city of Huelva is also affected by natural PM contribu. It is relevant to note that differences in BC and N con- mally driven breezes predominate. north and during daylight. 2002). NH+4 and Na phosphate.5 Huelva. where Tenerife is mainly driven by breeze circulation. 2008)..s. sions of ships and cargo operations in the harbour and an oil ted at the south of the city. refinery located in the southern side of the city (Rodrı́guez tates are located: Punta del Sebo and Nuevo Puerto. monitoring site placed at the University Campus.

but it would not alter the trends described. in lowest N/BC ratios. 2007. Black Carbon and particle number concentration 6213 Condensation Particles Counters (CPC) which counted parti. As regards BC. with an annual average bone (19. including the industrial site (with the highest in the different cities. the correction of BC values with local EC concentrations car.7 µg m−3 ) and SCO (0. respectively. els of BC were very high in MR.8 µg m−3 and decrease down to 3.7 vert the observed light attenuation to the mass concentration to 1. As in this study. 11.77) and the slope of ences in meteorology and by considering the importance of the regression line was 0.9 in Bern. Bigi and Harrison.. On the other hand. showed a value puts (Szidat et al. in order to perform an accurate comparison be. plants around London. LUG and NK) and (3) urban back- in BCN. the use of 6×106 particles ng−1 BC.6 m2 g−1 is recommended by the manufacturer to con. biomass burning emissions in Lugano and coal fired power the calculation of the experimental absorption coefficients. The use of CPCs with differ. with the exception of MR different instrumentations can still affect the seasonal trends (2. (2) urban back- results showed average absorption coefficients of 9.7) and closed to it in North Kensington (16. This fact may be explained by differ- ington (r 2 = 0. because of interferences of oxidized nitrogen compounds ent cut sizes is likely to influence the results somewhat. N/BC ratios range from 6 to On the other hand. 2007). pounds. 10.C. It is important to note that the ratio PM10 /BC BC (µg m−3 ) = σap (M m−1 )/σ (m2 g −1 ) (1) is higher at urban background sites (9–18) than at traffic where σap are the absorption coefficient measurements in sites (4–8) due to the relative prevalence of secondary com- M m−1 . Chem. different parameters. experimental groups: (1) traffic stations (MR and Bern). Nevertheless. in Thermo Optical Transmittance technique (Birch and Cary. 2010). the Aethalometer (Magee AE 21) mea. Table 4 lists the 2009 average values of 1996) using a Sunset Laboratory OC-EC analyser and the de..1 in LUG. resulting converters (Steinbacher et al.net/11/6207/2011/ Atmos. 6207–6227. BC) and SCO (15×106 particles ng−1 BC). 10. Regarding gaseous pollutants instrumentation. and also sea salt in SCO. This influence could modify the N/BC levels). levels are almost equal. 5 nm (TSI tant to mention that NO2 measurements can be overestimated 3785) or 7 nm (TSI 3022A). 12. As regards N. Thus. exhaust emissions. Phys.86) and Marylebone (0.8 µg m−3 ) recorded the low- experimental absorption coefficients (σ in m2 g−1 ) accord. Thus.2 m2 g−1 ground stations (BCN. despite differ- of BC. Reche et al. The reasons be- lations between BC and EC measurements considering the hind these unusually low and high N/BC ratios will be dis- whole year were significant in all the sites under study. with this range increasing to 22 000–28 000 cm−3 ratios calculated in this work for the different periods of the at traffic sites due to the direct impact of primary day. Levels of BC at urban background sites range from 1. www. The absorbance is converted to the mass concentration of BC using a fixed mass absorption co. as a in the conventional instruments equipped with molybdenum largest cut size can imply an underestimation of N. 16. LUG and NK. al.. butions of dust.19.8×106 particles ng−1 BC). BC concentrations were determined using the HU (0. the Multi-Angle Absorption Photome- ter (MAAP) (ThermoTM . carbon (EC) for high volume samples of 24 h by means of the with the influence of shipping and industrial emissions. expected.3 in HU and 9. However.3). it is impor- cles larger than 2.1 Levels of atmospheric pollutants at two different angles.6 m2 g−1 ) in Maryle. These experimental conversion factors were used Average levels of PM10 range from 18 to 32 µg m−3 .6 m2 g−1 rec.atmos-chem-phys. high correlation coefficients were obtained ences in percentages of diesel vehicles between sites. in spite of this correction.5 µg m−3 in Bern. of 7. HU (25×106 particles ng−1 of light absorbing carbonaceous aerosols..: Considerations for PM. 2010). Lev- higher than the recommended one (16. 2011 . ac- Therefore. the highest values (27–32 µg m−3 ) were registered On the other hand. Results were obtained by in situ determining elemental ence in the case of HU and subtropical island conditions. which contribute to increase BC out- by means of the determination of EC.. cordingly with the lower vehicle flow. In 2009.9 µg m−3 in BCN. cussed in the following sections.8 in ground stations with special characteristics (industrial influ- SCO. BC between BC mass and EC concentrations in North Kens.97 and 1. est concentrations of BC owing to a lesser impact of traf- ing the equation by Petzold and Schönlinner (2004) (1): fic in these smaller cities and favourable dispersive condi- tions (SCO). tween sites. Maximum values of this ratio are observed in HU Although the influence of possible coatings of BC particles and SCO (26–33) as a consequence of the important contri- by organic materials has not been taken into consideration. the case of SCO). 2009 averages ranged from 12 000– ried out in this study favours the comparability between BC 18 000 cm−3 . 2010) of 6. for kerbsides and also in the BCN urban background site. stations have been classified into three ommended by the manufacturer. model Carusso 5012) instrument 4 Results and discussion calculates absorbance from particles deposited on the filter using measurements of both transmittance and reflectance 4. due sured at 880 nm and a mass absorption cross section of to its proximity to one of the largest arterial roads of the city. corre. the parameters measured in each station during the sampling fault temperature steps of the EUSAAR2 program (Cavalli et period.5 nm (TSI 3025 and TSI 3776). For the analysis and description of the trends observed for the efficient at 637 nm (Müller et al.

6 1. Data from the air quality instrumentation working during the sampling period.5 0.1 0.9 3.1 0.2 0.4 2. Black Carbon and particle number concentration Table 3.net/11/6207/2011/ .1 0. 11. Dev Max Min Average St.7 1.6 1.1 Number of particles (n cm−3 ) 17 918 13 929 67 949 1091 12 008 7002 26 294 1076 SO2 (µg m−3 ) 9 5 27 3.3 0.5 Number of particles (n cm−3 ) 28 032 13 650 93 078 8888 22 156 12 910 58 017 4753 SO2 (µg m−3 ) – – – – 6.3 0.2 NO2 (µg m−3 ) 42 12 72 15 16 8 40 4 36 17 83 10 CO (mg m−3 ) 0.0 1.5 0.7 13 1. Dev Max Min Average St.2 O3 (µg m−3 ) 49 25 76 15 26 17 70 2 36 17 83 10 Bern Road Site Marylebone Road Site Average St.8 0.5−10000 ) SO2 (µg m−3 ) UV fluorescence UV fluorescence UV fluorescence UV fluorescence UV fluorescence UV fluorescence NO.1 4 3 15 0.4 7.8 2. NO2 .4 14 11 56 1.2 0.1 NO2 (µg m−3 ) 23 16 94 4.4 7 4 21 0.6 NOx (µg m−3 ) 54 25 128 14 233 78 439 86 NO (µg m−3 ) 27 19 89 5 106 27 178 49 NO2 (µg m−3 ) 24 7 42 10 127 53 261 29 CO (mg m−3 ) 0.3 O3 (µg m−3 ) 17 11 43 3 13 7 34 5 Huelva Urban Industrial Sta Cruz Tenerife Urban Shipping Average St.7 3.8 0.6 3. maximum and minimum concentrations of atmospheric pollutants (b) vehicle fleet information and ratios of atmospheric pollutants in the units derived from those in (a). Maximum values between stations are in bold.3 7. Average values of the main parameters measured in each site under study: (a) average.6 0.04 0.7 14 2.4 NOx (µg m−3 ) 32 20 136 4. Dev Max Min Average St.6 0.3 8.5−10000 ) 3776 (N2. 2011 www.7 NOx (µg m−3 ) 58 27 163 17 25 18 80 4.5 1.2 0..2 0.8 0.8 0.: Considerations for PM. Reche et al. Dev Max Min PM10 (µg m−3 ) 27 9 57 11 32 7 51 16 Black Carbon (µg m−3 ) 3.4 2.4 0.2 2.4 0.3 7.1 0. Dev Max Min PM10 (µg m−3 ) 23 9 58 6 21 7 34 7 Black Carbon (µg m−3 ) 0.3 0. CRUZ DE KENSINGTON TENERIFE PM10 (µg m−3 ) PM optical Reference Reference Reference Reference PM beta attenuation PM optical counters Grimm equivalent beta equivalent equivalent beta equivalent monitor (FAG FH-62) counters labortechnik measures TEOM-FDMS measures TEOM-FDMS Grimmlabortechnik GmB & Co.4 46 22 112 13 NO (µg m−3 ) 16 17 97 2 8 10 47 0.0 1. Dev Max Min PM10 (µg m−3 ) 30 7 60 12 23 7 40 12 18 6 30 7 Black Carbon (µg m−3 ) 1.7 1.1 0.2 7. (a) Barcelona Urban Background Lugano Urban Background North Kensington Urban Background Average St.02 O3 (µg m−3 ) 61 22 107 24 27 7 79 11 Atmos.7 0.7 0.3 0.8 Number of particles (n cm−3 ) 16 847 5117 29 449 6140 14 945 9750 47 562 2751 12 134 5810 27 295 792 SO2 (µg m−3 ) 3.1 1. 6207–6227.9 0.atmos-chem-phys. Chem.6 0.6214 C.7 1. BARCELONA LUGANO NORTH BERN MARYLEBONE HUELVA STA.1 7 4 18 0.2 NO (µg m−3 ) 7 5 30 0.1 1.9 0. models measures measures GmB & Co 1107 and 1108 Black Carbon Multi-angle Multi-angle Magee AE-21 Multi-angle Magee AE-21 Multi-angle Multi-angle (µg m−3 ) absorption absorption Aethalometer absorption Aethalometer absorption absorption photometer photometer photometer photometer photometer (MAAP Thermo (MAAP Thermo (MAAP Thermo (MAAP Thermo (MAAP Thermo ESM Andersen ESM Andersen ESM Andersen ESM Andersen ESM Andersen Instrument) with Instrument) with Instrument) with Instrument) with Instrument) with PM10 inlet PM1 inlet PM1 inlet PM10 inlet PM1 inlet Number of particles WCPC TSI model CPC TSI model CPC TSI model CPC TSI model CPC TSI model CPC TSI model CPC TSI model (n cm−3 ) 3785 (N5−1000 ) 3022A (N7−1000 ) 3022A (N7−1000 ) 3022A (N7−1000 ) 3022A (N7−1000 ) 3776 (N2.8 0.3 0.3 13 7 39 0.7 2. Dev Max Min Average St.2 1. Phys.1 CO (mg m−3 ) – – – – 0. NOx Chemiluminescence Chemiluminescence Chemiluminescence Chemiluminescence Chemiluminescence Chemiluminescence Chemiluminescence (µg m−3 ) CO (µg m−3 ) IR absorption IR absorption IR absorption IR absorption IR absorption IR absorption O3 (mg m−3 ) UV absorption UV absorption UV absorption UV absorption UV absorption UV absorption UV absorption Table 4.4 0.

(b) BCN LUG NK Bern MR HU SCO Vehicles km−2 6100 1400 1500 1600 1500 620 1100 NO2 /BC 24.2 6.2 7. with NO2 measurements can be overestimated because of inter- the exception of LUG (5).. differences in pat- 0.1 NOx /BC 34 14 24 16 30 45 17 CO/BC 0. to fresh road traffic emissions. tion of O3 by NO. and MR (14).1 9.7 0. with higher concentrations in BCN. In fact.4 0.5 to 0. the ratio NOx /CO in- site of MR (6.9 16. The same in Europe (Chaloulakou et al. with a more pronounced peak land. radiation intensity. from 0.. instruments equipped with molybdenum converters (Stein- ally NO levels.7 0.1 0. between traffic (0. the emission factor of SO2 from road relatively low levels (7 µg m−3 ) due to the good ventilation vehicle engines is 11.2 0. the variability of CO/BC ratio does not as a direct consequence of high industrial emissions and solar reflect the composition of the vehicle fleet in each city.2 to 0.1 9. NO2 concentrations reach Emission Inventory. Bern and SCO values ranged between 143 and 188. HU and SCO. while minimum values are obtained in MR (90). In SCO. fertilizer and oil refinery industries.0 PM10 /BC 18 13 9 8 4 33 26 N/BC 9910 8303 6386 8009 2840 25 598 15 010 N/SO2 5265 9341 4494 – 3307 1948 3431 NO2 /NOx 0. It should be noted that NO/BC ratio ranges from 7 to 10 in most of the sites. ground sites and 27–106 µg m−3 at the traffic ones.0 NO/BC 9.2) and urban background sites (2–3).5 0..7 µg m−3 ). probably related to the higher percentage of diesel vehicles (with en- hanced primary NO2 and NOx emissions) in fleet. the highest levels being recorded at MR.4 mg m−3 at urban background sites and from despite certain evidences described above. due to the emissions from a large copper mary emissions. Continued. 2008). 2007) and seem to be inde- trends were observed for CO concentrations.: Considerations for PM. O3 concentrations range between 26 and burning in Lugano is also indicated by the diurnal cycle of 49 µg m−3 at urban background stations.7 0. In LUG. increasing BC but not proportion. Levels at HU were the highest (61 µg m−3 ) On the other hand.7 mg m−3 at traffic locations. 2011 .0 19. with 1.8 µg m−3 (LUG) and 3.6 7. tern emissions of gasoline and diesel vehicles are not clearly tant reflects proximity and intensity of the traffic flow. NO2 concentrations ranged from 24–127 µg m−3 . At traffic sites. values are lar results have been reported in previous studies in nearby about 13–16 µg m−3 as a consequence of a major consump- regions (Sandradewi et al. smelter. These values are in the order of those obtained in other sites est values were registered for LUG. with the highest ground stations.2µg m−3 ). 6207–6227. NO2 levels mostly represent the pri- at HU (9.5 Kilotonne Mt−1 fuel consumed) and conditions on the island.2 NO2 /NO 2. 2005).2 3.9–1.9 1. 11.1 – 0.net/11/6207/2011/ Atmos. The shown in the stations under study.7 0. Phys.2 4.. which ranged pendent of the percentage of diesel vehicle in the fleet.2 1. Reche et al.5 µg m−3 (SCO) in the urban back.3 32. creases with the proportion of diesel vehicles and is very sions (according to data from the UK National Atmospheric similar in BCN and NK. as a direct effect of exhaust emis.0 2.. Thus.8 0. as this gaseous pollu. Black Carbon and particle number concentration 6215 Table 4. The low.5 NOx /CO 144 82 153 109 333 – 88 O3 levels (leads to faster NO oxidation to NO2 ) and the very elevated car density (6100 cars km−2 ).6 9. including on the is- CO and PM concentrations.atmos-chem-phys. NO2 levels reached 16–42 µg m−3 at the urban background environments.8 13. Simi. Very high values are measured at BCN. as a result of in the evening than the one obtained for NOx levels. SO2 levels reach between sites. higher www. ferences of oxidized nitrogen compounds in the conventional ence of biomass burning. an intense photochemical activity.2 0. At the traffic Concerning gaseous pollutants. probably due to a higher influ. imum values are recorded for BCN (235). 2007). Max. Maxima SO2 levels were recorded at the traffic don (Carslaw et al. NK.7 2. as a result of the proximity bacher et al. Chem. The influenced of biomass Finally.2 0. Marked differences in the NO2 /NO ratio are only found NO concentrations reach 7–16 µg m−3 at urban back.C. The slightly higher levels measured at BCN traffic flow (80 000 vehicles day−1 ) and probably also to a and SCO are caused by the significant influence of shipping significant proportion of diesel in the vehicle fleet of Lon- emissions.6 10.

0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) 1117 Hour (UTC) 1118 1119 Fig.0 45000 N (>5nm) BC N (>7nm) BC N (>7nm) BC Number of particles (n/cm 3) 3. Reche et al. 6207–6227.0 10000 5000 0.5nm) BC N (>2. O3 (µg/m3) 100 CO (mg/m3). 2b.5 25000 2. 1116 b) 50000 4.5 15000 1.0 35000 30000 2. Black Carbon and particle number concentration 1114 a) 120 100 BCN LUG NK 90 CO*100 (mg/m3).6216 C. 1121 1122 1123 1124 Atmos. Daily cycle of: gaseous pollutants concentrations (CO.5 Black Carbon (µg/m 3 ) 40000 3.5nm) BC Number of particles (n/cm ) HU SCO 3. 2011 www.net/11/6207/2011/ 1126 1127 1128 .1125 Phys.5 15000 1. 2a.0 35000 30000 2. Chem.5 25000 20000 2. O3 (µg/m3) 100 80 70 80 NOx (µg/m3) 60 60 50 40 40 30 20 20 CO*100 NOx O3 CO*100 NOX O3 CO*100 NOx O3 10 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) Hour (UTC) 120 100 350 100 BERN 90 MR 90 300 CO (mg/m3).0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) Hour (UTC) 50000 6 50000 12 N (>7nm) BC Number of particles (n/cm ) N (>7nm) BC 3 Number of particles (n/cm ) 45000 45000 3 5 10 Black Carbon (µg/m3) 40000 40000 Black Carbon (µg/m3) 35000 35000 4 8 30000 30000 25000 3 25000 6 20000 20000 2 4 15000 15000 10000 10000 1 2 5000 BERN 5000 MR 0 0 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) 50000 4.5 0 0. Daily cycle 1120 of: Black Carbon (BC) and Number concentration (N) levels for each monitoring site.0 45000 N (>2. 11.0 20000 1.0 10000 0.5 3 Black Carbon (µg/m 3) 40000 3.5 5000 BCN LUG NK 0 0.0 38 1. NOx and O3 ) levels for each monitoring site..atmos-chem-phys.: Considerations for PM. O3(µg/m3) 80 80 70 250 70 NOx (µg/m ) 80 NOx (µg/m ) 3 3 60 200 60 60 50 50 150 40 40 40 30 30 100 20 20 20 50 10 10 CO*100 NOX O3 NOx CO*100 O3 0 0 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) 120 100 100 CO*100 NOx O3 HU 90 SCO 90 100 CO (mg/m 3). O3 (µg/m3) 80 80 70 70 80 NOx (µg/m ) 3 O3 (g/m3) 60 60 60 50 50 40 40 40 30 30 20 20 20 NOx O3 10 10 0 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) 1115 Hour (UTC) Fig.

2011 . NOX and O3).0 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 1142 Hour (UTC) Hour (UTC) 1143 Fig.5 20 2.5 20 15 10 1. Chem. Daily cycle of: a) Gaseous pollutants concentrations (CO.: Considerations for PM. 11. 6207–6227.net/11/6207/2011/ Atmos.0 50 35 BC PM10 BC PM10 3.5 30 20 2.C. Phys..0 25 PM 10 (µg/m 3) 2. 1144 d) 50000 7 45000 BCN LUG NK Number of particles (n/cm ) 3 6 40000 35000 5 SO 2 (µg/m 3 ) 30000 4 25000 3 20000 15000 2 10000 N SO2 1 5000 N SO2 N SO2 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) Hour (UTC) 50000 12 45000 MR Number of particles (n/cm ) 3 10 40000 35000 8 SO2 (µg/m3) 30000 25000 6 20000 4 15000 10000 2 5000 N SO2 0 0 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) 50000 14 7 45000 HU SCO 40 Number of particles (n/cm ) 12 6 3 40000 35000 10 5 SO 2 (µg/m 3) SO2 (µg/m3) 30000 8 4 25000 6 3 20000 15000 4 2 10000 2 1 5000 N SO2 N SO2 0 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 1145 Hour (UTC) Hour (UTC) 1146 Figure 2.0 BC PM10 5 0.5 HU 45 SCO 30 40 Black Carbon (µg/m ) 3 3. 2c.5 5 5 0.atmos-chem-phys. and d) N and SO2 levels for 1148 each monitoring site.0 25 15 1.0 35 3. Black Carbon and particle number concentration 6217 1141 c) 4. Daily cycle (BC)for SO2 levels andeach Number concentration monitoring site.5 10 1. 2d. b) Black 1147 of: carbon Fig.0 35 25 PM 10 (µg/m 3) PM10 (µg/m3) 2.5 BC PM10 BC PM10 0.0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) Hour (UTC) 6 35 12 50 45 5 30 10 Black Carbon (µg/m ) Black Carbon (µg/m ) 40 3 3 25 35 4 8 PM10 (µg/m3) PM (µg/m 3) 30 20 3 6 25 15 20 2 4 10 15 10 1 2 BERN BC PM10 5 MR BC PM10 5 0 0 0 0 0 2 4 6 8 10 12 14 16 18 20 22 0 2 4 6 8 10 12 14 16 18 20 22 Hour (UTC) Hour (UTC) 4. c) BC and PM10. www.0 10 0. Reche et al.0 15 1.5 BCN LUG NK 30 Black Carbon (µg/m 3) 3. Daily cycle of: BC and PM10 levels for each monitoring site. (N).

con. reach. Pérez et al. and the traffic similar pattern of N and meteorological parameters (global flow. mixing layer. a behaviour induced by the of particles by means of photochemical nucleation processes continuous supply of fresh oceanic air masses coupled with from gaseous precursors. This phenomenon is Bern. the growth of the The same daily evolution described for NOx and CO is fol. 2007). winds blow inland from the Atlantic Ocean carry- and CO follow the diurnal pattern of traffic intensity.. the seaward transport of aged particulate pollutants. 2010. atmospheric OH concentrations correlate well with UV so- ies (Querol et al. NOx reflects emissions from diesel vehicles. While CO emissions are a tracer of gasoline ternoon rush-hours (07:00–09:00 and 17:00-20:00 UTC) are vehicles. with N being mainly possible explanation of the tendency above is the major pres. The occurrence of nucleation events at midday in fact that the BC and the gaseous pollutant monitors were not BCN was supported by means of an SMPS (scanning mobil- co-located. but instead were distant by approximately 150 m ity particle sizers) working during the international DAURE on opposite sides of the road.. The evolution of O3 levels shows a typical diurnal pattern.net/11/6207/2011/ . ing emission plumes with gaseous pollutants from industrial ing a maximum during the morning rush hour (07:00– estates (Sánchez de la Campa et al.. Furthermore. One may think that there is no need to measure BC lev. the instrumentation can also be responsible for the dissimi- centrations increase at midday when sea breezes transport larities. For all sites levels of NOx (NO2 + NO) daylight. Reche et al. The BC monitor was located campaign in 2009 (http://cires. In contrast.colorado. Peaks of N and BC at morning and af- all the stations. Sulphuric acid has been identified as a key nucle- the re-suspended mineral material from the city towards the ating substance in the atmosphere (Curtis et al. The opposed trends of ing (Fig. HU and SCO. This lack resuspended by traffic. low an opposite trend since 11:00 UTC. At SCO O3 daily pat. where the second peak of BC is produced earlier than not observed in the selected northern and central European expected. but of secondary formation lar to those registered at midday.atmos-chem-phys.. BC levels traced accurately the impact of ve. N in the evening show slight delays. with levels at night simi. where the decrease of N at midday was in the order of in Bern is still unclear. 2005).php/DAURE) when it was observed that the in- toring stations. accounting for 09:00 UTC). more marked in BCN and Bern but the tendency is equal for Cheung et al. spheric dilution processes. the density of vehicles. influenced by primary aerosols and by the formation of new ence of delivery HDV and LDV and of school buses in the particles during the dilution and cooling of the vehicle ex- morning. and increasing again in the N is also an appropriate tracer of traffic emissions in cer- evening (17:00-20:00 UTC). however. decreasing during the day because of atmo. when lower temperatures stant from the morning until the evening peak due to the ef.. haust emissions (Mariq et al. and lower mixing heights occur. where the sec- by vehicle exhaust emissions. Similar results were reported in earlier stud. Because UV Atmos. Black Carbon and particle number concentration 4. 2c). but it has been reported to be highly in- CO/NOx is observed comparing the evening peak with the fluenced by photochemically induced nucleation (Pey et al. which may be interpreted as secondary Fig. at BCN.. During lutants for each site. 2005. In all the other moni. Querol et al. Because of the proximity to roads. photochemistry and vertical dilution. 1998. 2010. S4). radiation.. Charron and Harrison. daily patterns of BC and N fol- The combination of PM10 and BC in urban areas poten. Chem. This midday nucleation takes place low local NO levels. The different location of fects of resuspension processes. 2011 www. the increase in wind speed and the consequent lowed by levels of BC (Fig. While BC daily cycle is mostly determined BC and N are specially significant in Bern. particles formed in the evening. Harrison et al... PM10 concentrations in HU reach the highest values at night due to Figure 2a shows the 2009 average daily cycle of gaseous pol. PM10 levels at the traffic sites remained nearly con. Fernández-Camacho et al. N shows a second peak with an increase at midday coinciding with the maximum at midday. Phys. The cause for the anomalous hourly trend detected cities. 2a and b). 2c). the different daily cycle of PM and gaseous pollutants. els if this aerosol component follows the variability of CO. wind speed. 11. lar radiation (Rohrer and Berresheim.: Considerations for PM. 2010).. confirming that this peak could not be a consequence of pri- terns differ from the above trend.. 2009). 2006). one recorded at morning rush-hours.6218 C. 2001. PM10 concentrations at these ond peak of BC is registered earlier than in the rest of sta- sites are also governed by non-exhaust particulate emissions tions and is about 40 % lower than morning peak. as a consequence of the high solar radiation. wind direction and boundary layer). In the case of traffic sites. although it is possibly related to the that of BC. 2006) as monitoring site. An increment of the ratio tain environments. except in the case of decrease of pollutants concentrations. mary emissions from road traffic. 2007. so that the peaks of tially constitutes a useful approach for air quality monitor. 6207–6227. simultaneously occurring with the BC decrease.2 Temporal variability of atmospheric pollutants 2001. Wehner et al. it was estimated that results regarding nucleation episodes NO and NO2 . by midday atmospheric dilution and of parallelism between N and BC is due to a source of N by other non-traffic emissions (see LUG and NK patterns in other than traffic.edu/jimenez-group/ closer to road traffic and to a railway. crement of N at midday was caused by a marked increment of hicle exhaust emissions on air quality. In the case of BCN. so a coincident in all the stations studied. 7–32) indicate that BC should be measured. This phenomenon is 2008. increasing with the nucleation mode particles (N5−20 ) (Fig. wiki/index. differences among sites in the ratios from Barcelona could be extrapolated to these sites in south- CO/BC (ranging from 90–235) and NO2 /BC (ranging from Europe.

S3). shows that the daily evolution was not the same at weekends 3 Fig. 1 0 10000 0 tion of particles at midday in the southern European cities 8 7 70000 60000 6 NK under study. the northward in. 2004. However. at LUG. Phys. 4. O3 levels are associated with processes of long- trations hinder condensation and coagulation processes but range transport and they show the typical spring maximum favour nucleation activated by photochemistry. 6207–6227. 2002. Fruin et al. emissions (Zhu et al. SO2 levels in BCN attain a 8 7 70000 60000 6 BERN 50000 maximum from 9:00 to 13:00 UTC and around 10:00 UTC 5 4 40000 30000 3 in SCO. 3) 1 2 Figure 3. and thus in these cases this pollutant may be at. confirming the potential for secondary forma. This fact highlights the direct depen- atmospheric pollution) for secondary aerosol formation by dence of O3 and N on photochemistry. NK and HU. 1 0 10000 0 On a weekly scale.. N scatter plots were analysed for four differ- pected. 0 16 0 70000 tributed to shipping emissions. Black Carbon and particle number concentration 6219 radiation has not been measured continuously at most of the BC N stations. coinciding with the higher dispersive con.3 BC/N relationship: similarities and differences with levels remaining relatively steady during the whole year. NOx declines in summer are also evident in BCN. polluted with SO2 from power 4 3 30000 2 20000 plants (Bigi and Harrison. breezes drive harbour emissions across 2 1 20000 10000 the city. 2007. 60000 6 LUG 50000 5 40000 4 160 in MR. 3. are higher in of these two parameters has been studied for each site using summer. those periods with maximum N at midday registered for BCN. increasing ent periods of the day (Fig. but maximum levels are 8 70000 registered at midday due probably to the convective mixing 7 6 SCO 60000 50000 5 40000 of upper tropospheric layers. SO2 concentrations are directly 7 6 HU 60000 50000 5 dependent upon exhaust emissions. because the morning road traffic maximum disappears. 5271 in HU and 3 2 30000 20000 1259 in SCO. SO2 (µg m−3 ). CO and NOx concentrations follow the same seasonal Different behaviours were observed depending on the time of trend described above for BC and N (Fig. Low pollutant concen..atmos-chem-phys. 1994). In NK the diurnal cycle 2 1 0 10000 0 is also highly influenced by traffic. SCO accounts for the maximum values urban environments owing to the impact of vehicle exhaust in summer probably due to major maritime traffic intensity. nucleation processes to take place. Chem. At SCO. 1103 in BCN.: Considerations for PM. 107 in LUG. and a relatively smoother daily evolution in aerosol concentra- tions during daylight was observed. In BCN and HU. 5 4 50000 40000 30000 Daily trends of SO2 levels in BCN. Lower PM. compared with the hourly average. the day. reaching higher values 4 3 40000 30000 20000 with increases in traffic volume. Reche et al. www. The degree of correlation and SCO. Mean values of the product 8 7 70000 at midday (11:00-14:00 UTC) were 171 Wµg2 m−8 in NK.. 2011 . the study of the daily evolution of N 0 4 8 121620 0 4 8 121620 0 4 8 121620 0 4 8 121620 0 4 8 121620 0 4 8 121620 0 4 8 121620 Hour (UTC) and BC for each day of the week and each station (Fig. S1). BC vs. O3 (µg m−3 ) and 4 3 40000 30000 H2 Ov (g Kg−1 ). the methodology described by Rodriguez and Cuevas (2007). Daily cycle of BC and N for each day of the week. S2). Daily cycle of: BC and N for each day of the week.. a seasonal trend for BC and N levels is not detected in stations with a direct influence of traffic (Fig. HU and SCO (especially concentrations of O3 match with those of maximum concen- marked on Sundays) due to the favourable conditions (low trations of N at midday. 2010). 8 70000 2010). N and BC during the months with the highest solar radiation intensi- levels at weekends are responsible for the sharper peak of ties (Fig.net/11/6207/2011/ Atmos. By contrast. 14 12 MR 60000 50000 10 land breeze blowing during the afternoon favours the inland 8 6 40000 30000 transport of the SO2 plumes over the city and the mixing of 4 2 20000 10000 0 0 urban and industrial pollutants (Fernández-Camacho et al. HU and SCO suggest 3 2 20000 Number of particles (n/cm3) 1 10000 a significant source of this pollutant different from vehicle 0 0 Black Carbon (µg/m3) exhaust emissions (Fig. 11.C. we use the global intensity of solar radiation (SR) 8 Monday Tuesday Wednesday Thursday Friday Saturday Sunday 70000 as its proxy with the purpose of obtaining the product of 7 6 BCN 60000 50000 5 solar radiation (W m−2 ). HU Cuevas. 4). In LUG and MR. This product was used as a surrogate pa. At this time. 2d). Rodrı́guez and As expected. 2 20000 1 10000 0 0 rameter for H2 SO4 production. across Europe However. specifically: 07:00–09:00.. Parallelisms between BC and N are repeatedly observed in ditions. In HU. Furthermore. Pérez et al. the N peaks at midday registered in BCN. 2010). concentrations are much lower in summer. As ex. O3 levels present an opposite tendency. of the subtropical latitudes (Oltmans and Levy.

4–4. presence of gaseous precursors (mainly SO2 ) to the condi- tions that favour nucleation.4 in HU. The 18:00–21:00 UTC period rep.0 1.0 0 3. The tion found for central Europe. Figure 5 shows the correlations between the mean annual At any time and for all the stations. sity reduction. HU and SCO. in- rush-hours.0 0. It is evident that ratios. hourly levels of N and BC for the above S1 ratios (Table 5) ter plots are grouped between two defined lines with slopes during the periods 07:00–09:00. Daily cycle of BC and N for each month. specially sig.1– Number of particles (n/cm3) 5000 0 0 Black Carbon (µg/m3) 8 7 100000 90000 80000 4. Black Carbon and particle number concentration BC N This analysis of the relationship between BC and N is per- January February March April May June July August September October November December 4 35000 30000 formed assuming that BC in urban areas is an accurate tracer 3 25000 2 20000 15000 BCN of primary traffic emissions.1 × 10 particles ng −1 BC in SCO and 3.: Considerations for PM. These factors result in a dilution of at.2 of biomass burning emissions during winter. 11:00–14:00. 6 11. with persistently high exhaust emissions.5 30000 25000 to occur. observed increases in N/BC ratios up to reach the maximum during these diurnal periods the cities from central Europe S2 value are caused by means of enhancements in the new and UK are aligned along a very well fitted regression line particle formation rates during the dilution and cooling of between BC and N.3 106 particles ng−1 BC in HU and 9. with the lowest values registered at the traffic sites. 18:00–21:00 S1 and S2 representing the minimum and maximum N/BC and 01:00–03:00 UTC for the different sites. The first period stands for the traf. S3). southern Europe differ markedly from the general correla- haust emissions per each nanogram of ambient air BC. resulting in similar N/BC sity.1– mospheric dynamics. It is important to note that 5 4 30000 25000 dissimilarities are partly caused by the selection of CPC 3 2 20000 15000 NK model at each location. diurnal (07:00–09:00 and 11:00-14:00) N-BC patterns for imum number of primary particles arising from vehicle ex. promotes condensation processes. 18:00–21:00.3×106 particles ng−1 BC in the rest of stations). respectively (Fig. As expected. In MR.0 30000 0.7 × 106 particles ng−1 of these time ranges is determined by variations in pollu. This dilution is enhanced by the devel- 2.7 106 particles ng−1 BC for most of the sites. In spite of the traffic inten- nificant at north and central European locations. 106 particles ng−1 BC in SCO. highlighting the lower relevance of secondary aerosol at this mospheric pollutants. although fic rush-hours. 6220 C. values are slightly higher at 18–21 h at most of the sites. 8. the ratio ranges between centrations in the order of those registered in the morning 3.atmos-chem-phys.0 1. Fur- 0. however. The selection those ratios at 07:00–09:00 UTC (5. S1 ranges 3. Phys. the decrease of the height of the mixing layer the night period is characterized by the lowest traffic inten.net/11/6207/2011/ . since higher the cut size of the in- 10000 1 strument is.0 0 4 Hour (UTC) thermore. 2011 www. At night (01:00–03:00 UTC). mainly governed by emission patterns and at.7 × 106 particles ng−1 in HU. the N/BC ratios is reached. lower the N/BC ratio will be. At 11:00–14:00 UTC there is an increase in the height of probably due to a major gas to particle transfer of matter the mixing layer and the highest solar radiation intensity by condensation and/or nucleation.1×106 particles ng−1 BC in central and north European 6 5 4 70000 60000 50000 40000 BERN cities. 5 6 Figure 4. blue symbols) along the line is dependent on the traffic flow Atmos. The formation of secondary particles by nucleation 2.5 20000 10000 these factors sets a favourable scenario for nucleation events 0. the influence of shipping emissions in these cities. The ratio. with higher N/BC trend. accounting for the highest exhaust emissions. 5. BC in BCN. causes a concentration of pollutants. expressed in 106 particles ng−1 BC.6 in SCO and 28.5 60000 50000 40000 HU opment of sea breezes in coastal cities. the N versus BC scat. The combination of 1. Reche et al.0 2.5 in BCN.. South European 12 10 8 50000 40000 30000 MR cities recorded the highest solar radiation just occurring when 6 4 2 0 20000 10000 0 the atmospheric dynamics result in the highest dilution of 2. tant levels. A similar approach was used by 10000 1 0 5000 0 Turpin and Huntzicker (1995) to differentiate primary and 5 4 50000 45000 40000 secondary organic carbon 3 2 35000 30000 25000 20000 LUG Important differences in S1 are observed between sites 15000 1 0 10000 5000 0 at 11:00–14:00 UTC (Table 5). The position of these cities (black and the vehicle exhaust emissions and/or in ambient air. 15. increases to 3 30000 2 20000 1 10000 0 0 16 14 70000 60000 6. Daily cycle of: BC and N for each month. and sea breezes. Finally. with pollutant con. the decrease of the height of the mixing layer ratios as those calculated at traffic rush-hours.5 10000 5000 09:00 UTC to 11:00–14:00 UTC in BCN. this period is also characterized by the influence creasing to 8.5 80000 70000 pollutants (midday). 4.5 20000 15000 SCO might account for the marked increase of S1 from 07:00– 1. 11. together with an important industrial source in HU. resents the evening traffic rush hours. adds the Fig. with the consequent development of mountain measured at 7–9 h and at 18:00–21:00 h are very similar. Chem. S1 is interpreted as the min. S1 at 18:00–21:00 UTC is in the order of 11:00–14:00. 6207–6227. Thus. site. 01:00–03:00 UTC.

9 4.2 22. sidering S2. 11:00–14:00.5 20.1 4. where: pounds (VOCs) from residential wood combustion may lead to significant secondary non-fossil organic aerosols in winter N1 = S1 × BC (2) as suggested to be important in Zürich (Lanz et al.5 22.4 Differences in primary emissions and nucleation afternoon (18:00–21:00 UTC).7 18.1 4.1 5..5 4 4.. Chem. Phys.3 19. since volatile organic com.1 6. N daily trends are similar As regards S2. (3) Similar ratios have been reported in previous studies in with N being the total number concentration.3 8.9 13. and as a suitable European cities seem to fit the same regression line with a indicator of the dynamics of the atmospheric mixing layer. 1165 N(n cm−3 ) /BC(ng m−3 ) S1 S2 07:00–09:00 h 11:00–14:00 h 18:00–21:00 h 01:00–03:00 h 07:00–09:00 h 11:00–14:00 h 18:00–21:00 h 01:00–03:00 h BCN 5. hourly 18-21 and levelsforoftheNdifferent 1-3 h (UTC) and BC forsites. where the maximum ratio at 18:00–21:00 and mainly at 01:00– In order to quantify the sources and processes contributing to 03:00 UTC is higher than in the rest of central and north UFP.4 SCO 9. 2008) and in Roveredo (Lanz et al.9 56. N2 = N − N1.6 3. 11.1 HU 8. 18:00–21:00 and 01:00–03:00 (UTC) for the different study sites. This could be attributed to the influence the methodology described by Rodrı́guez and Cuevas (2007). However.1 9.6 4.1 3.5 and proximity to roads as well as meteorological dispersion. central and north European cities.1 10.7 8. HU and SCO is more marked when con.7 3.4 20.2 226.7 Bern 3. Dur. 2011 . In Bern. the enhancement of N/BC enced by the occurrence of nucleation processes induced by at midday in BCN.4 LUG 3. photochemistry at midday.8 41.9 23.6 11. N2 accounting www. 1162 1163 Table 5.9 15.7 28.9 18.atmos-chem-phys. cle formation contributions result in a strong correlation be- with a clear positive slope. whereas in south Europe. particle number concentration data were analysed using European sites.3 54.7 4. imum primary emission of vehicle exhaust.6 3. the observed trends are almost the same as to those of BC. periods mean annual 11-14. 2010).6 14.5 18. During intensity.: Considerations for PM.5 3 3.0 MR 2. study the periods 07:00–09:00.5 3 3 BC (µg/m ) BC (µg/m ) 1159 1160 Figure 5. Correlation between: 1161 (a) the 7-9.7 24.2 17. N is highly influ- those described for S1.4 35. N1 the min- Milano (Rodriguez and Cuevas. Correlation between: a) the mean annual hourly levels of N and BC for the Fig. 44 some periods there seems to even be a negative slope. 2007). of biomass burning emissions.C. Values of S1 1164 and S2 representing the minimum and maximum N/BC ratios for each site.4 14.5 1 1.3 3. Reche et al. where the new parti. The results indicate that BC is an appropriate tracer for the ing the nocturnal periods both northern-central and southern intensity and proximity of traffic emissions.9 3.2 3. Such is the case of LUG.9 10. an increase of S2 is produced in the 4. the southern European tween the diurnal cycle of N/BC ratio and the solar radiation cities (red symbols) are well off this regression line. Black Carbon and particle number concentration 6221 1158 45000 40000 40000 7-9h 11-14h 35000 35000 30000 Southern Europe 30000 25000 25000 20000 20000 15000 15000 10000 10000 N(particles/cm ) 3 5000 5000 0 0 0 2 4 6 8 10 12 0 2 4 6 8 10 12 45000 30000 40000 18-21h 1-3h 25000 35000 Bacelona 30000 20000 Lugano 25000 15000 Kensington 20000 Bern 15000 10000 Marylebone 10000 5000 Huelva 5000 SCO 0 0 0 2 4 6 8 10 0 0. 6207–6227. In positive slope. 5.5 104.5 5..5 NK 3.1 8.4 8. since the peak of BC is pro- enhancements across European cities duced earlier than expected.net/11/6207/2011/ Atmos.3 44.5 2 2. However.7 5.9 6.1 71.

The value increases to 54 % in NK. indicating 5000 0 no dependence on exhaust emissions of N2 at midday (BCN. as a consequence of the impor. This association between in. factors such as solar radiation intensity and dilution (favour- cursors.net/11/6207/2011/ . representing secondary parts from gaseous pre. and S1 the minimum N vs. In south European cities. 45 % in higher than those registered in BCN and SCO) and the very Bern and to 78 % in MR.: Considerations for PM. 2.6222 C. respectively. Spearman rank cor- SO2 from a source different than traffic exhaust emissions. 2002). 60000 3 HU. mainly due to one registered in LUG in winter (38 %). maybe as Considering the relatively high concentrations of SO2 at a direct consequence of SOA formation from biomass burn.2 at LUG. in an increased boundary layer height.6 Number of particles (n/cm ) Number of particles (n/cm) Number of particles (n/cm ) Number of particles (n/cm ) Number of particles (n/cm) 14000 3 12000 at NK and Bern. This is cles inherited in the air mass). N1 (minimum primary emis. primary parts from non-traffic sources. These percentages are quite similar to the a mean daily basis (66–80 %) during Sundays. 11. BC representing the Black Carbon con. MR (with an average concentration at midday about 70 % ing emissions. Values 2500 0 of S1 (expressed as 106 particles/ngBC) of 3. high primary N load obtained. and (3) the input of To further confirm this hypothesis. it can be stated that higher tant and consistent traffic impact. NK and MR). an increase of N2 not coinciding with N1 20000 10000 is also observed in NK possibly related with the midday 0 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 SO2 increase from power plants. and (c) inherited particles present in 0 3 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 22500 the air mass. 5. resuspension. was 45000 40000 35000 used) and (2) the influence of the ambient air conditions on 30000 Bern 25000 the new particle formation during dilution and cooling of the 20000 15000 C vehicle exhaust. Black Carbon and particle number concentration for: (a) secondary particles formed in the atmosphere by ho. 30000 HU Nonetheless. Fig. Daily cycle of: N1 and N2 for each day of the week 45 sion of vehicle exhaust) accounts for 46. 7 nm. concentrations of SO2 are not enough to achieve an enhance- a 64 to 85 % N2 contribution is observed at midday (11:00– ment of the secondary N load. Chem. which receives anthropogenic emissions in a 20000 17500 given point in time. BC slope observed 10000 7500 5000 during the morning rush hours (07:00–09:00 UTC). (2) the dilution of pollutants tions (Charron et al. 6. 25000 SCO 20000 15000 creases of N and power plant emissions has been observed in 10000 5000 previous studies (Brock et al. Phys.atmos-chem-phys. and/or parti. 0 3 40000 ery day of the week. HU and SCO. Reche et al. It is a consequence of the described 50000 40000 nucleation processes favoured by photochemistry. 2011 www. around two hours be- 3 45000 40000 fore (12:00 UTC) as a result of the downward mixing upper 35000 30000 tropospheric layers (Fig. These differences in the S1 values are 8000 NK 6000 caused by: 1) the use of different CPC models (with different 4000 2000 cut sizes) at different sites (the lowest S1 values are observed 0 3 at the sites where the CPC with the largest cut size. 8. 3.7 in HU and 9.9 10000 in SCO were used.. 10000 5000 Figure 6 shows hourly average values of N1 and N2 for ev. 0 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 0 6 12 18 Table 6 lists the total average percentages of N1 and N2 1166 Hour (UTC) 1167 Figure 6. 38 and 46 % of the total N during the whole sampling period in BCN. 2007). SCO. 15000 LUG 12500 centrations.. Daily cycle of N1 and N2 for each day of the week and the average percentage at midday (11:00-14:00 UTC) on an hourly basis for each station. ing decreases in PM levels) appears to be essential. but the combination with other 14:00 h UTC. 2d). 15000 12500 BCN (b) primary particles from other sources different to traffic 10000 7500 such as biomass burning. As previously reported this supported by the observation of frequent nucleation events high N2 load is caused by the combination of 3 processes: at the rural Harwell (UK) site with lower SO2 concentra- (1) increased solar radiation.. significantly lower the lower levels of atmospheric pollutants. relation (ρ) tests were used to assess the relationship be- These high N2 loads are also obtained in the same cities on tween N2 and different factors. Differences between sites are marked.9 at MR. 25000 MR 20000 cles of N1 and N2 at midday (LUG and Bern) and stations 15000 10000 with a clear decoupling of the two components. Monday Tuesday Wednesday Thursday Friday Saturday Sunday N1 N2 mogeneous nucleation or other heterogeneous reactions from Number of particles (n/cm ) Number of particles (n/cm3) 20000 17500 gaseous precursors arising from traffic or any urban source. 6207–6227. specifically: N2 vs.1 at BCN. SO2 * Atmos. residential emissions 5000 2500 and biogenic emissions. 35000 30000 observing two different patterns: stations with parallel cy. than the percentage obtained in summer (53 %).

by HU (ρ = 0. and urban. such as CO.atmos-chem-phys. coupled with increases in the mix.atmos-chem-phys. % BCN LUG NK Bern MR HU SCO N1 46 39 54 45 78 38 47 N2 54 61 46 55 22 62 53 N1 (11:00–14:00 h UTC) 31 41 45 49 91 15 36 N2 (11:00–14:00 h UTC) 69 59 55 51 9 85 64 solar radiation intensity. direction and velocity.C. Due to this high corre. causes the dilution of atmospheric pollutants. However. wind direction on an hourly basis. However. Chem.01. tend to vary simultaneously. toring. 2008). 2004. The coefficient for the same sions. The occurrence of SO2 peaks may also contribute to the incidence of midday nucleation burst in specific industrial or 5 Conclusions shipping influenced areas. BC/NO2 and BC/NO Supplementary material related to this ratios vary widely among the studied cities. Although in central and northern Europe N and BC levels ing layer high. not only during the traffic rush favouring nucleation processes (Ketzel et al. urban-industrial. test resulted lower than 0. This change in wind variation of this ratio was determined for the noon period.20 in north and central European A subsequent question is focused on the evaluation of the sites. lutants are diluted and maximum insolation and O3 levels oc- cur. particle num. Phys. Therefore. while a wide mote the development of sea breezes. Thus.86). urban background. 6207–6227.. one may suppose that monitoring the levels of these gaseous pollutants would be enough to extrapolate exposure to BC levels. BC is a relevant indicator for the im- pact of anthropogenic emissions at a measurement site and should therefore be measured in air quality monitoring net- works. BCN (ρ = 0. The combination of PM10 and BC in urban areas po- tentially constitutes a useful approach for air quality moni- www. potential toxicity (Pérez et al.78) with midday atmospheric dilution and by other non-traffic emis- a level of significance of 0. although at several central Euro- pean sites similar levels of SO2 are recorded without yielding This study shows the results of the interpretation of the 2009 nucleation episodes. while PM10 concentrations at these sites are also governed by tween N2 and SO2 * solar global radiation were obtained in non-exhaust particulate emissions resuspended by traffic. Reche et al.. NO2 and NO. imum N levels coinciding with minimum BC levels are usu- According to the results obtained it is clearly evidenced ally recorded at midday.. quality in southern Europe. The results indicate a narrow variation of primary road that enhancements in solar radiation intensity directly pro. whereas BC is a more consistent The results show that the variations of PM and N levels tracer of such influence. from southern. 11. N2 vs.67) and SCO (ρ = 0. biomass burning. Black Carbon (BC). the vehicle fleet compo. as a function article is available online at: of the distance to traffic emissions. lation. wind velocity and N2 vs.. variability of levels of PM. we conclude that N vari- shipping environments. Thus. N should be measured do not always reflect the variation of the impact of road since ultrafine particles (<100 nm) may have large impacts traffic emissions on urban aerosols. However the BC/CO. it is known BC.pdf. reach the cardiovascular and cerebrovascular systems and the lutants.net/11/6207/2011/ Atmos.net/11/6207/2011/ sition and the influence of other emission sources such as acp-11-6207-2011-supplement. atmospheric processes. traffic N/BC ratios during traffic rush hours. BC levels on human health based on the very fine grain size that may vary proportionally to those of traffic related gaseous pol. Total average percentages of N1 and N2 and average percentages at midday (11:00–14:00 h UTC) on an hourly basis. Nevertheless. According to the results obtained it is clearly evidenced ber concentration (N) and a number of gaseous pollutants that N variability in different European urban environments at seven selected urban air quality monitoring sites covering is not equally influenced by the same emission sources and road traffic. BC is governed by vehicle exhaust emissions. 2009). http://www. 2011 .: Considerations for PM. Lee et hours but also during the whole day. in southern Europe max- al. central and northern ability does not always reflect the impact of road traffic on air Europe. These N maxima recorded in south- that N variability in different European urban environments ern European urban background environments are attributed is not equally influenced by the same emission sources and to midday nucleation episodes occurring when gaseous pol- atmospheric processes. Positive correlations be. Black Carbon and particle number concentration 6223 Table 6. No significant correlations were found in any case variability of levels of N and the comparison with those of when analysing wind components.

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