Action B4 Biomass burning in Southern Europe

AIRUSE

LIFE11 ENV/ES/584

Biomass burning in
Southern Europe

Action B4
Action B4: Biomass burning in Southern Europe

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INDEX

1. INTRODUCTION ..........................................................................................................................4

2. LEVELS OF BIOMASS BURNING TRACERS .........................................................................6

3. CONTRIBUTION OF BIOMASS BURNING TO PARTICULATE MATTER LEVELS ...10

3.1. CHEMICAL PROFILES ..................................................................................................................10

3.2. BIOMASS BURNING CONTRIBUTIONS .........................................................................................12
3.3. COMPARISON WITH OTHER REGIONS AROUND THE WORLD ....................................................15

4. CONCLUSIONS ...........................................................................................................................22

REFERENCES .....................................................................................................................................24

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Action B4: Biomass burning in Southern Europe

1. INTRODUCTION

Identification and quantification of particulate matter (PM) sources using receptor

modelling as a tool in many regions across Europe pointed out biomass burning (BB) as a
major contributor to the atmospheric levels during wintertime (e.g. Bernardoni et al., 2011;
Viana et al., 2013; Waked et al., 2014). Source apportionment of fine particles (PM2.5) in a
coastal/rural area in Portugal showed that 52 to 69% of the particulate organic carbon (OC)
results from residential wood combustion (Gelencsr et al., 2007). In Portugal, it was
estimated that, in 2010, on average, 37% of the population used BB for heating purposes,
which corresponded to a consumption of about 2 Mt y-1 of wood (Gonalves et al., 2012). A
recent investigation carried out in Greece (Saffari et al., 2013) indicated that as the price of
heating oil increases, Greek residents are switching to burning cheaper material, such as
wood, to warm their homes, which is having an effect on the environment and possibly
public health. Air quality in the Greek city of Thessaloniki has worsened during the recent
economic crisis, because residents burn more wood and other types of biomass to keep
warm. Saffari et al. (2013) have found a 30% increase in the concentration of PM 2.5
emissions associated with residential wood combustion (RWC) in 2012 and 2013. Evening
samples encompassed a higher proportion of organic matter (74%) compared with the
morning samples (58%), again suggesting more wood and biomass were used for heating in
the evening. Also, the concentrations of V and Ni, which imply combustion of residential
fuel oil and industrial activity, were 30-40% lower in 2013 compared with 2012. Besides
Portugal and Greece, BB has been recognised as a main source of atmospheric pollution in
other regions of Southern Europe (e.g. Giannoni et al., 2012; Paglione et al., 2014, as well in
many other places around the world (e.g. Moon et al., 2008; Wang et al., 2013; Yatrin et al.,
2008). However, in other Southern European areas the BB contribution has been quantified
as relatively low, for example 2.5% of PM2.5 mass in Barcelona on an annual basis (Reche et
al., 2012). Thus, the scenario may vary widely across Southern Europe.

Particles resulting from RWC encompass several toxic constituents, including carcinogenic
and/or mutagenic compounds, such as polycyclic aromatic hydrocarbons (PAHs). It has been
observed that the total PAH content is higher for combustion particles from wood smoke as
compared to vehicle exhaust (Kocbach et al., 2006). Wood smoke particles seem to affect
factors such as inflammation and blood coagulation, supposed to be involved in
cardiovascular morbidity and mortality (Barregard et al., 2006). The health effects caused by
particulate matter are dependent on its physical and chemical properties (Blling et al.,
2009), which have a clear relation with combustion appliances, fuels and combustion
conditions (Happo et al. 2013; Kaivosoja et al. 2013; Lamberg et al. 2011; Uski et al. 2014;
Vu et al. 2012).

Estimations of the contribution of BB to PM2.5 or PM10 are hard to obtain, because emission
factors vary greatly with wood type and RWC equipment (Gonalves et al., 2011). Moreover,
the amounts and types of wood burned, and the categories of burning appliances can also

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differ significantly from region to region. On the other hand, it is very difficult to get
environmental monitoring databases that have been obtained following the same
methodologies over matching time periods and, thus, the comparability of results from
receptor models accounting for different sources is restricted.

The AIRUSE LIFE+ project has offered an opportunity to create the first harmonised dataset
with PM10 and PM2.5 levels, and the corresponding chemical composition, in various
Southern European cities (Figure 1), following the same sampling protocol over 1 year at 5
monitoring sites: Barcelona (BCN-UB, urban background site, Spain), Porto (POR-TR, traffic
site, Portugal), Florence (FI-UB, urban background site) and Milan (MLN-UB, urban
background site, Italy) and Athens (ATH-SUB, suburban site, Greece). Based on both the
chemical composition and results from the application of Posite Matrix Factorisation (PMF),
this document examines the contribution of BB to the atmospheric particle loads and
compares this source strength in the AIRUSE cities with those in different regions of the
world.

Milan
Florence
Porto
Barcelona

Athens

Figure 1. Five AIRUSE cities where an one-year long PM10 and PM2.5 sampling campaign took
place.

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2. LEVELS OF BIOMASS BURNING TRACERS

Levoglucosan and K are universal tracers of BB (Fine et al., 2001, Gonalves et al., 2010,
2011). Levoglucosan is an anhydrosugar with a six-C ring structure formed from the pyrolysis
of carbohydrates, such as cellulose. Levoglucosan mean levels for the whole campaign
varied by one order of magnitude: 22 (BCN-UB), 53 (ATH-SUB), 287 (FI-UB), 303 (MLN-UB)
and 407 (POR-TR) ng/m3 in PM2.5 (Figure 2). In winter, average values of 774, 563, 548, 103
and 32 ng/m3 were reached in POR-TR, FI-UB, MLN-UB, ATH-SUB and BCN-UB, reflecting the
impact of RWC on air quality across specific regions of southern Europe. These values are
probably underestimated because levoglucosan can be degraded in the atmosphere,
especially oxidised by OH radicals as reported in some simulation experiments and model
studies (Hennigan et al., 2010; Hoffmann et al., 2010). It should be noted that in POR-TR and
MLN-UB some peak events were detected also in summer as a consequence of the impact
of the emissions of wildfires and/or agricultural fires, although the mean winter value is
higher than summer. The impact of BB on PM2.5 levels is clearly demonstrated by the daily
time series of levoglucosan levels (Figure 3). The lowest concentrations of levoglucosan
were registered at BCN-UB. In Barcelona natural gas is being supplied since 1870 to citizens,
helping to achieve that most homes (96% according to the Barcelona City Council) are now
heated by natural gas and, in contrant to the other cities, the input from BB emissions is
minimal. The levoglucosan concentrations were also relatively low in ATH-SUB. As far as
biomass is concerned, although it accounts to 17% of the overall energy consumed for space
heating in the residential sector, the Greek biomass market is not considered to be widely
developed. Consumers have only few choices when it comes to biomass suppliers and
biomass boiler installers. A crucial reason for the immaturity of the biomass market is a
barrier that exists in the Greek legislation. Specifically, according to a Ministerial Decree of
1993 (MD 103/1993/B-369), biomass boilers are not allowed to be installed in the two
major cities of Greece, Athens and Thessaloniki. Due to this restriction a very large part of
the Greek population cannot choose biomass as their energy source for space heating.
Another very important aspect that led to the increased penetration of natural gas is the
fact that from 2004 with a Joint Ministerial Decision (JMD D3/A/11346 FEK 963/B/15-7-
2003) it became mandatory in some big cities (e.g. Athens, Thessaloniki), for newly
constructed buildings to have natural gas installations as their standard equipment
(Giakoumi and Iatridis, 2009).

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800
700

Levoglucosan (ng/m3)
600
500
400
300
200
100
0
Total Winter Total Winter Total Winter Total Winter Total Winter
BCN-UB POR-TR MLN-UB FI-UB ATH-SUB

Figure 2. Average levoglucosan concentrations in PM2.5 obtained with results from all
samples (1-year long sampling campaign starting in the begginning of 2013) and with
winter samples (1 Jan to 21 Mar).

BCN-UB POR-TR
3000 3000
3677
Levoglucosan (ng/m3)

Levoglucosan (ng/m3)

2500 2500

2000 2000

1500 1500

1000 1000
500 500
0 0

MLN-UB FI-UB
3000 3000
4109
Levoglucosan (ng/m3)

2500
Levoglucosan (ng/m3)

2500

2000 2000

1500 1500

1000
1000
500
500
0
0

ATH-SUB
3000
Levoglucosan (ng/m3)

2500
2000
1500
1000
500
0

Figure 3. Time series of levoglucosan levels.

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Levels of K in the fine particle fraction may also increase as a consequence of the influence
of inorganic fly ashes from BB. In the case of this alkali metal, the differences are also
evident, but less marked than for levoglucosan: 98 (BCN-UB), 121 (ATH-SUB), 178 (FI-UB),
327 (POR-TR) and 348 (MLN-UB) ng/m3 in PM2.5 (Figure 4). The lower differentiation is due
to the fact that K may be in part supplied by mineral dust (clay minerals and feldspars) and
possibly by specific industrial sources. At the Italian sites, the winter values were clearly
higher than the global average, stressing the influence of residential BB during the cold
season. In POR-TR, the highest K seasonal average was obtained in summer (495 ng/m3),
when intense wildfires struck the region. For aerosols impacted by wildfires, Pio et al. (2008)
found a better correlation of OC with K than with levoglucosan, indicating that, during more
complete combustive processes, K is possibly a more reasonable BB tracer.

700
600
500
K (ng/m3)

400
300
200
100
0
Total Winter Total Winter Total Winter Total Winter Total Winter
BCN-UB POR-TR MLN-UB FI-UB ATH-SUB

Figure 4. Average K concentrations in PM2.5 obtained with results from all samples (1-year
long sampling campaign starting in the begginning of 2013) and with winter samples
(1 Jan to 21 Mar).

Concentrations of levoglucosan in PM2.5 samples from the AIRUSE cities are in the range of
values reported for other urban sites in the United States and Europe and higher than those
registered in mountain and oceanic background atmospheres (Table 1).

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Table 1. Levoglucosan levels reported for several locations worldwide.

Location and type of site Period Mean Range PM References

3 3
(ng/m ) (ng/m ) fraction
Traffic
Vienna (Austria) 2004 - Jan, Feb, Dec 230-240 PM10 Caseiro et al. (2009)
2004 - Jun-Aug 30-40
Graz (Austria) 2004 -Jan, Feb, Dec 740
2004 - Jun-Aug 90
Salzburg (Austria) 2004 - Jan, Feb, Dec 300
2004 - Jun-Aug 50
Sondrio (Italy) 2005 - Feb 21-27 885 PM10 Piazzalunga et al. (2010)
Milan (Italy) 2006-2009 (winter) 947 PM2.5 Perrone et al. (2012)
2006-2009 (summer) 33
Florence (Italy) 2009-2010 (winter) 355 PM2.5 Giannoni et al. (2012)
2009 (summer) 15
Urban
Bakersfield (California) Dec 1995 - Jan 1996 2390 PM2.5 Nolte et al. (2001)
Fresno (California) Dec 1995 - Jan 1996 2980
Gent, Belgium 1998 - Jan 12-Mar 11 477 121-1133 PM10 Zdrhal et al. (2002)
1998 - Jun 10-Aug 21 19.4 4.1-34.6
Oslo (Norway) 2001 - Nov 4-Dec 14 166 nd - 475 PM10 Yttri et al. (2005)
Elverum (Norway) 2002 - Jan 30-Mar 15 407 134-971
Missoula (Montana) 2003 - Aug 10-23 900-6000 PM2.5 Ward et al. (2006)
Graz (Austria) 2004 - Jan-Feb, Dec 860 PM10 Caseiro et al. (2009)
2004 - Jun-Aug 100
Salzburg (Austria) 2004 - Jan-Feb, Dec 330
2004 - Jun-Aug 50
Libby (Montana) Nov 2004 - Feb 2005 3040 PM2.5 Bergauff et al. (2008)
Dettenahusen (Germany) Nov 2005 - Mar 2006 806 35-3223 PM10 Bari et al. (2010)
Brno (Czech Republic) 2009 (winter) 326 PM2.5 Kmal et al. (2010)
2009 (summer) 47.1
Slapanile (Czech Republic) 2009 (winter) 572
2009 (summer) 55.6
Geeveston (Tasmania) Mar 2009 - Nov 2010 2430 720-6020 PM2.5 and PM10 Reisen et al. (2013)
Urban-Background
Vienna (Austria) 2004 - Jan-Feb, Dec 190-220 PM10 Caseiro et al. (2009)
2004 - Jun-Aug 20-30
Graz (Austria) 2004 - Jan-Feb, Dec 450
2004 - Jun-Aug 80
Salzburg (Austria) 2004 - Jan-Feb, Dec 250
2004 - Jun-Aug 30
Cant (Italy) 2005 - Feb 21-27 963 PM10 Piazzalunga et al. (2010)
Milan (Italy) 2005 - Feb 21-27 385
Mantova (Italy) 2005 - Feb 21-27 569
Florence (Italy) 2009-2010 (winter) 371 PM2.5 Giannoni et al. (2012)
2009 (summer) 13
Borgerhout (Belgium) Feb. 2010 - Feb. 2011 81 11.9-300 PM10 Maenhaut et al. (2012)
Gent (Belgium) 69 14.8-330
Gent (Belgium) Nov 2000- Mar 2001 420 PM10 Pashynska et al. (2002)
Lens (France) 2011-2012 10 310 PM10 Waked et al. (2014)
Barcelona (Spain) 2009 - Feb-Mar 60 PM2.5 Reche et al. (2012)
lapanice (Czech Republic) 2009 - Feb 420 PM1 Kmal et al. (2010)
570 PM2.5
Brno (Czech Republic) 2009 - Feb 220 PM1
320 PM2.5
Zurich (Switzerland) 2003 - Feb 620160 PM10 Szidat et al. (2006)
Zurich (Switzerland) 2006 - Jan 310160 PM1 Sandradewi et al. (2008)

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Gteborg (Sweden) 2005 Feb-Mar 6030 PM2.5 Szidat et al. (2009)

Suburban background
Mechelen (Belgium) Feb. 2010 - Feb. 2011 95 13.8-330 PM10 Maenhaut et al. (2012)
Lycksele (Sweden) 2002 Jan-Mar 900 PM10 Hedberg et al. (2006)
Vindinge (Denmark) 2005 - Feb-Abr 17090 PM2.5 Glasius et al. (2008)
Dettenhausen (Germany) Nov 2005 - Mar 2006 806 35-3223 PM10 Bari et al. (2006)
Rural background
Hamme (Belgium) Feb. 2010 - Feb. 2011 200 18.1-640 PM10 Maenhaut et al. (2012)
Lier (Belgium) 82 13.2-300
Retie (Belgium) 78 10.9-270
Houtem (Belgium) 34 5.2-138
Grove (Tasmania) Mar 2009 - Nov 2010 400 170-940 PM2.5 and PM10 Reisen et al. (2013)
Regional background
Azores Islands (Portugal) 2002-2003 (winter) 6.6 PM2.5 Puxbaum et al. (2007)
2002-2003 (summer) 2
Aveiro (Portugal) 2002-2003 (winter) 1290
2002-2003 (summer) 31.5
Puy de Dme (France) 2002-2003 (winter) 18.3
2002-2003 (summer) 7.1
Schauinsland (Germany) 2002-2003 (winter) 33.7
2002-2003 (summer) 12.3
Sonnblick (Austria) 2002-2003 (winter) 12.4
2002-2003 (summer) 10.2
K-Puszta (Hungary) 2002-2003 (winter) 653
2002-2003 (summer) 21.1
Bosco Fontana Natural 2005 - Feb 21-27 405 PM10 Piazzalunga et al. (2010)
Reserve (Italy)
Chichi-jima, western-north 2001-2004 (winter) 2.2 TSP Mochida et al. (2010)
Pacific
2001-2004 (summer) 0.32
Livorno (Italy) 2009-2010 (winter) 117 PM2.5 Giannoni et al. (2012)
2009 (summer) 6
nd not determined

3. CONTRIBUTION OF BIOMASS BURNING TO PARTICULATE MATTER LEVELS

3.1. Chemical profiles

PMF did not identify BB as a significant source contributing to the atmospheric particulate
matter levels in BCN-UB. The total impact of this source in the other AIRUSE cities showed
some dissimilarities, advising the adoption of region-specific mitigation measures.

In POR-TR, the BB factor comprised levoglucosan (84.1% of explained variation), as well as

OC (29.1% of OC explained variation) and EC (11.5%) (Figure 5). The high OC/EC ratio
obtained (2.9) is also characteristic of BB emissions (Gonalves et al., 2010). The presence of
K (17% of explained variation) helps corroborating the assignment to this source. Lower
proportions of ammonium, nitrate and chloride were also associated with this source.

In FI-UB, the BB profile was characterised by levoglucosan, EC, OC, K, and, to a lesser extent,
by S, Cl, Zn, Br, Pb and nitrate. This source explained 84% of levoglucosan, 30% of EC and

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36% of OC. Although levoglucosan, carbonaceous components (OC and EC), S, Cl and K are
all typical constituents of aerosol particles from BB, emission of Zn, Br and Pb may also occur
during bark and waste wood combustion (Joller et al., 2007; Saqib and Bckstrm, 2014).
The OC/EC ratio in this profile (6.1) was within the ranges reported in the literature for this
source (Gonalves et al., 2010).

In MLN-UB, the BB factor comprised organic particles (30% of OC and 75% of levoglucosan),
EC (23%), a large percentage of K (64%), as well as other characteristic marker compounds
(Rb 53%, Cl 29%). An OC/EC ratio of 4.6 was obtained.

In ATH-SUB, the BB source was identified by EC, OC and K with variations of 6-18% in the
factor. This encompassed tracers of waste combustion, such as As, Cd, Sb and Pb, with
variations ranging between 12% and 72%. Due to the economic crisis and the increased
diesel oil prices, which was the most common way of residential heating in Greece, citizens
of Athens have turned to alternative heating fuels, such as wood. In many cases, treated
wood or even combustible waste are used as fuel.

The wide range of OC/EC ratios between cities may have several reasons. OC/EC ratios were
found to be lower in woodstove emissions compared to prescribed burns in the field (Zhang
et al., 2013). In the case of wildfires, variable OC/EC ratios are often attributed to different
fire intensity: higher temperature of flaming phase burnings have been shown to produce
more soot (EC), and hence lower OC/EC ratios, than smouldering-type combustion (Psfai et
al., 2003). Smoke particles from residential biomass combustion may also present highly
variable OC/EC ratios, depending on the efficiency of the combustion equipment, burning
rates, fuel moisture content, etc. (Fernandes et al., 2011).

1
POR-TR
FI-UB
MLN-UB
0.1 ATH-SUB

0.01

0.001

0.0001
Mg

NH4+
levo
Na

Ca

Fe

Ba
La
Ce
Se
NO3-
K

V
Cr
Mn

Cu
Zn
Br

Rb
Cd
Sn
Sb

Pb
Sr
S

As
EC
OC

Al
Si
Cl

Ti

Ni

Li

Figure 5. Inter-city comparisonof the BB factor profile.

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3.2. Biomass burning contributions

Annual mean contributions and associated errors at each city are listed in Table 2. The
errors estimates were calculated based on the standard error of the coefficients of a
multiple regression between the daily PM concentration (independent variable) and the
different source contributions for that day (dependent variables). The symmetric error for
the contribution of each source was obtained.

Table 2. Annual mean contribution and standard error of BB source at the AIRUSE cities, as
estimated by the PMF model.

AIRUSE Annual mean contribution Standard error

Source bmonitoring 3
g/m (%) g/m3
site
PM10 PM2.5 PM10 PM2.5

POR-TR 4.2 (12) 4.4 (18) 0.2 0.2

BCN-UB n.i. n.i --- ---
Biomass burning MLN-UB n.a. 5.3 (16) --- 1.4
FI-UB 3.0 (16) 2.9 (21) 0.2 0.1
ATH-SUB 1.4 (7) 1.2 (12) 0.6 0.3
n.i. - source not identified as significant by PMF; n.a. - not available (only PM2.5 measurements were
made)

Although levoglucosan has been detected in some samples from BCN, BB could not be
assigned as a significant contributor to PM.

In POR-TR, on average, BB accounted for 12% (4.2 g/m3) and 18% (4.4 g/m3) of the PM10
and PM2.5 levels, respectively. The impact of BB emissions is especially high in the winter
months (Figure 6), due to the generalised use of wood for residential heating (Gonalves et
al., 2012). The contribution of BB to PM was also higher in September. Several wildfires
were registered in the Porto district in this particularly hot and dry month. According to the
Institute for Nature Conservation and Forests (ICNF, 2014), this district recorded the highest
number of occurrences and one of the largest burnt areas. When the mean source
contributions that have been estimated with the annual dataset are compared with the
assignments for days in which the PM10 levels exceeded the limit of 50 g/m3, a salient
feature stands out. The percentage contribution from BB to PM10 and PM2.5 doubles on
exceedance days: 16.5 g/m3 (25%) and 23.6 g/m3 (37%), respectively. It is worth noting
that approximately half of the exceedances were recorded in late August and early
September, when intense wildfires struck the region. The other half was registered in winter
months, indicating the input from residential wood combustion to the atmospheric
particulate loads.
3
In FI-UB, the average contribution of BB was estimated to be 3.0 g/m (16%) in PM10 and
2.9 g/m3 (21%) in PM2.5, with a very high PM2.5/PM10 ratio (0.95), which is reasonable for a

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Action B4: Biomass burning in Southern Europe

combustion source. As expected, the contributions of this source are highly season-
dependent. The maximum inputs occurred in winter, when most of the exceedances of the
limits were registered. During the days in which PM10 concentrations were above 50 g/m3,
BB accounted for 29 and 29% of the PM10 and PM2.5 levels, respectively.

In MLN-UB, on average, 19% of the PM2.5 mass concentrations, which corresponded to 5.3
g/m3, were assigned to BB. As observed in other cities, the highest contributions from BB
to the PM levels were recorded in winter due to domestic heating and the specific stagnant
and reduced boundary layer depths induced by the typical meteorology of the Po Valley.
The source contribution to PM2.5 during the days in which this particle size fraction exceeded
3
35 g/m represented 23.1% of the mass concentrations.

In ATH-SUB, BB was found to contribute to both PM10 (1.4 g/m3, 7%) and PM2.5 (1.20
g/m3, 12%). This source also showed a clear seasonal pattern contributing to PM mass
exclusively in the colder months of the year, with the exception of some events taking place
in August, which could be attributed to some uncontrolled waste burning incidents or forest
fires. It has been found that, over the monitoring campaign, BB did not contribute to
exceedances of the daily limits.
PM2.5
50
POR-TR
FI-UB
40 ATH-SUB
MLN-UB
Source contribution ( g/m3)

30

20

10

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

PM10
50

40
Source contribution ( g/m3)

30

20

10

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

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Figure 6. Daily contributions of BB at four AIRUSE cities for which this source has been
pointed out by PMF as a significant contributor to PM.
For BCN-UB, POR-TR, MLN-UB, ATH-SUB and FI-UB, another factor identified by PMF was
secondary nitrate (SNI). Although in urban environments nitrate mainly arises from NOx
from traffic, a substantial fraction can also derive from BB emissions. The SNI factor was also
extracted from the BCN-UB databases, but, as previously stated, in this city BB was not
identified as a significant source contributing to the atmospheric particle loads. One of the
weaknesses of receptor modelling is its inability to assign most of secondary inorganic
aerosols to specific sources. An inter-city comparison of the SNI factor profile is presented in
a companion report focused on traffic sources. To estimate the contribution of BB to this
factor it is necessary to take into consideration the NOx emission inventory for each study
area and the respective shares for different sources. Based on this approach, percentages of
16 and 13 were adopted in POR-TR and MLN-UB, respectively, to account for SNI from BB. In
FI-UB, on the basis of the emission inventory, ~ 10% of NOx emissions are due to domestic
heating, with only ~ 2% attributable to stoves and chimneys
(http://servizi2.regione.toscana.it/aria/); it is however highly suspected that this datum
underestimates the contribution of domestic heating BB to NO x. Thus, the total contribution
from BB can be appraised as the sum BB + 0.02*SNI, which results in 3.1 and 2.9 g/m3 in
PM10 (16%) and PM2.5 (21%), respectively (Figure 7). In POR-TR, the total contribution from
BB was estimated to be 4.71 g/m3 (13% of PM10) and 4.67 g/m3 (19% of PM2.5). In MLN-
UB, the total contribution from BB represented 6.4 g/m3 in PM2.5 (24%). For BCN-UB, based
on previous studies (Reche et al., 2012) we expect that, although BB was not identified by
PMF, BB contributed less than 0.2 g/m3 (2.5% of PM2.5 mass) on an annual basis.

14 PM10 14 PM2.5
12 12

10 10

8 Biomass
8 burning Biomass burning
mg/m3
mg/m3

6 6
Secondary nitrate from
biomass burning
4 4
Total biomass burning
Secondary nitrate from
biomass burning
Total biomass burning

2 2

0 0

Figure 7. Annual average contributions (and standard error) for BB sources at the five AIRUSE
cities.

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3.3. Comparison with other regions around the world

Within the European project TRANSPHORM (Transport related Air Pollution and Health
impacts Integrated Methodologies for Assessing Particulate Matter), source
apportionment results for PM10 and PM2.5 were obtained for 20 urban areas in Europe
(Table 3). The sampling campaigns were conducted between October 2008 and April 2011
and covered an entire year in each of the study areas. At each site, samples were taken over
three 14-day periods spread over a year, in different seasons. In each area, five stations and
a reference site were monitored simultaneously, representing all different site types
(regional background, urban background and street). PMF was employed to determine PM
sources for two particle size fractions, PM2.5 and PM10. For PM2.5 mass, cities included in the
study were grouped into four main clusters. The first cluster included northern European
cities such as Copenhagen (Denmark), Helsinki (Finland), Oslo (Norway) and Manchester and
London/Oxford (United Kingdom). The second cluster was Vienna (Austria) and Gyor
(Hungary), geographically close and similar (landlocked) cities. The third cluster included
cities as geographically diverse as Paris (France), Athens (Greece) and Kaunas (Lithuania).
The third cluster was, however, spatially distinct from the first cluster. The fourth cluster
consisted of Gyor (Hungary) and Turin (Italy). With regard to K, different clusters were
obtained. With the exception of Gyor (Hungary), there was a clear north/south divide in the
cities for this BB tracer. Southern regions (e.g. Athens, Rome and Catalonia) were in the first
cluster, while cities further north (e.g. Helsinki, Copenhagen, and Oslo) were in a different
cluster. Due to climatic and social differences, there is a north/south divide to wood burning
across Europe, and this has been reflected in the clustering pattern (NILU, 2011). In Athens
and Catalonia, two regions common in both the TRANSPHORM and AIRUSE projects,
domestic heating was estimated to contribute up to 37% of the PM levels. However, mixed
signals of long range transport, domestic heating and other industrial and combustion
sources made it difficult to separate BB itself. It should be noted, however, that the
TRANSPHORM and AIRUSE data are not dictectly comparable. In fact, while the source
apportionment results of TRANSPHORM refer to multi-station monitoring, within AIRUSE
one urban site was monitored in each target city. For example, in TRANSPHORM, the
Catalonia study area covered two cohorts placed in the cities of Sabadell and BCN, and a
third cohort spread over the Girona region. These cohorts comprised urban background,
traffic and rural sites, covering towns next to the sea to countryside and Pyrenean locations,
where BB is much more entrenched. Contrary to what happens in BCN, where natural gas is
the main energy source, in rural areas and small towns of Catalonia, due to the widespread
use of wood fuels, emissions of BB in wintertime have been found to contribute to
exceedances of the benzo[a]pyrene target value of 1 ng/m3 (Querol, 2014).

BB can significantly contribute to the aerosol loads in many regions of the world (Table 4). In
previous works, the input of this source was estimated to account for 11-13% of the PM
mass at some traffic sites in Switzerland and Germany (Gianini et al., 2011; Gu et al., 2011).

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Action B4: Biomass burning in Southern Europe

Contributions from 3% (Izmir, Turkey) to 44% (Rockwood, USA) have been apportioned in
suburban background sites (Kim et al., 2003; Yatkin et al., 2008). Annual average inputs of
12-13% have been found at urban background sites in French and Swiss cities (Bressi et al.,
2014; Gianini et al., 2011; Waked et al., 2014). Around 14 and 27% of the PM wintertime
levels have been assigned to BB, respectively, in the Alpes and in a nature reserve, in Italy
(Perronne et al., 2012). The annual mean contributions in MLN-UB and FI-UB are in the
range of these latter percentages. From measurements previously carried out at urban
background sites in Athens, it has been estimated that BB emissions represented 15% of the
PM2.5 mass (Karanasiou et al., 2009). This value is in line with the current estimate of the
AIRUSE project for the same city (12% of PM 2.5). In accordance with what has been observed
in the AIRUSE project, in earlier works, lower contributions (<8% of PM2.5) have also been
determined for Barcelona (DallOsto et al., 2013; Reche et al., 2012; Viana et al., 2013).

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Action B4: Biomass burning in Southern Europe

Table 3. Contribution of wood combustion and/or domestic heating to PM levels in different European regions, as estimated by the
TRANSPHORM project (NILU, 2011).

Location and type of site Source Key compounds PM fraction Source

contribution (%)

Belgium and Netherlands Combustion K, Zn, Br, Pb, AC, S PM2.5 52.5
Wood combustion K, levoglucosan, Br, Zn, Pb PM2.5 (inc. org) 36.9
Denmark, Copenhagen Domestic heating Pb, K, Zn, Se, Br, AC PM2.5 33.1
Pb, OC, Zn, K, S PM2.5 (inc. org) 27.6
Pb, Zn, As, AC, S, K PM10 32.0
Finland, Helsinki and Turku Domestic heating Pb, S, Zn, K, AC PM2.5 35.7
Domestic heating/Long range transport (LRT) Pb, S, Zn, Br, Cr, K PM2.5 (inc. org) 34.6
Secondary, industrial, domestic heating Pb, S, Zn, Br, AC PM10 24.1
France, Paris Combustion (mixed inc. LRT) Cl, Ni, K, Br, Pb, AC, S PM2.5 37.7
Domestic heating Cl, PAHs, OC, Ni, K PM2.5 (inc. org) 26.4
Mixed combustion/Domestic heating/SIA Pb, S, Se, Ni, Zn, As, AC PM10 36.6
Germany, Munich Domestic heating K, Rb, Pb, Zn, As, AC PM2.5 42.9
PAHs, levoglucosan, benzanthrone, K PM2.5 (inc. org) 22.2
Pb, K, AC, S, Zn, As, Se, Br, Rb PM10 41.2
Greece, Athens SIA/Combustion Se, As, S, K PM2.5 25.3
Domestic heating PAHs, OC, K PM2.5 (inc. org) 12.8
Combustion (biomass burning/coal/industry) Se, Pb, AC, Zn, Ni PM10 20.1
Greece, Heraklion Combustion (burning of agricultural waste) K, As, Br, Ni, V, AC PM2.5 17.5
Germany, Ruhr Area Domestic heating Cl, Br, Rb, K, Pb; AC PM2.5 19.3
Cl, Br, As, V PM10 20.8
Hungary, Gyr Combustion (domestic heating) K, Zn, As, Rb, Br, AC, Pb PM2.5 41.7
Cl, As, K, Zn PM10 20.8
Italy, Rome Wood combustion, domestic heating Rb, K, Br, Pb, AC, Zn PM2.5 38.9
K, Rb, Pb, AC, Br PM10 24.1

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Action B4: Biomass burning in Southern Europe

Italy, Turin Domestic heating K, Pb, Ni, Br, Zn PM2.5 48.9

Combustion, heating Cl, Ni, Rb PM10 24.4
Lithuania, Kaunas Combustion (domestic heating) Zn, Pb, K PM2.5 27.7
Pb, Zn, K, AC, S PM10 17.5
Norway, Oslo Domestic heating Pb, Zn, K, AC PM2.5 36.1
PAHs, levoglucosan PM2.5 (inc. org) 17.3
Domestic heating / Other combustion sources As, AC, Zn, Rb PM10 28.4
Sweden, Stockholm Domestic heating Pb, Zn, AC, S, K PM2.5 23.9
Pb, S, Na, V, Br, AC PM10 15.5
Switzerland, Lugano Domestic heating Pb, K, AC, Zn, Br, Ni PM2.5 39.5
Pb, Br, Zn, Ni, AC, K PM10 38.5
United Kingdom, Manchester Combustion (inc. domestic heating) Pb, Br, K, AC PM2.5 30.3
Domestic heating/SIA Pb, Zn, Ni, V, S, AC, K PM10 24.3
United Kingdom, London and Oxford Domestic heating Cl, Na, Pb, Br, K PM2.5 24.7
Combustion (biomass burning, coal, industry) Cl, PAHs, Pb, Br, As, Zn, K PM2.5 (inc. org) 24.9
Combustion (domestic heating) As, Br, Pb, AC, K, Cl, Zn PM10 30.4
Spain, Catalonia Domestic heating K, Br, Pb, AC PM2.5 37.2
Austria, Voralberg Domestic heating and road salt Na, Cl, K, Zn, Pb, AC PM10 25.0

AC: absorption coefficient; SIA: Secondary inorganic aerosol

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Action B4: Biomass burning in Southern Europe

Table 4. BB contribution to PM levels estimated by receptor models for different regions around the world.

Receptor model Location and Sampling Sampling campaign PM BB contribution to PM mass (%) References
type of site period fraction
Spring Summer Fall Winter Average

Urban
background
PMF (9 factor Lens (France) 2011-2012 Sampling over 1year period. Samples collected every third PM10 4 - 18 25 13 Waked et al.
solution) day from 9 Mar. 2011 to 6 Mar. 2012 (2014)
PMF (7 factor Paris (France) 2009 - 2010 Sampling from 11 Set. 2009 to 10 Set. 2010 (24h samples). PM2.5 - - - - 12 Bressi et al. (2014)
solution)
PMF (9 factor Barcelona 2009 Sampling over 1year period. The campaign was performed in PM2.5 - - - - 3 Reche et al.
solution) (Spain) winter (Feb. to Mar. 2009) and summer (Jul. 2009). The (2012)
sampling period was 24 h with a frequency of one sample
every four days.
PMF (9 factor Barcelona 2010 Sampling from 20 Sep. to 20 Oct. 2010. Hourly-resolved PM2.5 - - 5 - - DallOsto et al.
solution) (Spain) samples. (2013)
PMF (4 factor Barcelona 2011 Sampling from 12 to 21 Jan. 2011. PM2.5 concentrations (by PM2.5 - - - 8 - Viana et al. (2013)
solution) (Spain) optical counters, GRIMM 1107, 10-min time resolution) and
24h samples of PM2.5.
PMF (9 factor Zaragoza 2003 - 2004 Samples were collected every week. Sampling from 7 Apr. PM10 - - - - 6 Calln et al.
solution) (Spain) 2003 to 5 Jul. 2004. (2009)

PMF (7 factor Milan (Italy) 2006 Samples with 4-hour resolution. Sampling from 27 Jun. to 11 PM10 - 1 - 14 - Bernardoni et al.
solution) Jul. and from 21 Nov. to 6 Dec. (2011)

PMF (6 factor Zurich 2008 - 2009 Sampling from 01 Aug. 2008 to 31 Jul. 2009 (24h samples). PM10 - - - - 13 Gianini et al.
solution) (Switzerland) (2012)

PMF (7 factor Athens (Greece) 2002 Sampling was conducted at three sites located in the Athens PM2 - - - - 15 Karanasiou et al.
solution) urban area. Sampling from Mar. 2002 to Dec. 2002 (24h (2009)
samples except for one sampling site, where four 6-h
samples were taken each day).
PMF (7 factor Bandung 2002 - 2004 Sampling from Jan. 2002 to Dec. 2004 (24 h samples twice a PM2.5 - - - - 20 Santoso et al.
solution) (Indonesia) week) (2008)
PMF (7 factor Chennai (India) 2008- 2009 Sampling from 10 Nov. to 26 Dec. 2008; from 17 Jan. to 16 PM10 - - - - 0.7 Srimurugananda
solution) Feb. 2009 and from 23 Mar. to 13 Apr. 2009 (24h samples). m et al. (2012)
PM2.5 - - - - 14

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Action B4: Biomass burning in Southern Europe

PMF (6 factor Chengdu 2011 Sampling during four 1-month periods. Sampling from 6 to PM10 7 1 19 16 11 Tao et al. (2014)
solution) (China) 30 Jan, from 3 Apr. to 3 May, from 1 to 31 Jul. and from 1 to
31 Oct. (24h samples).
PMF (8 factor Beijing (China) 2000 Sampling at 6-day interval (24 h samples) in Jan., Apr., Jul. PM2.5 - - - - 11 Song et al. (2006)
solution) and Oct. at five locations in the
Beijing metropolitan area.
PMF (8 factor San Jose 2002 - 2012 Sampling from Oct. 2002 to Feb. 2012 (3 or 6 days samples) PM2.5 16.4 13.5 24.3 35.1 24.3 Wang et al. (2013)
solution) (California, U.S)

CMB Milan (Italy) 2006 - 2009 At least 30-40 daily samples (24 h) were collected in summer PM2.5 8 1 30 25 - Perronne et al.
as well as in winter. Shorter campaigns were conducted (2012)
during spring (years 2007 and 2008) and fall (year 2007
only), and about 1520 daily samples were taken during
both seasons.
PM10 - 1 - 18 -

CMB Elms road 2007 - 2008 Sampling from May 2007 to April 2008 (5 days samples). PM2.5 - 0.5 - 0.8 0.6 Yin et al. (2010)
observatory site
(UK)
CMB Marseille 2008 Sampling from 30 Jun. to 14 Jul. Samples collected PM2.5 - 0.52 - - - Haddad et al.
(France) continuously on a 12h-basis. (2011)
CMB Izmir (Turkey) 2004 - 2005 Sampling from Jun. 2004 to May 2005. Samples collected PM10 3.8 Yatkin et al.
every 6 days (24h samples). Samples were collected on two (2008)
sequential days a week (first day PM10 and second day
PM2.5).
PM2.5 - 0.7 - 1.2 1

COPREM Copenhagen 1999 - 2004 Sampling from Jan. 1999 to Dec. 2004 (24 h samples). PM10 - - - - 15 Andersen et al.
(Denmark) (2007)
Rural
background
PMF (6 factor Payerne 2008 - 2009 Sampling from 01 Aug. 2008 to 31 Jul. 2009 (24h sampling). PM10 - - - - 15 Gianini et al.
solution) (Switzerland) (2012)

Magadino - - - - 31
(Switzerland)
CMB Churchill 2007 - 2008 Sampling from May 2007 to April 2008 (5 days samples) PM2.5 - 0.5 - 0.7 0.6 Yin et al. (2010)
pumping
station site (UK)

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Action B4: Biomass burning in Southern Europe

CMB "Oasi Le Bine" 2006 - 2009 At least 30-40 daily samples (24 h) were collected in summer PM2.5 - 3 31 27 - Perronne et al.
Nature reserve as well as in winter. Shorter campaigns were conducted (2012)
(Italy) during spring (years 2007 and 2008) and fall (year 2007
only), and about 15-20 daily samples were taken during both
seasons.
Regional
background
PMF (14 factor Gosan (Korea) 2001 - 2003 Sampling from 13 to 25 Nov. 2001; from 29 Mar. to 11 Apr. PM2.5 - - - - 7.1 Moon et al.
solution) 2002; from 27 Aug. to 11 Set. 2002; from 14 to 26 Feb.; from (2008)
6 to 22 Jun 2003 and from 18 Aug. to 1 Set. 2003. (24 h
samples)
High altitude
remote
CMB Alps (Italy) 2006 - 2009 At least 30-40 daily samples (24 h) were collected in summer PM2.5 - 2 5 14 - Perronne et al.
as well as in winter. Shorter campaigns were conducted (2012)
during spring (years 2007 and 2008) and fall (year 2007
only), and about 15-20 daily samples were taken during both
seasons.
Traffic
background
PMF (6 factor Augsburg 2006 - 2007 Sampling from Dec. 2006 to Mar. 2007 (24h samples) PM10 - - - - 13.3 Gu et al. (2011)
solution) (Germany)

PMF (7 factor Bern 2008 - 2009 Sampling from 01 Aug. 2008 to 31 Jul. 2009 (24h samples). PM10 - - - - 11 Gianini et al.
solution) (Switzerland) (2012)
Suburban
background
PMF (5 factor Tanumshede 2007 - 2008 Sampling from 17 Nov. 2007 to 15 Apr. 2008 (24h samples) PM2.5 - - - - 25 Molnr et al.
solution) (Sweden) (2013)
PMF (6 factor Lembang 2002 - 2004 Sampling from Jan. 2002 to Dec. 2004 (24 h samples twice a PM2.5 - - - - 40 Santoso et al.
solution) (Indonesia) week) (2008)
PMF (7 factor Rockwood 1995 - 1997 Sampling between Jan. 1995 and Dec. 1997. Daily PM2.5 filter PM2.5 - - - - 44 Kim et al. (2003)
solution) (USA) samples were collected.

PMF (6 factor Basel 2008 - 2009 Sampling from 01 Aug. 2008 to 31 Jul. 2009 (24h samples). PM10 - - - - 14 Gianini et al.
solution) (Switzerland) (2012)
CMB Izmir (Turkey) 2004 - 2005 Sampling from Jun. 2004 to May 2005. Samples collected PM10 2.9 Yatkin et al.
every 6 days (24h samples). Samples were collected on two (2008)
sequential days a week (first day PM10 and second day
PM2.5).
PM2.5 - 0.4 - 1.6 0.8

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Action B4: Biomass burning in Southern Europe

4. CONCLUSIONS

Contrasting results between BCN-UB and other AIRUSE cities were obtained. While a very
high degree of natural gas penetration in the Spanish city is clearly reflected in very low
contributions from BB to the atmospheric PM levels, the extensive use of wood in
residential combustion appliances in other cities, especially in Portugal and Italy, contributes
to high inputs from this source. Nevertheless, BB should be faced as a regional problem in
Catalonia and other autonomous communities of Spain, since RWC is commonly practiced in
small towns and in the countryside.

Due to the widespread use of natural gas for residential space heating, the concentrations
of BB tracers (levoglucosan and potassium) in BCN-UB were low compared with other cities.
PMF receptor modelling could not assign BB as a significant source contributing to the
atmospheric particle loads in this city. A clear BB assignment was found for POR-TR, MLN-
UB, FI-UB and ATH-SUB.

Despite the sampling campaign in POR-TR being carried out at a traffic station, it was
observed that, after vehicle emissions, sea salt and mineral matter, BB was the most
significant source, accounting for 12% of the PM10 levels. After vehicle exhaust emissions, BB
was the second most important source of PM2.5, explaining 18% of the mass concentrations.
These percentages are, respectively, 13 and 19% if the fraction from secondary nitrate
derived from BB emissions is taken into account. The fractional contribution from this
source to PM2.5 and PM10 doubles on exceedance days (> 50 g/m3). It is worth noting that
approximately half of the exceedances were recorded in late August and early September,
when intense wildfires struck the region. The other half was registered in winter months,
indicating the input from residential wood combustion to the atmospheric PM levels.

In the urban background of Milan (MLN-UB), after traffic, BB is the most important source of
PM2.5 (24%). The average BB contribution during the days with concentrations above 35
g/m3 accounted for 26% of PM2.5.

The total BB contribution in FI-UB was estimated by adding 2% of secondary nitrate.

However, it is highly likely that this percentage, deduced from the regional emission
inventory, underestimates the NOx from residential BB. Total emissions from this source
were estimated to contribute to 16 and 21% of the PM10 and PM2.5 masses, respectively.
Toghether with traffic, BB is the most important source contributing to the exceedances
registered in the cold season.

At Athens (ATH-SUB), BB represented the third largest contribution to PM2.5. This source
accounted for 7% and 12% of the PM10 and PM2.5 levels, respectively. It is important to
highlight that this site is considered as suburban, whereas the other AIRUSE sites are
classified as urban background or traffic stations. This means that the levels of pollution at
this site are probably lower than at other urban background sites of Athens, which are
probably more comparable to the other AIRUSE sites.

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Action B4: Biomass burning in Southern Europe

In summary, with the exception of BCN-UB, BB is, besides traffic, one of the most important
sources contributing to the PM levels in southern European cities. Annual average
contributions from 7 to 16% and from 12 to 24% of PM10 and PM2.5, respectively, were
estimated. However, due to the extensive use of wood for household heating, in winter the
BB fraction has a much larger share. In many cases, this source was found to be responsible
for the exceedances of the European air quality limit values. The fractional contribution of
biomass to the bulk particulate matter load is in the range of values reported for mountain
sites or for countries with colder climates. Taking into account that, currently, the RWC
equipment in southern Europe is largely represented by outdated and inefficient stoves,
strategies promoting, through financial incentives, the replacement of older wood-burning
appliances by cleaner home heating are required. Policies with an intersectoral perspective,
coordinated by the EU, for woody biomass development and use need a balanced approach
considering environmental, social and economical issues.

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Action B4: Biomass burning in Southern Europe

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