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Article history:
Received 17 August 2010
Received in revised form
11 January 2011
Accepted 12 January 2011
There is good evidence for an increase in the global surface level of ozone in the past century. In this work
we present an analysis of 18 surface ozone series over the Iberian Peninsula, considering the target values
of ozone for the protection of human health and for the protection of vegetation, as well as the information
and alert thresholds established by the current European Directive on ambient air quality and cleaner air
for Europe (Directive 2008/50/EC). The results show that the stations located on the Cantabrian coast
exceeded neither the target value for the protection of human health nor the target value for the protection
of vegetation. The information threshold was exceeded in most of the stations, while the alert threshold
was only exceeded in one. The seasonal and daily evolution of ozone concentrations were as expected.
A trend analysis of three surface ozone concentration indices (monthly median and 98th percentile, and
monthly maximum of the daily maximum 8-h mean) was performed both for the whole period of each
station and for the common period from 2001 to 2007 for all the months of the year. It was noted that
generally the south of the Iberian Peninsula presented increasing trends for the three indices, especially
in the last six months of the year, and the north decreasing trends. Finally, a correlation analysis was
performed between the daily maximum 8-h mean and both daily mean temperature and daily mean
solar radiation for the whole and the common periods. For all stations, there was a signicant positive
association at a 5% signicance level between the daily maximum 8-h mean and the two meteorological
variables of up to approximately 0.5. The spatial distribution of these association values from 2001 to 2007
showed a positive northwest to southeast gradient over the Iberian Peninsula.
2011 Elsevier Ltd. All rights reserved.
Keywords:
Tropospheric ozone
Ozone variability
Ozone trends
Iberian Peninsula
1. Introduction
The global distribution of ozone is an important aspect in the
study of the atmosphere. Changes in atmospheric ozone are also
important for climate change (Intergovernmental Panel on Climate
Change (IPCC), 2007): decreases in stratospheric ozone lead to
enhanced UVB radiation in the troposphere, which in turn accelerates
certain important photolysis rates. Consequently, the formation rate
of tropospheric ozone and the oxidation capacity of the troposphere
are affected, depending on the concentrations of nitrogen oxides
(Staehelin et al., 2001). On a global scale, ozone formation depends
mainly on nitrogen oxides (NOx), whereas on a local scale volatile
organic compounds (VOCs) are more important than nitrogen oxides,
and on a regional scale both types of ozone precursors have to be
considered in the net photochemical ozone production. Tropospheric
or surface ozone is a secondary air pollutant, causing health problems
and adverse effects on living beings and the physical environment
* Corresponding author. Tel.: 34 924289300x89116; fax: 34 924289651.
E-mail address: maricruz@unex.es (M.C. Gallego).
1352-2310/$ e see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2011.01.027
(Parmet et al., 2003; Janneane et al., 2003; EPA, 1996; Finnan et al.,
1997; Agrawal et al., 2003). The background ozone has several sources, both natural and anthropogenic (Vingarzan, 2004; Castell et al.,
2008). Recently, ozone research has been attracting great interest
because, during the last century, surface ozone concentrations were
considerably raised over rural areas in Europe. Comparisons of ozone
background levels with those measured in the late 19th to early 20th
centuries indicate that current ozone levels have risen approximately
twofold (Stevenson, 2001; Bozo and Weideinger, 1995; Staehelin
et al., 1994; Cartalis and Varotsos, 1994). This rise occurred in
parallel with industrial development and motor trafc which resulted
in a strong increase of emissions of many species, including nitrogen
oxides and volatile organic compounds. However, measures have
been taken to reduce the emissions of these ozone precursors (NOx
and VOCs). Between 1990 and 2008, emissions of VOCs in Spain and
Portugal decreased by around 21% and 34% respectively. Emissions of
NOx decreased in Spain by 8%; however in Portugal they increased by
around 7% (EEA, 2010).
Some authors have found that since the 1950s in the northern
hemisphere surface ozone has increased at a mean rate of w1e2% per
1947
Fig. 1. Geographical locations of the studied stations. Red circles indicate the stations
which do not exceed the target value for the protection of vegetation (AOT40). Green
circles indicate the stations which do not exceed the information threshold
(180 mg m3). (For interpretation of the references to colour in this gure legend, the
reader is referred to the web version of this article.)
Table 1
Locations, coordinates, altitudes, study period, and percentage of missing values of
the selected stations.
Code Observatory
Longitude Latitude
( N)
( E)
ES01
4.34861
39.54777
917
1993e2000
6.76
3.6
0.49139
2.50305
8.92361
4.31666
3.53333
4.85027
3.14277
3.31694
6.92278
1.10194
5.86667
0.71667
4.35
7.69972
6.55
8.8
37.2
720
40.82055
44
42.45779
445
42.72805
683
39.86666
78
37.23333 1265
43.44222
134
41.28111 1360
42.31944
23
38.47583
393
39.08611
885
41.28333
985
41.4
470
39.51667 1241
43.23111
506
37.05
5
39.08333
43
1993e1995
1993e2000
1993e2001
1993e2000
2008e2009
1995e2009
1998e2009
1998e2009
1998e2009
1999e2009
1998e2009
2000e2009
2000e2009
2000e2007
2001e2009
2008e2009
1990e2007
13.16
4.66
6.30
10.11
3.35
11.00
2.52
4.86
3.84
3.00
2.93
2.38
2.19
9.84
3.76
4.54
18.17
San Pablo de
los Montes
ES02 La Cartuja
ES03 Roquetas
ES04 Logroo
ES05 Noia
ES06 Mahn
ES07 Vznar
ES08 Niembro
ES09 Campisbalos
ES10 Cabo de Creus
ES11 Barcarrota
ES12 Zarra
ES13 Peausende
ES14 Els Torms
ES15 Risco Llano
ES16 O Saviao
ES17 Doana
PT04 Monte Velho
Altitude Period
(m)
Missing
values %
1948
Table 2
Threshold values for ozone.
Threshold
Value
Measured as
120 mg m3
18 000 mg m3h1
180 mg m3
240 mg m3
AOT40 is the sum of the differences between the hourly mean surface ozone
concentration greater than 80 mg m3 and 80 mg m3 using only the 1 h values
measured between 8:00 and 20:00 from May to July.
3. Methods
As was mentioned above, the current European Directive on
ambient air quality and cleaner air for Europe is Directive 2008/50/EC.
This Directive establishes target values of ozone for the protection of
human health and for the protection of vegetation as well as information and alert thresholds (Table 2). According to this Directive, UE
Member States must inform the population of the dates and duration
of periods when the target and threshold values are exceeded and the
ozone concentrations that are reached at those times.
To analyse the possible existence of statistically signicant trends
in the IP surface ozone time series, the non-parametric ManneKendall
(MeK) test was used. This statistical test was rstly introduced by
Kendall (1976), and has been widely applied in a lot of scientic elds,
i.e.: hydrology (Kundzewicz and Robson, 2000), climatology (Gallego
et al., 2006, 2011), air quality (de Leeuw, 2000; Ruoho-Airola et al.,
2004; Sicard et al., 2009, 2011) and precipitation chemistry (Kvaalen
et al., 2002; Sicard et al., 2007). The null hypothesis Ho is that the
data (X1, X2, . Xn) are identical and independently distributed random
variables, and the alternative hypothesis H1 is that the data are
n1 X
n
X
i 1 j i1
sgn Xj Xi ;
vars
nn 12n 5
:
18
The exact distribution of s can be evaluated. For n > 10, the distribution
approaches a normal, especially if the following correction is made:
s0 s sgns:
The normalised variable is evaluated from s0
s0
vars
Fig. 2. AOT40 and the number of exceedance days related to protection of human health, information threshold, and alert threshold at the Niembro (ES08), Cabo de Creus (ES10),
Monte Velho (PT04), and La CartujaeVznar (ES02eES07) stations.
1949
Table 3
Summary of the analysis of the directive.
Station
e
1998,
1990,
2003,
ES02_ES07 1998,
ES08
ES10
PT04
Years above
Years above protection human health
alert threshold
e
2000, 2001, 2002, 2003, 2004, 2005, 2006. e
1996, 1997, 1999, 2001, 2002,
1997
2005, 2006
1999,2001
e
Fig. 3. Monthly evolution of ozone at the eighteen stations. (a) Stations with maximum concentrations in April and May. (b) Stations with maximum in June and July. Green circles
indicate the stations with the highest ozone levels. Red circles indicate the stations with the lowest ozone levels. (For interpretation of the references to colour in this gure legend,
the reader is referred to the web version of this article.)
1950
1951
Fig. 5. Example of daily evolution of (a) NO and (b) NO2 concentrations in spring.
2Sr1 ; .; rn
;
nn 1
where ri is rank of Y belonging to the pair (X,Y) for which the rank of
X is equal to i, and S 2N n(n 1)/2, with N being the number of
elements of the sample for which j > i and rj > ri simultaneously.
The inequality 1 sc 1 always holds. The Kendall coefcient of
rank correlation has been extensively used (see Kendall, 1970) as
an empirical measure of dependence. In particular, the test was
applied to determine the possible correlations between the daily
maximum 8-h mean of surface ozone concentration and daily
means of temperature and solar radiation, respectively.
4. Results
4.1. Analysis of the directive
Surface ozone concentrations at each station were analysed
in accordance with the current Directive. The results for the 18
stations showed the target value for the protection of human health
to be exceeded at all the stations except O Saviao (ES16) and
Niembro (ES08), both located on the Cantabrian coast. The target
value for the protection of vegetation was surpassed in all the
stations with the exception of Roquetas (ES03) in the Ebro valley,
and Niembro (ES08), Noia (ES05), O Saviao (ES16), and Monte
Velho (PT04) on the north and west coasts of the IP (see Fig. 1).
Table 4
Magnitude of the trend and p-value of the median for the whole period at each station.
INDIC
January
B
ES01eES15
ES05
ES08
ES10
ES11
ES13
ES14
PT04
INDIC
ES01eES15
ES02eES07
ES08
ES09
ES10
ES13
a
12.65
28.25
3.25
L22.27
11.52
27.03
4.27
4.56
February
p-value
0.03
0.09
0.38
0.001
0.19
0.09
0.46
0.23
July
March
April
May
June
p-value
p-value
p-value
p-value
p-value
9.36
36.58
8.06
L23.9
17.78
1.49
26.32
5.73
0.07
0.02
0.12
0.0006
0.11
0.5
0.01
0.12
5.1
31.02
12.74
25.31
4.18
5.72
18.76
4.5
0.31
0.03
0.01
0.0004
0.38
0.38
0.09
0.27
8.34
28.25
13.83
L21.86
9.05
18.39
16.65
8.18
0.12
0.19
0.02
0.0004
0.11
0.17
0.23
0.04
7.24
25.96
8.31
L18.77
20.46
4.84
28.08
6.76
0.08
0.13
0.11
L0.01
0.02
0.46
0.04
0.07
11.24
23.9
2.44
10.25
1.28
L31.85
14.28
5.99
0.1
0.05
0.38
0.06
0.38
L0.004
0.23
0.1
August
September
October
November
December
p-value
p-value
p-value
p-value
p-value
p-value
12.74
3.84
4.27
8.89
L16.52
L22.13
0.03
0.37
0.38
0.19
L0.04
L0.04
6.02
11.95
8.89
13.25
L18.11
10.09
0.23
0.02
0.27
0.10
L0.001
0.08
8.18
10.63
24.49
6.19
L18.88
4.77
0.25
0.04
0.01
0.23
L0.01
0.24
1.36
11.06
6.27
L16.95
L27.72
10.08
0.50
0.005
0.37
L0.01
L0.003
0.06
3.57
11.58
7.86
L13.19
L23.65
6.47
0.31
0.01
0.06
L0.01
L0.01
0.24
11.97
1.95
11.37
4.73
15.61
3.17
0.11
0.38
0.12
0.29
0.10
0.36
1952
Table 5
Magnitude of the trend and p-value of the 98th percentile for the whole period at each station.
INDIC
ES01eES15
ES04
ES05
ES08
ES10
ES11
ES13
ES14
PT04
INDIC
ES01eES15
ES02eES07
ES09
ES10
ES11
ES12
ES13
PT04
a
January
February
March
April
May
June
Ba
p-valuea
p-value
p-value
p-value
p-value
p-value
11.85
17.47
28.31
10.57
20.39
4.71
18.76
21.94
8.39
0.01
0.09
0.05
0.06
0.02
0.30
0.23
0.04
0.02
6.80
19.14
33.50
13.74
18.44
5.67
9.48
19.81
4.57
0.20
0.03
0.03
0.03
0.002
0.36
0.13
0.02
0.18
1.29
6.70
25.97
8.80
7.74
4.77
14.80
19.12
2.48
0.38
0.19
0.05
0.18
0.04
0.18
0.17
0.13
0.26
0.52
7.45
14.46
14.77
8.04
22.90
27.00
8.11
6.59
0.36
0.27
0.27
0.03
0.23
0.01
0.06
0.42
0.02
7.48
8.42
24.17
2.93
20.71
9.68
10.03
19.96
7.40
0.08
0.36
0.09
0.32
0.01
0.18
0.30
0.15
0.08
8.64
2.48
8.56
2.29
17.00
1.03
31.40
3.31
12.07
0.14
0.45
0.45
0.32
0.04
0.44
0.01
0.38
0.01
July
August
September
October
November
December
p-value
p-value
p-value
p-value
p-value
p-value
20.28
4.59
9.23
13.33
2365.00
5.46
17.07
12.09
0.004
0.29
0.23
0.12
0.41
0.14
0.06
0.01
14.31
6.50
14.10
20.76
0.35
9.56
8.41
9.32
0.008
0.007
0.08
0.02
0.50
0.19
0.36
0.08
15.96
3.30
11.25
19.54
9.02
10.85
12.61
6.76
0.03
0.20
0.02
0.04
0.32
0.04
0.11
0.04
10.29
11.89
6.32
20.16
3.72
1.85
10.23
4.31
0.03
0.02
0.19
0.03
0.50
0.50
0.24
0.24
5.32
8.95
10.08
14.91
0.96
3.04
7.17
4.87
0.31
0.04
0.04
0.06
0.50
0.42
0.04
0.14
8.69
2.48
6.23
9.26
15.09
13.72
1.86
10.45
0.16
0.42
0.27
0.18
0.01
0.10
0.50
0.09
March 1997, with this being the only station of the set studied at
which this threshold was surpassed. At La CartujaeVznar
(ES02eES07), in the southeast interior of the IP, all years presented
exceedances of the target value for the protection of human health
except 1993. The highest AOT40 was reached in 1998 and 1999. The
alert threshold was not exceeded on any occasion. The information
threshold was exceeded in 1998, 1999, and 2001. The results for
these four stations shown as examples are summarised in Table 3.
This type of analysis of the Directive has also been carried out in
other European countries. de Leeuw (2000), for instance, analysed
the ground level ozone concentrations in the European Union
for the period between 1994 and 1998. For the majority of
stations, exceedances of the threshold for health protection,
vegetation protection, and population information were found.
However, those stations showed downward trends in the number
of exceedance days.
Table 6
Magnitude of the trend and p-value of the monthly maximum of the daily maximum 8-h mean for the whole period at each station.
INDIC
ES01eES15
ES04
ES05
ES08
ES10
ES13
ES14
PT04
INDIC
ES01eES15
ES02eES07
ES04
ES08
ES09
ES10
ES13
PT04
a
January
February
March
April
May
June
Ba
p-valuea
p-value
p-value
p-value
p-value
p-value
13.79
18.19
25.61
8.15
21.19
13.21
18.65
10.07
0.004
0.04
0.03
0.27
0.08
0.03
0.09
0.03
6.95
14.13
34.25
20.60
20.15
4.14
10.23
3.59
0.14
0.09
0.03
0.02
0.08
0.30
0.04
0.19
3.39
11.10
21.87
7.54
11.36
0.08
16.50
1.64
0.21
0.27
0.27
0.38
0.04
0.50
0.17
0.24
4.21
23.32
14.54
15.57
2.94
9.48
24.90
5.75
0.21
0.19
0.27
0.02
0.32
0.38
0.06
0.10
9.92
4.47
28.58
1.96
20.62
5.28
7.98
3.72
0.05
0.45
0.13
0.38
0.01
0.38
0.38
0.09
11.81
19.09
5.40
3.84
12.78
39.50
1.44
9.13
0.06
0.09
0.50
0.38
0.19
0.002
0.50
0.03
July
August
September
October
November
December
p-value
p-value
p-value
p-value
p-value
p-value
12.75
6.14
27.35
5.88
5.94
12.81
14.24
12.17
0.04
0.19
0.01
0.22
0.19
0.15
0.02
0.01
15.56
7.84
34.58
1.96
15.65
19.60
7.01
9.15
0.062
0.10
0.13
0.38
0.007
0.003
0.24
0.10
15.21
12.40
20.87
7.74
12.66
8.20
9.94
5.81
0.01
0.02
0.09
0.27
0.03
0.27
0.05
0.22
8.70
10.08
16.19
6.10
11.42
7.15
5.30
7.64
0.08
0.02
0.13
0.37
0.19
0.10
0.43
0.15
3.99
11.40
12.76
11.04
13.63
16.10
9.47
1.88
0.33
0.01
0.19
0.12
0.08
0.02
0.11
0.33
14.42
4.54
6.85
10.85
4.04
11.66
7.45
5.21
0.06
0.22
0.27
0.01
0.47
0.19
0.36
0.19
1953
island of the same name, and Cabo de Creus (ES10) on the Mediterranean coast, both stations inuenced by the Mediterranean Sea
which is a more polluted region than those bordering the Atlantic.
In Fig. 3b, the stations located in the interior of the IP show maxima in
summer. The lowest monthly mean concentrations were observed
in Roquetas (ES03) in the Ebro valley. The highest monthly mean
concentrations were observed in San Pablo de los MonteseRisco
Llano (ES01eES15) almost in the centre of the IP. Nevertheless, this
Fig. 6. ManneKendall test for monthly median series of surface ozone concentration for the period from 2001 to 2007 (from left to right and from top to bottom): January, February,
March, April, May, June, July, August, September, October, November, and December. Upward triangles represent increasing trends and downward triangles decreasing trends.
The size of each triangle is proportional to the magnitude of the normalised trend (normalised to the standard deviation). Solid black triangles represent trends signicant at the 5%
level, solid grey triangles indicate trends signicant at the 10% level, and triangles and transparent triangles indicate non-signicant trends at the 5% and 10% levels. Isolines
correspond to interpolated values of the normalised trend (percentages).
1954
last station is one of the highest altitude stations of our set, and these
commonly show only slight seasonal variation possibly because they
sample more tropospheric air. With respect to the season when the
maximum concentrations were registered, all the features described
are consistent with the ndings of Castell et al. (2008) who note that
stations located on the coast present maxima in spring. This spring
maximum may be explained by the smaller spatial development of
the breeze cell during these months, i.e., the levels stay conned
relatively close to the production areas. However, at the stations
located within the Peninsula, the spring maximum was secondary,
while the main maximum was recorded during the summer months
reecting the typical smog maxima.
Fig. 7. ManneKendall test for monthly 98th percentile series of surface ozone concentration for the period from 2001 to 2007 from January to December. Symbols as in Fig. 6.
1955
concentrations here correspond to maxima in NOx. The phenomenon can be explained as follows. The NO from trafc emissions is
produced in the early morning when human activities begin. Once
the minimum ozone levels are reached, the elimination of further
ozone by NO is not very effective; the NO2 concentration is greater
than the NO concentration, thus enhancing ozone formation
(Adame et al., 2008). Another process which can decrease surface
O3 concentrations during the night is dry deposition, and this is not
effective in the residual layer whose air is mixed downwards in the
late morning by vertical mixing when the surface inversion layer
breaks up.
Fig. 8. ManneKendall test for monthly maximum of daily maximum 8-h mean of surface ozone concentration for the period from 2001 to 2007 from January to December. Symbols
as in Fig. 6.
1956
Table 7
Kendall rank correlation between daily maximum 8-h mean and daily mean
temperature.
Code
Period
Association (Kendalls s)
ES01eES15
ES02eES07
ES04
ES06
ES08
ES09
ES10
ES11
ES12
ES13
ES14
ES16
ES17
PT04
1993e2007
1993e2009
1993e2001
2008e2009
1998e2009
1998e2009
1998e2009
1999e2009
1998e2009
2000e2009
2000e2009
2001e2009
2008e2009
1990e2007
0.48
0.41
0.46
0.2
0.08
0.45
0.32
0.43
0.48
0.46
0.55
0.22
0.27
0.07
Table 8
Kendall rank correlation between daily maximum 8-h mean and daily mean solar
radiation.
Code
Period
Association (Kendalls s)
ES01eES15
ES02eES07
ES04
ES06
ES08
ES09
ES10
ES11
ES12
ES13
ES14
ES16
ES17
1993e2007
1993e2009
1993e2001
2008e2009
1998e2009
1998e2009
1998e2009
1999e2009
1998e2009
2000e2009
2000e2009
2001e2009
2008e2009
0.45
0.52
0.59
0.35
0.26
0.48
0.41
0.50
0.53
0.50
0.54
0.34
0.39
1957
Fig. 11. Association values between daily maximum 8-h mean and daily mean solar
radiation.
Fig. 9. Red circles indicate the stations which present the highest association values
between daily maximum 8-h mean and daily mean temperature. Green circles indicate
the stations that present the highest association values between daily maximum 8-h
mean and daily mean solar radiation. (For interpretation of the references to colour in
this gure legend, the reader is referred to the web version of this article.)
Fig. 10. Association values between daily maximum 8-h mean and daily mean
temperature.
1
SOMO35 Accumulated ozone concentrations in excess of 70 mg m3 (or 35 ppb).
SOMO35 is the sum of the amounts by which maximum daily 8-h concentrations
(in mg m3) exceed 70 mg m3 on each day in a calendar year (WHO, 2001).
2
MTDM mean of the 10 highest daily maximum ozone concentrations (based on
hourly mean data) during AprileSeptember, corresponding approximately to the
mean of the data 95th percentile.
1958
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