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Water Air Soil Pollut (2011) 221:275286

DOI 10.1007/s11270-011-0789-6

Have Meteorological Conditions Reduced NO2


Concentrations from Local Emission Sources
in Gothenburg?
Lin Tang & David Rayner &
Marie Haeger-Eugensson

Received: 22 November 2010 / Accepted: 2 March 2011 / Published online: 24 March 2011
# Springer Science+Business Media B.V. 2011

Abstract The risks of exceeding EU limit values for


NO2 concentrations have increased in many European
cities, and compliance depends strongly on meteorological conditions. This study focuses on meteorological
conditions and their influences on urban background
NO2 concentrations in the city of Gothenburg for 1999
2008. The relations between observed NO2 concentrations and meteorological conditions are constructed
using two modelling approaches: multiple linear regression and synoptic regression. Both approaches assume
no trends in emissions over the study period. The
multiple linear regression model is established on
observed local meteorological variables. The synopticregression model first groups days according to synoptic
conditions using Lamb Weather Types and then uses
linear regression on each group separately. A model
comparison shows that linear regression model and
synoptic-regression model perform satisfactory. The
synoptic-regression model gives higher explained variance (R2) against observations during the calibration
years (19992007), in particular for the morning peak
and afternoonevening peak concentrations, but the

improvement in the validation period is weak. The


annual mean NO2 variations, and their trends during the
study period, were assessed using the synopticregression model. The synoptic-regression model is able
to explain 54%, 42% and 80% of the annual variability
of daily mean, morning peak and afternoonevening
peak NO2 concentrations, respectively. The observed
and modelled annual means of the daily mean and
morning/afternoonevening peak NO2 concentrations
show decreasing trends from 1999 to 2008. All trends,
except the trend in annual-average observed morning
peak NO2 are statistically significant. The presence of
trends in the modelled NO2 concentrationseven
though emissions are assumed to be constantleads
us to conclude that weather and climate alone are
responsible for a substantial fraction of the recent
declines in observed NO2 concentrations in Gothenburg.
Favourable meteorological conditions may have mitigated increases in local NO2 emissions during 1999 to
2008.
Keywords NO2 concentrations . Dispersion
conditions . Statistic downscaling . Linear regression
model . Synoptic-regression model . Gothenburg

L. Tang : M. Haeger-Eugensson
IVL Swedish Environmental Research Institute Ltd,
P.O. Box 5302, 40014 Gothenburg, Sweden

1 Introduction

L. Tang (*) : D. Rayner


Department of Earth Sciences, University of Gothenburg,
Sweden,
P.O. Box 460, 405 30 Gothenburg, Sweden
e-mail: lin.tang.gu@gmail.com

Despite significant decreases in nitrogen dioxide


(NO2) concentrations in the last 15 years, the EU
standard for annual-average NO 2 concentration
(40 g/m3) was exceeded at a city street site and a

276

Water Air Soil Pollut (2011) 221:275286

traffic route site in Gothenburg during all years from


2003 to 2006 (Pleijel et al. 2009). During 19902000,
anthropogenic nitrogen oxide (NOx = NO + NO 2)
emissions in Western Europe declined steeply, due
to the introduction of improved vehicle technologies
and stringent inspection systems, while from 2000 to
2005, the downward emission trend had flattened out
(Vestreng et al. 2009). In addition, increased "direct"
NO2 emissions, due to increased use of oxidative
catalytic converters in diesel vehicles, and increased
background ozone concentrations, are thought to be
offsetting the effect of reductions in NOx emissions
on NO2 concentrations (Carslaw et al. 2007; Grice et
al. 2009). The NO2 fraction in primary emissions is
higher for diesel-fuelled cars (Pleijel et al. 2009), and
the fraction of vehicle-kilometres using diesel has
increased by a factor of 2.5 in Sweden between 1994
and 2008 (Haeger-Eugensson et al. 2010).
Local NOx emissions from different sources contribute to local NO2 concentrations. Road transport has
been the dominating source of NOx emissions over
Europe since 1970 and contributes with 40% to the
total emissions in 2005 (Vestreng et al. 2009). In the
city of Gothenburg, NOx emissions from vehicles and
ships occupy the major portion of total emissions, with
40% and 38% in 2005 (Haeger-Eugensson et al. 2010).
The NOx emissions from vehicles and ships in the city
of Gothenburg slowly deceased from 9,300 ton/year in
1998 to 5,930 ton/year in 2004 but increased again to
7,104 ton/year by 2007, with particular increases from
ships (Haeger-Eugensson et al. 2010).
The variation of air pollutant concentrations is
controlled by not only natural and anthropogenic
emissions but also chemical transformations, removal
processes (wet and dry deposition), local dispersion
conditions and long-range transport. Chemical loss
for NO2 in the atmosphere occurs during daytime and
night-time. During daytime, one important removal
path is the photolysis of NO2 to generate oxygen
atoms driven by solar actinic flux (Eqs. 13), which is
the key reaction in photochemical smog formation.
NO2 hv > 340 nm ! NO O

O O2 ! O3

NO O3 ! NO2 O2

The other is the formation of nitric acid (HNO3) by


the reaction of gas phase NO2 and hydroxyl radical
(OH; Eq. 4)
NO2 OH ! HNO3

During the night-time, the appearance of nitrate


radical (NO3), formed by the reaction of NO2 and
ozone (O3; Eq. 5), further reacts with NO2 to form
dinitrogen pentoxide (N2O5; Eq. 6). A considerable
loss of N2O5 is assumed to occur on the surface of
aqueous aerosol particles by reaction Eq. 7 (Platt et al.
1984). Thus, the hydrolysis of N2O5 on the surfaces
of aerosol particles is the dominant removal channel
for nitrogen oxides at night (Riemer et al. 2003).
NO2 O3 ! NO3 O2

NO3 NO2 ! N2 O5

N2 O5 H2 O ! 2HNO3 aerosol

Large-scale meteorological fluctuation and local


meteorological conditions speed up or slow down
these processes through the change of temperature,
humidity, wind speed, etc., and finally decide the
inter-annual variation of air pollutants (Velders and
Matthijsen 2009). Carslaw et al. (2007) predicted the
impact of changes in the NO2 fraction of primary
emissions on future ambient concentrations in London
and highlighted that the risks of exceeding the EU limit
value in 2010 depended strongly on the prevailing
meteorological conditions. Grundstrm et al. (2011)
found that the number winter-time NO2 and NO airquality standard exceedances in Gothenburg is correlated with the North Atlantic Oscillation (NAO). They
found a positive trend in the number of hourly NO2
concentrations exceeding 90 g/m3/year over 1997
2006, which they concluded was related to an
increasing trend in the NAO.
In line with this, climate change has been identified
as an important factor influencing air quality and
should be taken into account for future policy design
(Giorgi and Meleux 2007; Jacob and Winner 2009).
Therefore, constructing impact models with appropriate meteorological conditions and climate change
signals is becoming essential, both to guide policy

Water Air Soil Pollut (2011) 221:275286

and to understand the effect of meteorological conditions and climate change on regional/local air
quality.
A conventional way to analyse the response of air
quality to meteorological conditions and climate
change is to run complex chemical transport models
(CTMs) driven by fields generated from a regional
climate model (RCM). The RCM has itself been
forced with boundary conditions from a global
climate model, a process known as dynamical
downscaling (Giorgi et al. 2001; Schmidli et al.
2007). Dynamical downscaling involves explicitly
solving equations that describe the physical dynamics
of the atmospheric system (Giorgi and Mearns 1991).
However, running a high-resolution CTM is time
consuming and expensive work (Giorgi and Meleux
2007). Alternatively, statistical downscaling methods,
where relationships in the system are derived from
observational data, are relatively simple and easily
implemented. Statistical downscaling methods have
been widely applied in Sweden, for studies covering
monthly and daily precipitation (Hanssen-Bauer et al.
2005; Chen et al. 2006; Wetterhall et al. 2009); annual
surface ozone levels (Tang et al. 2009) and urban
climate (Thorsson et al. 2011).
According to Wilby and Wigley (1997), statistical
downscaling techniques can be roughly grouped into
three categories: regression methods, circulationbased methods and weather generator methods.
Regression methods are most common in statistical
downscaling studies, including linear (such as linear
regression, multivariate regression and canonical
correlation analysis) and non-linear methods (neural
networks). Circulation-based methods classify atmospheric circulation into a limited number of classes
and simulate variables based on the circulation types.
Recently, a new downscaling approach combining
regression methods and circulation-based methods
has been applied in air quality research (Cheng et al.
2007a, b; Demuzere and van Lipzig 2010a, b). This
synoptic-regression approach, applying a circulation
pattern classification prior to the multiple linear
regression analysis, has proven to be superior to a
simple regression approach.
This study focuses on the impact of meteorological
conditions on urban background NO2 concentrations
during 19992008 in the city of Gothenburg. Two
statistical downscaling methodsmultiple linear regression and synoptic regressionwere established

277

and evaluated against observed daily mean, morning


peak and afternoonevening peak NO2 concentrations.
Both models produced results that were highly
correlated with observed concentrations. We then used
the synoptic-regression model to further investigate the
inter-annual variations and trends in observed NO2
concentrations. The hypotheses of this study were:
&

&

The variation of NO2 concentrations in the city of


Gothenburg would be strongly influenced by local
meteorological conditions as well as synoptic
weather patterns.
The inter-annual variations and trends of NO2
concentrations depend strongly on the eventual
meteorological conditions.

2 Data and Methods


2.1 Data
2.1.1 Air Quality and Local Meteorological Data
Gothenburg is a city on the western coast of Sweden,
with about 600,000 inhabitants and an area of
451 km2. The air pollution monitoring site Femman,
an urban background site, is located on a rooftop
(25 m) in the city centre and close to the harbour. The
site has been maintained by the Environmental Office
in Gothenburg since 1965. We complemented the
meteorological records from Femman (see below)
with data from the nearby sites Lejonet (located
around 1.3 km north-east of the Femman site) and
Jrnbrott (located approximately 7 km south-west of
Gothenburg city centre). Jrnbrott, a meteorological
site with a 100-m mast, is the nearest site to the city
equipped with vertically distributed temperature and
wind instruments. The meteorological parameters that
determine the dispersion conditions are rather similar
between the Jrnbrott and Femman site, even if there
may be a small time lag and somewhat different
inversion heights (Haeger-Engensson 1999). The
temperature gradient at Jrnbrott has been used to
investigate the relationship between winter inversions
and urban aerosol by Janhll et al. (2006), demonstrating that the temperature gradient at Jrnbrott can
capture the urban morning ground-level inversion.
The predictands in this study were daily mean
(24-h average), morning peak (hourly maximum

278

Water Air Soil Pollut (2011) 221:275286

during 0500 to 1200 hours local time (LT)) and


afternoonevening peak (hourly maximum during
1400 to 0200 hours LT) NO2 concentrations at
Femman. The predictors were the local meteorological variables measured at Femman, rainfall and
global radiation at Lejonet and vertical temperature
difference between 3 and 73 m at Jrnbrott.
In this study, the impact of meteorological conditions on local NO2 concentrations is our focus. In
order to minimise the influence from emission
reductions, we selected the time period from 1999 to
2008 during which there was a modest downward
trend in NOx emissions over Europe (Vestreng et al.
2009).

al. 2009). In this study, a backward step-wise method


was conducted to find predictive equations for the
NO2 concentrations with the meteorological variables
as the predictor variables. The independent meteorological variablestemperature, relative humidity,
wind speed, rainfall, etc.were included in the initial
model, then the least-relevant variables were removed
based on the p value of an F statistic. The objective is
to find the variables that best correlate with the NO2
concentrations and the order-of-magnitude of influence. MATLAB was used to conduct the backward
step-wise regression for each season separately, with
the exit tolerance (minimum p value for a predictor to
be removed) of 0.10.

2.1.2 Lamb Weather Classification

2.2.2 Synoptic-Regression Method

Daily and 6-h mean sea level pressures (SLP) for a


16-point gird centred over the Gothenburg city centre
(57.7 N, 11.97 E) were obtained from the NCEP/
NCAR Reanalysis database 2.52.5 degree pressure
fields (Kalnay et al. 1996). Circulation indices
(describing the geostrophic winds) and Lamb weather
types (Jenkinson and Collison 1977) were then
calculated following Chen (2000). This classification
scheme has 27 weather types: anticyclone (A),
cyclone (C), eight directional types (NE, E, SE, ),
16 hybrid types (ANE, AE, ASE, CNE, CE, CSE, )
and one unclassified type (U). In this study, the 27
weather types were consolidated into 11 weather
types according to their directions: U, A, C, NE, E,
SE, S, SW, W, NW, N. For a more detailed
description for each weather type, see Chen (2000)
and Tang et al. (2009).

Synoptic regression is a combination of circulationbased and regression-based methods. The circulationbased method contains information about the largescale atmospheric conditions. The regression method,
based on local meteorological variables, reflects the
impact of local meteorological conditions. The
synoptic-regression model, thus reflecting both local
meteorological conditions as well as atmospheric
circulation, has been applied in air-quality assessment
(Cheng et al. 2007a, b). Table 1 shows that the three
circulation indices used for classification of circulation patternswesterly wind component (u), southerly
wind component (v) and vorticity ()show significant correlations with NO2 concentrations. Therefore,
Lamb weather type based on daily mean SLP and SLP
at 0600 and 1800 hours were used for the synopticregression models for daily mean, morning peak and
afternoonevening peak NO2 concentrations, respec-

2.2 Methods
2.2.1 Multiple Linear Regression Method
Multiple linear regression is used to establish a
quantitative relationship between a group of predictor
variables and a predictant. The relationship is useful to
understand which predictors have greatest effect and
the direction of the effect, and to predict future values
of the predictant. The stepwise linear regression
method has been widely used in synoptic climatological air pollution studies due to its ability to identify
sequentially the optimum subset of predictor variables
(Lam and Cheng 1998; Demuzere et al. 2009; Tang et

Table 1 Correlation coefficient for circulation indices and


daily mean, morning peak, afternoonevening peak NO2 during
19992008 after detrending
Daily Morning Afternoon
mean peak
evening peak
Westerly wind component (u) 0.23

0.18

0.23

Southerly wind component (v) 0.28

0.30

0.26

0.19

0.15

0.20

Vorticity ()

Westerly wind component (u), southerly wind component (v) and


vorticity (). All correlations are statistically significant at p<0.05
level

Water Air Soil Pollut (2011) 221:275286

tively. With 11 consolidated weather types (A, C, NE,


), 44 (11 weather types4 seasons) regression models
in total were established for each predictant.
2.2.3 Predictor Selection
With statistical downscaling, an important step is to
select appropriate predictors. One of the demands in
selection of appropriate predictors is that the largescale variables should be strongly correlated with the
surface variables of interest (Wetterhall et al. 2009).
Table 2 lists local observed meteorological variables
used as predictors in the multiple regression models.
Daily mean meteorological variables are used as
predictors for daily mean NO2 concentrations, the
sub-daily meteorological conditions at 0600 and 1200
hours are used to model the morning peak and those
at 1800 and 0000 hours for the afternoonevening
peak. Most of predictors are significantly correlated
with corresponding NO2 concentrations, except for
relative humidity at 0600 hours and global radiation at
1800 and 0000. Among those predictors, local wind
speed and near-surface vertical temperature difference, dictated by atmospheric stability, are the most
significant variables influencing NO2 dispersion and
transport. The multiple regression models were constructed for seasonal and annual time series.

279

NOx emission index in Gothenburg was calculated


for a typical road in the city centre (Grda) for year
2006. It was determined from actual traffic intensity
measurements and type of vehicles. NOx emission
factors for each type of vehicles were based on the
Artemis emission model (Andre 2005). The calculations were carried out for daily mean, morning peak
and afternoonevening peak of NOx emissions,
respectively (see Fig. 1). These emission indices were
then used as one of the predictors in the responding
prediction models.
2.2.5 Model Evaluation Measures
A set of statistical measures was used to quantitatively measure and compare the performances of the
linear regression model and the synoptic-regression
model. The following measures were used in this
study: correlation coefficient (r), mean bias error, root
mean square error (RMSE) and explained variance
(R2). In addition, the MannKandell method (Yue et
al. 2002) was used to assess whether trends were
statistically significant, and the TheilSen method
(Sen 1968) was used to estimate trends.

3 Results

2.2.4 Weekly Emission Index

3.1 Seasonal, Weekly and Diurnal Cycles

The variability of city activities induces significant


short-term variations of emissions, especially in urban
areas (Ziomas et al. 1995). The weekly emission
index, one of the significant predictors in Table 2,
should be taken into account in any prediction model
(Ziomas et al. 1995; Cheng et al. 2007a). A weekly

Diurnal, seasonal and weekly variations of NO2


concentrations depend on NOx emissions, meteorological conditions, chemical formation, chemical loss
(Boersma et al. 2008) and loss through deposition.
Figure 2a shows two daily peaks in NO2 concentrations. The morning peak NO2 concentrations are

Table 2 Predictors for daily mean, morning peak and afternoonevening peak NO2 concentrations
Daily mean

Weekly emission index, daily maximum temperature, daily minimum temperature, daily mean relative humidity,
daily mean wind speed, daily mean surface pressure, daily mean global radiation, daily total rainfall, daily
mean vertical temperature difference between 73m and 3m

Morning peak

Weekly emission index, temperature at 0600 and 1200 hours, relative humidity at 0600 and 1200 hours, wind
speed at 0600 and 1200 hours, surface pressure at 0600 and 1200 hours, global radiation at 0600 and 1200
hours, daily total rainfall, vertical temperature difference between 73m and 3m at 0600 and 1200 hours.

Afternoon-evening
peak

Weekly emission index, temperature at 1800 and 0000 hours, relative humidity at 1800 and 0000 hours, wind
speed at 1800 and 0000 hours, surface pressure at 1800 and 0000 hours, global radiation at 1800 and 0000
hours, daily total rainfall, vertical temperature difference between 73m and 3m at 1800 and 0000 hours.

Except for relative humidity at 0600 hours and global radiation at 1800 and 0000 hours, all the other meteorological variables have
significant correlation with responding predictors at p<0.05 level after detrending for 19992008

280

Water Air Soil Pollut (2011) 221:275286

1.4

explained by the higher traffic volume in urban areas


and poor dispersion before daytime vertical mixing is
established. The afternoonevening peak NO2 concentrations typically peak later than the rush hour
maximum, largely due to decreased mixing height and
stagnant atmospheric conditions in the evening. The
morning peak occurs at a similar time for all seasons,
while afternoonevening peaks occur at different
times in different seasons: around 17001800 hours
in winter and fall, 23000000 hours in spring and
summer. The delayed spring/summer afternoonevening peak is associated with delayed evening/nighttime traffic volume and a later decline in the wind
speed and mixing height (Bigi and Harrison 2010).
In the northern countries, higher NO2 concentration in winter time (Fig. 2b) is mainly due to higher
emissions from combustion and traffic in combination

Traffic emission index

1.2
1
0.8
Daily mean
Morning peak
Afternoonevening peak

0.6
0.4
0.2
0
Sun.

Mon.

Tue.

Wed.

Thu.

Fri.

Sat.

Fig. 1 Calculated weekly emission index for daily mean,


morning peak and afternoonevening peak in Gothenburg

a
45
WinterDJF

SpringMAM

SummerJJA

AutumnSON

40

NO2 (g/m3)

35

30

25

20

15
00:00

04:00

08:00

12:00

50

60
Daily mean
Morning peak
Afternoonevening peak

50

35

45
NO2 (g/m3)

40

40
35

30

30

25

25

20

20

15
Jan. Feb. Mar. Apr. May Jun. Jul. Aug. Sep. Oct. Nov. Dec.

15
Sun.

Fig. 2 a Durinal cycle of NO2 concentrations for each season


during 1999 to 2008. b Seasonal cycle of daily mean, morning
peak, afternoonevening peak NO2 concentrations in Gothenburg

Daily mean
Morning peak
Afternoonevening peak

55

45
NO2 (g/m3)

20:00

60
55

16:00

Mon.

Tue.

Wed.

Thu.

Fri.

Sat.

for 19992008. c Weekly cycle of daily mean, morning peak,


afternoonevening peak NO2 concentrations for 19992008

Water Air Soil Pollut (2011) 221:275286

281

with frequently occurring poor dispersion in the


early morning during high-pressure situations
(Haeger-Engensson 1999). Another reason for
higher NO2 concentrations is lower OH concentrations in winter, which results in the weak chemical
loss of NO2 during the daylight hours (Boersma et
al. 2009). Apart from better dispersion in summer,
higher water vapour concentrations and more ultraviolet flux lead to higher OH concentrations in that
season (Spivakovsky et al. 2000). Therefore, stronger daytime chemical loss is strengthening the low
NO2 levels in summer.
The weekly variability of NO2 is entirely a
consequence of human activity (Flemming et al.
2005). Similar with USA, Europe and Japan (Beirle
et al. 2003), the weekly cycle of NO2 in Gothenburg
(Fig. 2c) reflects the life-style of highly developed
industrialised society: industrial activity and traffic
are reduced during weekends and Sunday/Saturday
minimum of NO2 are expected. NO2 concentrations
are kept at a similar high level from Monday to
Friday.
3.2 Model Comparison
Our comparison of the linear regression and synopticregression models was based on the statistical
measures shown in Table 3 and Fig. 3. The R2 of
both models against observations were calculated in
each season for calibration years 19992007 and
validation year 2008 separately (Table 3). Figure 3
shows that both models were able to reproduce much
of the variation in observed NO2. However, the
synoptic-regression model captured more of the
observed variability in daily mean, morning peak
Table 3 Explained variance
(R2) of the multiple linear
regression and synopticregression models against
observations for each season

Calculations were conducted


for daily mean, morning peak
and afternoonevening peak
NO2 concentrations during
calibration years (19992007)
and validation year (2008),
respectively. All correlations
are statistically significant at
p<0.05 level

and afternoonevening peak NO2 concentrations


during the calibration years. In particular, the
synoptic-regression model was better able to represent
the higher observed values, especially for the morning
peaks. RMSE and MAE for calibration years, given in
Fig. 3, show better performance for the synopticregression model, especially in simulating the morning and afternoonevening peaks. For the validation
year 2008, the performance of the two models is more
similar. Disappointingly, the highest observed morning peak value that year is severely underestimated.
3.3 Assessment of Annual Mean NO2 Variations
and Trends
In order to display how much of the year-to-year
variability and trends in NO2 concentrations are
captured by the synoptic-regression model, the annual
mean variation and the trend of observed and
modelled daily mean, morning peak and afternoon
evening peak NO2 concentrations from 1999 to 2008
are shown in Fig. 4. Annual mean values from the
synoptic-regression model were based on calibration
year 19992007 and validation year 2008.
The synoptic-regression model is able to explain
54%, 42% and 80% of the annual variability of daily
mean, morning peak and afternoonevening peak
NO2 concentrations, respectively. Furthermore, the
modelled annual trends follow the observed decreasing trends. The slopes of linear trends, estimated by
TheilSen method, for observed daily mean, morning
peak and afternoonevening peak annual mean NO2
concentrations are 0.45, 0.20 and 0.78 g/m3/
year and 0.23, 0.27 and 0.65 g/m3/year for
synoptic-regression modelled values. All trends,

Calibration years (19992007)

Validation year (2008)

Multiple linear regression model (daily mean/morning peak/afternoonevening peak)


Winter (DJF)

0.73/0.58/0.57

0.57/0.44/0.57

Spring (MAM)

0.66/0.57/0.38

0.71/0.64/0.50

Summer (JJA)

0.61/0.49/0.36

0.71/0.50/0.37

Annual

0.71/0.59/0.50

0.68/0.55/0.49

Synoptic-regression model (daily mean/morning peak/afternoonevening peak)


Winter (DJF)

0.80/0.71/0.67

0.59/0.34/0.49

Spring (MAM)

0.77/0.71/0.54

0.70/0.58/0.49

Summer (JJA)

0.71/0.62/0.50

0.71/0.60/0.49

Annual

0.78/0.72/0.61

0.71/0.50/0.51

282

Water Air Soil Pollut (2011) 221:275286

a
200

(a)

200

Calibration year 19992007


Verification year 2008

180
160

R2 = 0.78

140

Model NO2 (g/m3)

Model NO2 (g/m3)

Calibration year 19992007


Verification year 2008

160

R2 = 0.71
RMSE = 7.24
120
MAE = 5.49
100
80
60

140
RMSE = 6.28
120
MAE = 4.63
100
80
60

40

40

20

20

(b)

180

50

100

150

200

Obs NO2 (g/m3)

50

b
Calibration year 19992007
Verification year 2008

(a)
300

200

300

150

200
150

100

100

50

50
0
0

50

100

R2 = 0.72
RMSE = 15.24
MAE = 10.85

250
Model NO2 (g/m3)

200

150

200

250

300

Calibration year 19992007


Verification year 2008

(b)

R2 = 0.59
RMSE = 18.29
MAE = 13.24

250
Model NO2 (g/m3)

150

350

350

100
Obs NO2 (g/m3)

350

50

100

150

200

250

300

350

Obs NO2 (g/m3)

Obs NO2 (g/m )

c
350

350

(a)
300

150

200
150

100

100

50

50

50

100

R2 = 0.61
RMSE = 16.12
MAE = 12.05

250
Model NO2 (g/m3)

200

150

200

Obs NO2 (g/m3)

250

300

Calibration year 19992007


Verification year 2008

300

R2 = 0.50
RMSE = 18.36
MAE = 14.04

250
Model NO2 (g/m3)

(b)

Calibration year 19992007


Verification year 2008

350

50

100

150

200

Obs NO2 (g/m3)

250

300

350

Water Air Soil Pollut (2011) 221:275286

283

Fig.

3 Observed and modelled NO2 concentrations from the


multiple linear regression (a) and synoptic-regression (b)
models. The major statistical measures for the calibration years
(19992007) are shown. a daily mean, b morning peak and c
afternoonevening peak NO2 concentrations, respectively

modelled using a multiple linear regression model and a


synoptic-regression model. The two models are in
reasonable agreement with observed NO2 concentrations. The synoptic-regression model captured more of
the daily and yearly variability in mean and extreme
NO2 concentrations. Different from the multiple linear
regression model, the synoptic-regression model
includes circulation pattern classification which has
clear physical links with high/low air pollution in this
region (Tang et al. 2009). The circulation pattern
classification provides a clear insight in typical largescale atmospheric structures and associated anomalies in
meteorological variables during high/low pollution
events (Demuzere et al. 2009). The synoptic-regression
approach has been demonstrated to be suitable for rural
O3 concentration for a mid-latitude area, and the better
performance of the synoptic-regression model is bene-

except the trend in annual-average observed morning


peak NO2, are statistically significant.

4 Discussion and Conclusions


The study presents firstly the characteristics of NO2
concentrations in the urban background site in
Gothenburg by investigating the diurnal, weekly and
annual cycles. Secondly, the daily mean, morning peak
and afternoonevening peak NO2 concentrations are

NO2 (g/m 3)

29
28

Obs
Syn.Reg.
TrendObs*

27

TrendSyn.Reg.*

26
25
24
23
22
1998 1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009
year

c
45

51

49

Obs
Syn.Reg.
TrendObs*

48

TrendSyn.Reg.*

50
44

NO2 (g/m 3)

NO2 (g/m 3)

43

42

41

40

Obs
Syn.Reg.
TrendObs
TrendSyn.Reg.*

39
1998 1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009
year

Fig. 4 Annual variations and linear trends for observed and


synoptic-regression model based NO2 concentrations from
1999 to 2008. a Annual-average daily mean, b morning peak

47
46
45
44
43
42
41
1998 1999 2000 2001 2002 2003 2004 2005 2006 2007 2008 2009
year

and c afternoonevening peak NO2 concentrations, respectively. Trends marked with asterisk in the legend represent
statistically significant linear trends at p<0.05 level

284

ficial for representing higher-order statistical moments


of the air quality level distributions (Demuzere and van
Lipzig 2010a). Our study extends the application of
synoptic-regression approach to the urban environment
and NO2 concentrations, even though urban NO2
variations depend dramatically on local emissions. The
results confirm the hypothesis that local and synoptic
weather conditions strongly influence urban NO2 concentrations in the city of Gothenburg, as well as
demonstrating the advantage of the synoptic-regression
approach for air quality assessment.
It appears that for the study period 1999 to 2008,
54%, 42% and 80% of the annual variability of daily
mean, morning peak and afternoonevening peak
NO2 concentrations, respectively, can be ascribed to
variations in local and synoptic weather conditions.
Although both the primary emitted NO2 fraction and
the total NOx emissions from transportation have in
fact increased in city of Gothenburg during recent
years (Haeger-Eugensson et al. 2010), statistically
significant decreasing trends were detected in both
observed and modelled NO2 concentrations at the
urban background site. Comparing the trends in the
modelled and observed NO2, it appears that weather
and climate alone are responsible for 51% (0.23/
0.45), 135% (0.27/0.20) and 83% (0.65/0.78)
of the declines in annual-average daily mean, morning
peak and afternoonevening peak NO2, respectively.
That is, our modelling suggests that the decline in
daily mean and afternoonevening peak NO2 concentrations would have been much less if it were not for
favourable meteorological conditions and that morning peak NO2 concentrations would in fact have risen
under average conditions.
Our finding of statistically significant, decreasing
trends in average NO2 concentrations might seem to
contradict Grundstrm et al. (2011), who found a
positive trend in the number of hourly NO2 concentrations exceeding 90 g/m3/year in Gothenburg in
winter. This apparent discrepancy is explained by the
details of the two studies. Firstly, Grundstrm et al.
(2011) analysed 19972006, whereas we analysed
19992008 and the number of winter exceedences in
20062007 and 20072008 were comparatively low.
When data for 20062007 and 20072008 are
included, the trend in exceedences disappears. Secondly, in our study, we modelled average daily mean,
morning peak and afternoonevening peak NO2
concentrations rather than threshold exceedences.

Water Air Soil Pollut (2011) 221:275286

Average concentrations are statistically more sensitive


to trends than exceedence counts, although exceedence counts are more closely aligned with policy
objectives. Finally, our study investigated trends in
annual averages, whereas Grundstrm et al. restricted
their study to winter season. Only 40% of the hourly
NO2 concentrations exceeding 90 g/m3/year in city
of Gothenburg occur during wintertime.
At this stage, we are not able to determine whether
the trends in modelled NO2 are specific to the study
period or whether they are part of a longer-term trend.
However, it appears thatat least in the recent past
weather and climate conditions in Gothenburg have
been an important factor contributing to the trend
towards lower average NO2 concentrations.
Acknowledgements This work was supported by the GMV
(Centre for Environment and Sustainability, Gothenburg,
Sweden) and GAC (Gothenburg Atmospheric Science Centre)
foundations. The authors appreciate the assistance of Mr. Jan
Brandberg from Environmental Agency in Gothenburg in
providing measured meteorological and air quality data for
Femman. We gratefully acknowledge the NOAA/OAR/ESRL
PSD, Boulder, Colorado, USA, for providing the NCEP
Reanalysis data. Finally, we would like to thank an anonymous
reviewer for the careful reading and interesting suggestions.

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