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Atmospheric Environment 126 (2016) 218e224

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Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Impact of passenger car NOx emissions and NO2 fractions on urban


NO2 pollution e Scenario analysis for the city of Antwerp, Belgium
Bart Degraeuwe a, *, Philippe Thunis a, Alain Clappier b, Martin Weiss c, Wouter Lefebvre d,
Stijn Janssen d, Stijn Vranckx d
a
European Commission, JRC, Institute for Environment and Sustainability, Air and Climate Unit, Via E. Fermi 2749, Ispra (VA) 21027, Italy
b
Universit
e de Strasbourg, Laboratoire Image Ville Environnement, 3, Rue de l'Argonne, Strasbourg 67000, France
c
European Commission, JRC, Institute for Energy and Transport, Sustainable Transport Unit, Via E. Fermi 2749, Ispra (VA) 21027, Italy
d
VITO, Flemish Institute for Technological Research, Boeretang 200, Mol, Belgium

h i g h l i g h t s

 We model street canyon NO2 for different diesel car NOx emissions and NO2 fractions.
 We consider the changes in European, regional and local street canyon emissions.
 Air quality would benefit from compliance of diesel cars with Euro 6 under real-driving conditions.
 High NO2 fractions impact the exceedance of the hourly limit value of 200 mg/m3.

a r t i c l e i n f o a b s t r a c t

Article history: The annual NO2 concentrations in many European cities exceed the established air quality standard. This
Received 12 June 2015 situation is mainly caused by Diesel cars whose NOx emissions are higher on the road than during type
Received in revised form approval in the laboratory. Moreover, the fraction of NO2 in the NOx emissions of modern diesel cars
18 November 2015
appears to have increased as compared to previous models. In this paper, we assess 1) to which level the
Accepted 19 November 2015
Available online 27 November 2015
distance-specific NOx emissions of Diesel cars should be reduced to meet established air quality stan-
dards and 2) if it would be useful to introduce a complementary NO2 emissions limit. We develop a NO2
pollution model that accounts in an analysis of 9 emission scenarios for changes in both, the urban
Keywords:
Urban air quality modelling
background NO2 concentrations and the local NO2 emissions at street level. We apply this model to the
NOx emissions of diesel cars city of Antwerp, Belgium. The results suggest that a reduction in NOx emissions decreases the regional
NO2 fraction and urban NO2 background concentration; high NO2 fractions increase the ambient NO2 concentrations
only in close spatial proximity to the emission source. In a busy access road to the city centre, the average
NO2 concentration can be reduced by 23% if Diesel cars emitted 0.35 g NOx/km instead of the current
0.62 g NOx/km. Reductions of 45% are possible if the NOX emissions of Diesel cars decreased to the level
of gasoline cars (0.03 g NOx/km). Our findings suggest that the Real-Driving Emissions (RDE) test pro-
cedure can solve the problem of NO2 exceedances in cities if it reduced the on-road NOx emissions of
diesel cars to the permissible limit of 0.08 g/km. The implementation of a complementary NO2 emissions
limit may then become superfluous. If Diesel cars continue to exceed by several factors their NOx
emissions limit on the road, a shift of the vehicle fleet to gasoline cars may be necessary to solve per-
sisting air quality problems.
© 2015 European Commission, Joint Research Centre, IES, Air and Climate Unit. Published by Elsevier Ltd.
This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).

1. Introduction

Despite a significant reduction of pollutant emissions in past


Abbreviations: RDE, real driving emissions; PEMS, portable emission measure- years (EEA, 2013), many European regions still face problems in
ment system. complying with the European Union's (EU) air quality directive
* Corresponding author. (European Commission (EC), 2008). Nitrogen dioxide (NO2) has
E-mail address: bart.degraeuwe@jrc.ec.europa.eu (B. Degraeuwe).

http://dx.doi.org/10.1016/j.atmosenv.2015.11.042
1352-2310/© 2015 European Commission, Joint Research Centre, IES, Air and Climate Unit. Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).
B. Degraeuwe et al. / Atmospheric Environment 126 (2016) 218e224 219

received special attention for its adverse respiratory effects (WHO, and the general activity pattern. Second, pollution modelling has to
2013) and because it acts as a precursor of both tropospheric ozone be accurate. This implies modelling at very different scales ranging
(O3) and particulate matter (Beelen et al., 2014). The ambient NO2 from the background pollution at the larger regional and conti-
concentrations in many European cities continue to exceed the nental scale to the details at city and street level. This section ex-
annual limit of 40 mg/m3 while the hourly limit (200 mg/m3) not to plains how we address these two challenges of modelling NO2
be exceeded more than 18 times per year is less problematic and pollution.
mostly occurs when the yearly limit of 40 mg/m3 is already excee-
ded (EC, 2008; Kiesewetter et al., 2014, 2013). In fact, most of the 2.1. Emission scenarios
NO2 non-compliances occur in city centres (EEA, 2013), mainly
caused by traffic-related NOx emissions originating from diesel We establish the current level of NOx emissions based on the
vehicles. In fact, diesel passenger cars, including new Euro 6 cars, TNO-MACC-II inventory for the year 2009 (Kuenen et al., 2014). In a
show much higher distance-specific NOx emissions on the road next step, we develop scenarios for future road traffic emissions.
than under type-approval conditions in the laboratory. The intro- The scenarios capture the plausible range of (i) distance-specific
duction of progressively lower emission limits has thus not trans- emissions of novel vehicles certified according to the Euro 6 and
lated into an adequate reduction of on-road NOx emission. This was VI standards, (ii) the future share of Diesel and gasoline within the
demonstrated both with Portable Emission Measurement Systems vehicle fleet and (iii) the future vehicle kilometres driven. The
(PEMS) (Franco et al., 2014; Weiss et al., 2012) and remote sensing chosen scenarios also include extreme cases; we would thus expect
(Chen and Borken-Kleefeld, 2014). In addition, the NO2 fraction in that the actual future road traffic emissions lie somewhere in be-
the NOx exhaust of diesel cars has been continuously increasing tween the scenarios considered here. As scenario year 2030 was
following the introduction of oxidative after-treatment technolo- chosen and we assume that the whole fleet complies with Euro 6/
gies. As a direct effect, NO2 ambient concentrations close to the VI. Other traffic emissions (VOC and particulate matter) and all the
emission source may increase. Indirectly, higher O3 levels could be emissions of other sectors (e.g. industry, residential …) were kept
reached within cities as a result of the reduced titration of O3 by constant despite the fact that they may decrease substantially in
nitrogen monoxide (NO). the future (Amann et al., 2015). We did this to be able to assess the
To address this situation, policy makers consider a bundle of impact of traffic NOx and NO2 fraction alone. Below we explain the
measures, including the introduction of 1) a complementary on- scenario assumptions in detail.
road test procedure for the type-approval of light-duty vehicles
and 2) dedicated NO2 emission limits, next to the already existing 2.1.1. Distance-specific emissions of Euro 6 passenger cars
Euro 6 NOx limits. The necessity of a complementary test procedure A big discrepancy has been observed between the NOx emis-
is well established (Franco et al., 2014; Weiss et al., 2013, 2012, sions of Euro 6 Diesel cars measured on the road and those
2011). The effect of plausible NOx emission factors for Diesel Euro measured during type approval in the laboratory. By contrast, for
6 was studied by Kiesewetter et al. (2014). They looked at their gasoline passenger cars (Chen and Borken-Kleefeld, 2014; Weiss
effect on the annual average NO2 concentration. However, it is still et al., 2011) as well as for heavy-duty vehicles (Vermeulen et al.,
unclear whether the introduction of a NO2 emission limit for light- 2012) in general, the discrepancy is negligible. We base our sce-
duty vehicles is an effective and necessary measure to decrease narios on emission measurements performed by JRC (2013) with
traffic-related NO2 emissions. Portable Emissions Measurement Systems (PEMS) on five Euro 6
Here, we address this question by assessing the impact on air Diesel cars over various test routes. The results are summarized in
quality of a dedicated NO2 emission limit for diesel cars, in addition Fig 1. The small dots represent the distance-specific NOx emissions
to the already existing NOx limit. To this end, we model for various (x-axis) and NO2 fraction (y-axis) per trip. Euro 6 Diesel cars with
plausible emission scenarios the urban NO2 concentrations in a low distance-specific NOx emissions tend to show a high NO2
case study for Antwerp (Belgium). We account for both, the large- fraction and vice versa. This is as a consequence of the NOx after-
scale transport of pollution at European and regional scale as well treatment technology. Indeed, cars equipped with selective
as the dispersion of pollution at city scale. While a coarse spatial
resolution is sufficient to capture background pollution levels, this
is not true at the city scale and even more so at the street level
where only a very high spatial resolution can capture local pollution
phenomena. A drawback of a higher spatial resolution is obviously
the high computational and data demand, which prevents a
simultaneous modelling of local NO2 pollution for many cities. We
therefore present here our modelling approach and its application
to the city of Antwerp, Belgium.
The paper is structured as follows: Section 2 describes the
methods in three steps, i.e., 1) the definition of emission scenarios,
2) modelling the European background pollution at a coarse reso-
lution and 3) modelling city scale pollution at a high resolution. The
results of these simulations are presented in Section 3. The paper
finishes with a discussion of results and conclusions for policy
makers in Section 4.

2. Methods

Modelling NO2 pollution faces two challenges. First, pollution Fig. 1. : Trip average NOx emissions (g/km) and NO2 fractions for PEMS measurements
of different Euro 6 diesel passenger cars (small dots) and the assumptions for possible
modelling has to account for a large spectrum of likely emission future Euro 6 Diesel fleet average emission factors (big dots). The Euro 6 emission limit
scenarios which will eventually materialize depending on the ve- is 0.08 g NOx/km (Source: JRC, 2013; May et al., 2014; Vlachos et al., 2015; Weiss et al.,
hicle's emissions performance, the evolution of the vehicle fleet 2012).
220 B. Degraeuwe et al. / Atmospheric Environment 126 (2016) 218e224

catalytic reduction (SCR) tend to show low NOx emissions and a 2.1.5. Overview of the selected emission scenarios
high NO2 fraction, whereas cars using exhaust gas recirculation We consider eleven scenarios for the emission factors of light
(EGR) and injection timing tend to have higher NOx emissions and a and heavy duty vehicles. Six scenarios cover the range of distance
low NO2 fraction. The emissions of cars equipped with a NOx trap specific NOx emissions and NO2 fractions. Two scenarios are worst
are somewhere in between. Since the dominant NOx after- case with high NOx and NO2 fraction for light duty vehicles. One is a
treatment technology of the future is yet unknown, we try to best-case with a complete shift to gasoline for light duty. These nine
capture the future Euro 6 emissions with nine combinations of a scenarios are marked as big dots in Fig. 1. Two scenarios with
NOx emission factor and a NO2 fraction (big red dots in Fig. 1) (red in increased heavy duty emissions are added. These eleven emission
the web version). Six combinations cover the measurements on factor scenarios are combined with the vehicle kilometres of
Euro 6 Diesel cars (small brown, green, light blue, dark blue and TREMOVE for 2010 and 2030. This gives 22 scenarios. The as-
pink dots in Fig. 1) (In the web version). Two extra combinations sumptions of these scenarios are listed in Table 1. For these sce-
represent worst cases with NOx emissions of 0.55 g/km and NO2 narios the emissions were calculated for all European countries
fractions of 50% and 70%, respectively. One combination represents combining emission factors, fleet composition and vehicle kilo-
the best case with distance-specific NOx emissions equal to those of metres. Out of the 22 scenarios, we retain nine scenarios that cover
gasoline vehicles (0.031 g NOx/km) and a NO2 fraction of 2%. This the likely range of future traffic NOx emissions and NO2 fraction.
best-case scenario implies a full shift to gasoline passenger cars. In These nine scenarios and the baseline scenario have a number in
all scenarios, we keep the particle mass (PM) emissions unchanged Table 1. They will be used for the air quality calculations described
to allow isolating the effect of NOx on secondary PM. We thereby in the next section.
neglect, however, that PM emissions have been decreasing
following the introduction of diesel particulate filters. 2.2. Modelling urban background and street canyon concentration

2.1.2. Distance-specific NOx emissions of Euro VI heavy-duty We model the hourly concentration of NO2, PM and O3 by
vehicles considering three spatial scales:
Heavy-duty vehicles are responsible for roughly half of the NOx
emissions originating from road transport (TREMOVE database, 1 We start out by modelling Europe-wide air pollution with a
Breemersch et al., 2010). Since recent measurements show that resolution of 28  28 km. Concentration maps of the main
Euro VI heavy-duty vehicles generally comply with the Euro VI limit pollutants have been generated by TNO with the LOTOS-EUROS
(Vermeulen et al., 2012), we uniformly apply here an emission Chemical Transport Model (CTM; Schaap et al., 2008) for an
factor of 0.507 g NOx/km as stated in COPERT 4 (Ntziachristos and entire meteorological year. The meteorology of 2009 was chosen
Samaras, 2014; Ntziachristos et al., 2011). This is a big reduction because it is an average year in terms of temperature. The
compared to the average emission factor of heavy duty vehicles in emission inputs for the model are the baseline and the nine
2010 (5.6 g NOx/km for Belgium). However, Euro VI heavy duty scenarios described in the previous paragraph.
vehicles seem to comply, two scenarios are considered with an 2 For the Benelux region, we zoom into at finer spatial resolution
emission factor of 1.0 g NOx/km. of 7  7 km to better capture the local pollution and dispersion
phenomena. We perform the CTM simulations with the same
2.1.3. Fleet composition
Prognoses for the future fleet composition in Belgium and
Table 1
Europe are retrieved from TREMOVE (Breemersch et al., 2010).
NOx emission factors, NO2 fraction and year of vehicle kilometres (vkm) for light and
TREMOVE covers both passenger and freight transport in 31 Euro- heavy-duty vehicles used in the baseline and 22 scenarios. The nine scenarios
pean countries at time intervals of 5 years over the period between selected for CTM calculations are numbered.
1995 and 2030. We chose 2010 as the reference year for our
Light-duty Heavy-duty
modelling to match as closely as possible the reference year of the
TNO-MACC-II inventory, i.e. 2009 (Kuenen et al., 2014). The share of Scenario NOx [g/km] f-NO2 NOx [g/km] f-NO2 vkm year

Diesel passenger cars predicted for 2030 is used for the scenarios 1 (base) 0.62 (BE) 0.34 5.60 (BE) 0.13 2010
(e.g. in Belgium 92% of passenger car kilometres will be driven with e 0.35 0.35 0.50 0.1 2010
Diesel cars). One scenario with a complete shift to gasoline for 2 0.35 0.35 0.50 0.1 2030
0.35 0.35 1.00 0.1 2010
passenger cars is also considered. Our scenarios thus cover a wide e
0.35 0.35 1.00 0.1 2030
range of plausible fleet compositions. E.g. in Belgium currently the e
3 0.10 0.5 0.50 0.1 2010
share of diesel cars is decreasing as a result of the recently changed
0.10 0.5 0.50 0.1 2030
taxation (Mayeres and Proost, 2013). We further assume that the e
0.20 0.7 0.50 0.1 2010
whole car fleet will consist of Euro 6 vehicles by 2030. Although this e
0.20 0.7 0.50 0.1 2030
assumption may not hold for all European countries, we consider it e
4 0.20 0.7 1.00 0.1 2010
to be reasonable given the current and predicted car turn-over. 0.20 0.7 1.00 0.1 2030
TREMOVE indeed predicts that 95% of the fleet will comply with
e
e 0.20 0.2 0.50 0.1 2010
Euro 6/VI by 2030.
e 0.20 0.2 0.50 0.1 2030
0.03 0.02 0.50 0.1 2010
2.1.4. Vehicle kilometres driven
e
5 0.03 0.02 0.50 0.1 2030
Similar to the projections of the future fleet composition, we use 6 0.45 0.05 0.50 0.1 2010
the future vehicle kilometres driven of TREMOVE (Breemersch e 0.45 0.05 0.50 0.1 2030
et al., 2010) for 2030. TREMOVE provides vehicle kilometre pre- e 0.55 0.2 0.50 0.1 2010
dictions per vehicle type and road type for each country. For 7 0.55 0.2 0.50 0.1 2030
Belgium a growth is predicted between 2010 and 2030 of about 10% e 0.55 0.5 0.50 0.1 2010
and 20% for heavy-duty and light-duty vehicles, respectively. A 8 0.55 0.5 0.50 0.1 2030
second scenario with a preservation of the kilometres driven at the 9 0.55 0.7 0.50 0.1 2010
10 0.55 0.7 0.50 0.1 2030
2010 level is also included.
B. Degraeuwe et al. / Atmospheric Environment 126 (2016) 218e224 221

LOTOS-EUROS model. These simulations are used to provide the


background pollution levels for Antwerp.
3 In a final step, we apply the IFDM and the OSPM model. IFDM
(Lefebvre et al., 2011) is a bi-Gaussian dispersion model
combining the background concentration from LOTOS-EUROS
and the local traffic sources to calculate the concentration of
NO2 and O3 at a high resolution over a city. At this level the
resolution is variable between 5 and 25 m and depends on the
concentration gradient. OSPM (Berkowicz et al., 1997; Ketzel
et al., 2012) is a box model and calculates the concentrations
inside the street canyons combining the rooftop concentration
provided by IFDM with the traffic emissions and geometry of the
street canyon.

In the case of Antwerp, LOTOS-EUROS under predicts the annual


average NO2 concentrations of the baseline scenario by 20%. This
error might be due to under prediction of the emissions or inac-
curacies in the CTM or a combination of both. To obtain more ac-
curate predictions for the scenarios a correction is applied based on
a comparison between measured and modelled data for the base-
line scenario. We know that the LOTOS-EUROS results at 7  7 km
resolution are a good prediction for the urban background con-
centration. Hence, we fit a correlation between the daily average
modelled concentrations and the ones measured in two urban
background concentrations near Antwerp (Schoten and Hoboken).
This correlation is applied to the concentrations of the scenarios.
Fig. 2. Impact of the NO2 fraction on the annual NO2 concentrations in the Benelux
zoom area; concentration difference between Scenario 10 (0.55 g NOx/km, f-
3. Results NO2 ¼ 70%) and Scenario 7 (0.55 g NOx/km, f-NO2 ¼ 20%).

In this section we look at the impact of the scenarios on the


concentration of NO2, PM and O3. We will look both at the impact
on the background concentrations and at street canyon level. For
the first we select a 7  7 km cell that coincides with Antwerp and
look at the LOTOS-EUROS results. For the later we select one street
canyon, the Plantyn-Moretus Lei. This street is close to a mea-
surement station (Borgerhout) where the annual average NO2
concentration exceeds 40 mg/m3. The street is 50 m wide and
building height is 18 m. There are 2 lanes in each direction and the
orientation is east-west. The peak hour traffic is 870 vehicles per
hour per lane which is close to the maximum capacity of a lane
(around 1000 vehicles per hour per lane). It is a busy access road to
the city centre. To determine the effect of a change in NO2 fraction
at constant NOx emissions we will compare scenarios 7 and 10.
They have a NO2 fraction of 20 and 70%, respectively. To determine
the effect of a change in NOx emissions only we will compare
scenarios 3 and 8.

3.1. Impact on the urban background pollution of Antwerp

In general the regional NO2 levels decrease with decreasing NOx


emissions with respect to the baseline (see Fig. 4, left). Even for
scenarios with a small decrease in passenger car NOx (scenarios 7 to
10) there is a decrease of NO2 levels due to the decrease of heavy
duty emissions. Spatially, changes in NOx emissions and NO2 frac-
tion have different effects. Fig. 2 shows the difference in NO2 con-
centration between scenarios 7 and 10. The impact of the NO2 Fig. 3. Impact of NOx emission levels on annual NO2 concentrations in the Benelux
fractions in the total NOx emissions is restricted to the vicinity of zoom area; Scenario 8 (0.5 g NOx/km, f-NO2 ¼ 50%) and Scenario 3 (0.1 g NOx/km, f-
NO2 ¼ 50%). City locations are A: Anwerp, B: Brussels and P: Paris.
large NOx emission sources. These correspond to the biggest cities
within the study area: Paris, Brussels, Antwerp, Rotterdam,
Amsterdam, the Ruhr area. We interpret this observation as fol- an influence on the NO2 concentration.
lows: when enough ozone is available, NO emissions are instan- Comparing Scenarios 3 and 8 that both assume the same NO2
taneously converted into NO2. Hence, the NO2 fraction within the fractions but different NOx emission factors (i.e., 0.1 and 0.5 g NOx/
emissions has little impact on the NO2 concentration. On the con- km, respectively) suggests that the absolute level of distance-
trary, when NOx emissions are large, not enough ozone is available specific NOx emissions at a given fleet composition and vehicle
to convert all NO into NO2 and the NO2 fraction in the emissions has
222 B. Degraeuwe et al. / Atmospheric Environment 126 (2016) 218e224

Fig. 4. Annual average NO2 concentration in an urban background location (left) and in a street canyon (right) in Antwerp for different scenarios; numbers in the diagram refer to
the scenarios indicated in Table 1.The X-axis represent the percentage emission reduction with respect to the base case (point 1) whereas the Y-axis indicates the fraction of NO2
within the Diesel car NOx emissions.

activity impacts substantially the annual average NO2 concentra- characterized by high distance-specific NOx emissions and high
tion. The observed impact is not limited to the vicinity of main cities NO2 fractions (e.g., Scenario 10: NOx ¼ 0.55 g NOx/km, f-NO2 ¼ 70%)
but can be traced in the regional and continental-scale NO2 back- would even lead to a possible deterioration of NO2 concentrations
ground levels (Fig. 3). Of course the background level impact needs (i.e. more severe and frequent pollution episodes) despite an
to be refined at street level (see Section 3.2.), where it might even overall reduction of the NOx emissions. This worst case Scenario 10,
be amplified. in which Euro 6 Diesel cars would emit as much NOx as the Euro 5
The change in distance-specific NOx emissions has a small, but cars and in addition have a high NO2 fraction is, however, not based
not negligible, impact on ozone and particulate matter pollution. on actual measurements.
The increase in the annual average ozone concentration between
the baseline and the best-case scenario is around 5 mg/m3. The
ozone concentration in the Benelux is around 40 mg/m3. This in- 4. Discussion
crease is due to the reduced ozone titration by NO when NOx
emissions are reduced. In urban areas, the increase in ozone con- 4.1. Strengths and limitations
centrations is larger than in rural areas, proportional to the larger
emission reductions there. For the same reason the extreme values This article presents a NO2 air pollution model that accounts for
(93rd percentile of 8 h maximum) get a bit worse in cities. The both, the background concentration and the NOx emissions at
effect of NOx emission reductions on PM concentrations is very street canyon level. We demonstrate the functionality of this model
small. Between the baseline and the best case scenario there are in a case study for Antwerp, Belgium. We acknowledge that the
reductions of around 1 mg/m3. Hence, traffic NOx emissions have a modelling future NO2 air pollution is intrinsically uncertain as key
small impact on secondary PM. parameters such as the emissions behaviour of vehicles, fleet
composition and activity are unknown. By assuming a wide range
of plausible emission scenarios, including extremes, we try to
3.2. Impact at street level on yearly and hourly NO2 concentrations ensure coverage of the likely future NO2 pollution resulting from a
fleet composed of Euro 6 vehicles. Only NOx emissions of traffic
Fig. 4 shows the annual average NO2 concentration for the were varied despite the fact that the emissions of other sectors will
baseline and the nine scenarios in a background location (left) and decrease. This allows seeing the impact of traffic NOx alone.
the selected street canyon (right).The NO2 concentration is A main source of uncertainty may result from the under-
expressed in terms of the NOx emission reduction compared to the prediction of the annual average NO2 concentrations by 20% by
baseline (X-axis) and NO2 fraction (Y-axis). An interpolation among LOTOS-EUROS. We correct the under-prediction by applying a bias
these 10 points is then performed to construct isolines. For the correction to the baseline and the scenarios. While the cause of the
street canyon we find that isolines are almost vertical, indicating underestimation remains unknown, we expect it to result from
that the reduction on NO2 pollution largely stems from a reduction uncertainties in emissions, meteorology or an incomplete repre-
in the distance-specific NOx emissions rather than the change of the sentation of chemical processes in the LOTOS-EUROS model. If this
NO2 fraction in the NOx emissions (see Fig. 4). The yearly averaged underestimation is mostly arising from underestimated traffic
NO2 pollution in a street canyon in Antwerp is therefore not emissions, the correction would then lead to an underestimation of
impacted by changes in the NO2 emitted fraction. If we consider the impact of the scenarios. The relative importance of traffic
that also other sectors will contribute to the reduction of NOx emissions would be too low. If non-traffic emissions are under-
emissions the impact of the NO2 fraction will be even smaller. estimated, the correction would exaggerate the impact of traffic
Fig. 5 shows the same approach applied to the 99.79th measures. In the case of a lack of accuracy in modelling atmo-
percentile of the NO2 concentrations, corresponding to the 19th spheric processes, e.g., assuming too much vertical dispersion
highest hourly concentration within a year. This value should not leading to lower street-level NO2 concentrations, the correction of
exceed 200 mg/m3. For the same street canyon in Antwerp, we note the modelled data would scale the effects of the scenarios to their
that the iso-percentile lines for the 99.79th percentile of the NO2 correct value. The reality is a combination of these effects and the
concentration are more horizontal than for the annual NO2 average, importance of different errors changes over the domain.
indicating a larger impact of the NO2 fraction. Some scenarios The results presented here for Antwerp cannot be simply
B. Degraeuwe et al. / Atmospheric Environment 126 (2016) 218e224 223

Fig. 5. 99.79th percentile of NO2 in an urban background location (left) and a street canyon (right) in Antwerp for different scenarios; numbers in the diagram refer to the scenarios
indicated in Table 1.The X-axis represent the percentage emission reduction with respect to the base case (point 1) whereas the Y-axis indicates the fraction of NO2 within the Diesel
car NOx emissions.

extrapolated to other cities because the conditions (e.g. the back-


ground concentrations of ozone and NO2, the vehicle fleet, weather NO þ O3 4NO2 þ O2
…) are different. This will be addressed in a next publication in Hence the NO2 fraction in the NOx emissions does affect the NO2
which the same methodology is applied to several European cities. concentrations in the canyon. However, with increasing ambient
NOx concentrations, e.g., due to higher NOx emissions, there is not
enough ozone present any more to convert all NO into NO2. In this
4.2. Interpretation of results case, higher NO2 fractions in the NOx emissions cause higher NO2
concentrations in the street canyon. For this reason the NO2 con-
In this section we explain why episodes of high NO2 concen- centration distribution of scenario 10 has a heavier tail which
trations are more sensitive to the NO2 fractions than the annual translates in a higher 99.79th percentile.
average NO2 concentrations are. For this purpose, we look at sce-
narios 7, 8, and 10 that keep the NOx emissions constant but assume
variable NO2 fractions of 20%, 50% and 70%, respectively. Fig. 6 5. Conclusions
shows the probability density function of the NOx and NO2 con-
centration for these scenarios (solid lines) and the average ozone We have developed a NO2 air pollution model that was applied
concentration at each level of NO2 emissions (dashed lines). The to the city of Antwerp, Belgium. Based on our findings, we draw the
distribution of NOx concentrations is almost identical for the three following conclusions:
scenarios because the NOx emissions are the same. However, the
distribution of NO2 concentrations differs between the scenarios  The absolute level of NOx emissions has a larger effect on NO2
following differences in the fractions of NO and NO2. At low pollution than the NO2 fraction in the NOx emissions. Reducing
ambient NOx concentrations, there is enough ozone to convert all overall NOx emissions may thus be more effectively curb urban
NO emissions into NO2 by means of the equilibrium reaction: NO2 pollution than the introduction of a dedicated NO2 emis-
sions limit for diesel cars.
 Compliance of diesel cars with the Euro 6 NOx emission limit
0.03 80 under real-driving conditions would result in important bene-
pdf NO2 scenario 7
fits for urban air quality. The introduction on a complementary
pdf NO2 scenario 8 70
0.025 Real-Driving Emissions on-road test procedure for the type-
pdf NO2 scenario10
approval of light-duty vehicles can thus be an effective mea-
pdf NOx scenario7 60
sure for decreasing both on-road NOx emissions of diesel cars
ConcentraƟon (ug/m3)

0.02 pdf NOx scenario 8


Probability dnesity

50 and urban NO2 pollution


pdf NOx scenario 10
 The NO2 fraction in the NOx exhaust only affects NO2 air pollu-
[O3] scenario 7
0.015 40 tion close to the emission sources and therefor impacts the
[O3] scenario 8
exceedance of the hourly limit value of 200 mg/m3. However, if
[O3] scenario10 30 Euro 6 diesel cars (i) do not comply on the road with the NOx
0.01
limits and (ii) emit high NO2 fractions, this can become a serious
20 issue.
0.005  If Euro 6 cars don't comply under real driving conditions a policy
10
option to solve this problem would be a progressive shift to
gasoline passenger cars in city centres. This can be done with e.g.
0 0
0 25 50 75 100 125 150 taxation or an environmental zone excluding diesel cars.
ConcentraƟon (ug/m3)  Reduced NOx emissions will cause a small increase of the annual
average ozone concentrations. The effect on the 93rd percentile
Fig. 6. Probability density function (pdf) of NOx concentrations (grey solid lines), NO2
concentrations (coloured solid lines) and the average ozone concentration at each level
of the 8 h maximum is indeed a trend to lower values, excepted
of NO2 concentration (coloured dashed lines) for three scenarios with identical NOx in big cities. The effect of NOx emission reductions on secondary
emissions and variable NO2 fractions of 20%, 50% and 70%, respectively. PM is negligible.
224 B. Degraeuwe et al. / Atmospheric Environment 126 (2016) 218e224

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