Trends in national emissions
Significant reductions were observed for the emission of all primary pollutants, i.e. − 4.7% year− 1 for SOx, − 2.7% year− 1 for NOx, − 2.6% year− 1 for NMVOCs, − 0.6% year− 1 for NH3, − 2.9% year− 1 for CO and − 1.8% year− 1 and − 1.7% year− 1 for PM2.5 and PM10, respectively, over the time period 2000–2017 in the EU-28 (Table 2). The SOx emissions decreased in all EU-28 countries, from − 2.9% year− 1 (Germany) to − 6.0% year− 1 (Slovenia). For NOx, the highest decrease was observed in the United Kingdom (− 3.4% year− 1), while the lowest reduction was found in Lithuania (− 0.6% year− 1) and Poland (− 0.7% year− 1). For NMVOCs, the decrease ranged from − 0.6% year− 1 (Poland) to − 4.0% year− 1 (France). A slight decrease was also observed in Ireland (− 0.7% year− 1), Netherlands and Romania (− 0.9% year− 1). The sector “agriculture” contributes to 92% of NH3 emissions (EEA, 2019), and their emissions usually exhibited small reductions, with an increase in Austria, Estonia, Germany, Latvia, and Lithuania, ranging from 0.1 to 1.0% year− 1. The domestic heating represents 48% of CO emissions (EEA, 2019). Also, the CO emissions usually decreased, except in Romania (− 0.5% year− 1) and Malta (+ 0.6% year− 1). A decrease of PM2.5 emissions was observed in all EU-28 countries, except Bulgaria (+ 0.5% year− 1), Hungary (+ 0.9% year− 1) and Romania (+ 0.3% year− 1), associating with a slighter reduction in PM10 emissions (− 0.2% year− 1 in Bulgaria; − 0.1% year− 1 in Hungary). An increase of PM10 emissions was noted in Lithuania (+ 0.8% year− 1) and Romania (+ 0.1% year− 1). The highest decrease for PM2.5 (− 4.2% year− 1) and PM10 (4.0% year− 1) emissions occurred in Malta (Table 2).
Table 2
Annual trends of national emissions (% year− 1) in the 28 European Union countries (EU-28) for sulfur oxides (SOx), nitrogen oxides (NOx), non-methane volatile organic compounds (NMVOCs), ammonia (NH3), carbon monoxide (CO), particulate matter with an aerodynamic diameter lower than 2.5 µm and 10 µm (PM2.5 and PM10) over the time period 2000–2017. All trends are significant at p < 0.05 (Mann-Kendall). The increasing trends are in bold.
EU-28 Countries
|
SOx
|
NOx
|
NMVOCs
|
NH3
|
CO
|
PM2.5
|
PM10
|
Austria
|
− 3.83
|
− 2.11
|
− 2.41
|
+ 0.51
|
− 1.57
|
− 2.31
|
− 1.74
|
Belgium
|
− 4.98
|
− 3.12
|
− 3.20
|
− 1.07
|
− 3.85
|
− 2.53
|
− 2.45
|
Bulgaria
|
− 5.35
|
− 2.41
|
− 1.47
|
− 0.54
|
− 1.59
|
+ 0.47
|
− 0.19
|
Croatia
|
− 4.84
|
− 2.63
|
− 2.25
|
− 1.34
|
− 2.85
|
− 1.71
|
− 1.72
|
Cyprus
|
− 4.58
|
− 1.77
|
− 2.23
|
− 1.22
|
− 3.65
|
− 3.03
|
− 3.39
|
Czech Republic
|
− 3.15
|
− 2.60
|
− 1.60
|
− 0.96
|
− 1.27
|
− 0.99
|
− 1.16
|
Denmark
|
− 4.45
|
− 3.35
|
− 2.30
|
− 1.48
|
− 3.00
|
− 1.49
|
− 1.13
|
Estonia
|
− 3.92
|
− 1.88
|
− 2.48
|
+ 0.24
|
− 2.07
|
− 3.01
|
− 3.41
|
Finland
|
− 3.77
|
− 2.92
|
− 3.23
|
− 0.64
|
− 2.51
|
− 2.17
|
− 1.88
|
France
|
− 4.85
|
− 3.12
|
− 3.96
|
− 0.30
|
− 3.75
|
− 3.37
|
− 2.87
|
Germany
|
− 2.93
|
− 1.86
|
− 2.07
|
+ 0.13
|
− 2.29
|
− 2.48
|
− 1.67
|
Greece
|
− 5.59
|
− 2.79
|
− 3.36
|
− 1.11
|
− 3.46
|
− 2.94
|
− 3.25
|
Hungary
|
− 4.59
|
− 2.35
|
− 2.04
|
− 0.44
|
− 3.00
|
+ 0.93
|
− 0.10
|
Ireland
|
− 5.97
|
− 2.40
|
− 0.75
|
− 0.26
|
− 3.84
|
− 2.33
|
− 1.94
|
Italy
|
− 5.63
|
− 3.40
|
− 2.63
|
− 1.12
|
− 3.03
|
− 1.07
|
− 1.40
|
Latvia
|
− 4.94
|
− 1.63
|
− 1.73
|
+ 0.61
|
− 3.49
|
− 2.16
|
− 1.36
|
Lithuania
|
− 3.60
|
− 0.61
|
− 1.35
|
+ 1.01
|
− 1.39
|
− 1.49
|
+ 0.79
|
Luxembourg
|
− 4.18
|
− 3.25
|
− 2.02
|
− 0.84
|
− 2.80
|
− 3.00
|
− 2.42
|
Malta
|
− 5.66
|
− 2.37
|
− 2.06
|
− 1.86
|
+ 0.60
|
− 4.20
|
− 3.95
|
Netherlands
|
− 4.14
|
− 2.72
|
− 0.88
|
− 1.76
|
− 1.78
|
− 3.53
|
− 2.65
|
Poland
|
− 3.62
|
− 0.69
|
− 0.62
|
− 0.81
|
− 1.67
|
− 0.72
|
− 0.79
|
Portugal
|
− 5.73
|
− 3.06
|
− 2.46
|
− 1.34
|
− 3.50
|
− 1.96
|
− 2.56
|
Romania
|
− 4.94
|
− 1.77
|
− 0.95
|
− 0.67
|
− 0.55
|
+ 0.28
|
+ 0.15
|
Slovakia
|
− 4.46
|
− 2.31
|
− 2.69
|
− 0.98
|
− 2.36
|
− 3.22
|
− 3.06
|
Slovenia
|
− 6.03
|
− 2.50
|
− 2.70
|
− 0.89
|
− 2.79
|
− 0.52
|
− 1.22
|
Spain
|
− 5.44
|
− 2.99
|
− 2.62
|
− 0.82
|
− 2.08
|
− 1.30
|
− 1.63
|
Sweden
|
− 3.71
|
− 2.32
|
− 2.15
|
− 0.66
|
− 2.77
|
− 2.54
|
− 1.64
|
United Kingdom
|
− 5.26
|
− 3.42
|
− 3.28
|
− 0.52
|
− 4.21
|
− 1.40
|
− 1.70
|
EU-28
|
− 4.74
|
− 2.67
|
− 2.63
|
− 0.65
|
− 2.89
|
− 1.76
|
− 1.70
|
The emissions of all primary air pollutants contributing to ambient levels of PM, O3, and NO2 decreased between 2000 and 2017 in the EU-28 (observed reductions SOx: − 80%; NOx: − 46%; NMVOCs: − 44%; NH3: − 10%; CO: − 49%; PM2.5: − 31%; PM10: − 29%), in line with stringent EC Directives, e.g. Air Quality Framework Directive (1996/62/EC), Large Combustion Plant Directive (2001/80/EC), and National Emission Ceilings Directives (2001/81/EC; 2016/2284/EC), setting emission reduction commitments by 2030 compared to 2005 (expected reductions SO2: − 79%; NOx: − 63%; NMVOCs: − 40%; NH3: − 19%; PM2.5: − 49%). The emission reductions were mainly achieved as a result of the progress in e.g. the use of flue-gas abatement techniques, energy production and distribution, storage and distribution of solvents (Vestreng et al., 2008; EEA, 2014), and vehicle technologies related to legislative “Euro” standards (Sicard et al., 2020a). In EU-28 countries, the “transport” sector is the largest contributor (road transport: 39%) to total NOx emissions (EEA, 2019). The Euro-2 to Euro-6 standards for light-duty vehicles were enforced from 1997 to 2015. For diesel cars, the average NOx + VOCs limit ranged from 0.70 g/km (Euro-2) to 0.17 g/km (Euro-6), from 1.00 g/km to 0.50 g/km for CO and from 0.08 g/km to 0.0045 g/km for PM. For gasoline cars, the average NOx + VOCs limit ranged from 0.500 g/km (Euro-2) and 0.128 g/km (Euro-6) and from 2.2 g/km to 1.0 g/km for CO. In 2017, the successive Euro standards have lowered the PM (94%), CO (50%) and NOx + VOCs (76%) emission intensity in the EU compared to early 2000s.
Trends in urban population exposure
Despite the reduction of PM10 emissions over the time period 2000–2017, the minimum and maximum percentage of the EU-28 urban population exposed to PM10 concentrations above the EU daily limit value ranged from 18–44% in 2000–2010 to 13–30% in 2010–2017 (Fig. 1), with the highest extent of exposure observed in 2003 (44%). Between 2000 and 2017, the EU daily limit value for PM10 was widely exceeded in Europe, mostly in Eastern Europe (Guerreiro et al., 2014), e.g. Bulgaria, Cyprus, Czech Republic, Hungary, Poland, Slovakia, Greece, and Italy. In 2005, Estonia, Finland, Ireland, Luxembourg, and the United Kingdom did not record exceedances of this limit value. In 2017, the limit value was exceeded in Bulgaria, Croatia, Czech Republic, Poland and Italy (EEA, 2011–2019). Before 2006, more than 80% of the EU-28 population was exposed to levels exceeding the WHO AQG value for the protection of human health, decreasing to 42–52% in 2014–2017 (EEA, 2007; 2011–2019). From 2000 to 2017, the annual averaged PM10 concentrations decreased by 0.65 µg m− 3 year− 1 on average at urban stations in the EU-28 (EEA, 2019). In 20102017, 6–14% of the EU28 population was exposed to PM2.5 levels above the EU annual target value, while the range was 16–52% in 2000–2010. The target value was exceeded mostly in Bulgaria, Czech Republic, Poland, and Slovakia between 2000 and 2013. The population exposure to PM2.5 levels above the WHO AQG ranged from more than 90% before 2006 to 74–80% in 2014–2017. Between 2000 and 2017, the annual averaged concentrations of PM2.5 decreased by on average 0.42 µg m− 3 per year at urban background stations in the EU-28 (EEA, 2019).
The percentage of the EU-28 population exposed to NO2 concentrations above the EU annual limit value and the WHO AQG value decreased from 14–31% before 2006, with the maximum recorded in 2003, to less than 10% since 2012 (Fig. 1). The annual limit value was mostly exceeded in Italy, Greece, and in the United Kingdom in 2000–2005, and in Germany in 2010, 2011, 2012, 2014, and 2016 (EEA, 2011–2019). The NO2 annual mean concentrations decreased by on average 0.39 µg m− 3 year− 1 over the time period 2002–2011 by joining 708 urban stations in the EU-28 (Guerreiro et al., 2014). The percentage of the EU-28 urban population exposed to SO2 levels above the EU daily limit value ranged from 1–2% in 2000–2005 to lower than 0.5% since 2007 (data not shown). The percentage of the EU-28 urban population exposed to SO2 levels exceeding the WHO AQG decreased from more than 70% before 2006 to less than 40% since 2013 (EEA, 2011–2019). Less than 2% of the EU-28 urban population was exposed to maximum CO daily 8-hour mean concentrations above the EU and the WHO AQG limit values (data not shown). Only a few traffic stations in Bulgaria, Poland and Romania have reported exceedances of the SO2 and CO EU limit values over the time period 2000–2017 (Guerreiro et al., 2014; EEA, 2019).
The EU-28 urban population exposed to O3 levels above the EU target value for human health protection ranged from 7–62% since 2000 (Fig. 1), with the highest extent of exposure observed in 2003. Higher background O3 levels (annual mean > 30 ppb) were observed in Southern Europe (Sicard et al., 2013). The EU target value was mostly exceeded in Southern Europe, such as Croatia, Cyprus, France, Greece, Italy, Slovenia, Spain, Malta, Portugal, but also in Austria, Hungary, Luxembourg, and Poland recently. More than 95% of the total EU-28 urban population was exposed to O3 levels exceeding the WHO AQG since 2000 (data not shown). In the EU, the annual mean of daily O3 concentrations increased by on average 0.05 ppb year-1 at 260 urban stations over the time period 2000–2014 (Table 3). The annual O3 mean concentrations increased by on average 0.34 ppb year-1 at more than 80% of urban stations between 2005 and 2014, except in the United Kingdom where a decrease (− 0.18 ppb year-1) was observed at 65% of urban stations (Sicard et al., 2020a). In Germany, an increase of 0.18 ppb year-1 was reported at 79 urban stations over the time period 2005–2018 (Sicard et al., 2020a). A significant increase in the annual O3 mean (on average, + 0.29 ppb year-1) was found at urban stations in Southern Europe between 2000 and 2010 (Sicard et al., 2013; Kulkarni et al. 2015). In France, an increase of + 0.14 ppb year-1 at 76% of urban stations was reported between 1999 and 2012 (Sicard et al., 2016b). Despite an increasing fleet size, the reduction in NOx and VOCs emissions since the early 1990s, due to the vehicle emission regulations, allowed a reduction in O3 peaks and high percentiles (EEA, 2016; Sicard et al., 2018; de Foy et al., 2020). At EU-28 urban stations, a reduction in O3 annual mean of the maximum daily 8-hour mean values (− 0.75 ppb year-1) was found over the time period 2000–2014 (EEA, 2016). In Southern Europe, significant reductions in 98th percentile (− 0.51 ppb year-1) and hourly maximum (− 1.81 ppb year-1) values were found at urban stations between 2000 and 2010 (Sicard et al., 2013). Simpson et al. (2014) found an increase of O3 concentrations of 0.1–0.4 ppb year-1 up to the 95th O3 percentile over the time period 1990–2009. The surface O3 levels are rising in cities in Europe from 2000 (e.g. Simon et al., 2015; Sicard et al., 2016b; Chang et al., 2017; Lefohn et al., 2018; Yan et al., 2019; Sicard et al., 2020a), mainly due to a reduced titration of O3 by NO (Huszar et al., 2015; Sicard et al., 2020a).
Table 3
National-averaged trends magnitude (ppb per year ± standard deviation) of annual ozone mean concentrations at urban and rural background monitoring stations worldwide. The studies were selected for more than 10-year time-series of ozone data, for stations with at least 75% of validated hourly data over the time period, and with a significant trend, i.e. with a p-value < 0.05. Number of stations (n, with n ≥ 2).
Countries
|
Time period
|
References
|
n
|
Urban stations
|
Europe
|
1995–2012
|
Yan et al., 2019
|
289
|
+ 0.27 ± 0.10
|
Austria
|
1995–2014
|
Sicard et al., 2018
|
6
|
+ 0.17 ± 0.12
|
Belgium
|
2
|
+ 0.08 ± 0.15
|
Germany
|
60
|
+ 0.19 ± 0.06
|
Greece
|
3
|
+ 0.18 ± 0.50
|
Netherlands
|
5
|
+ 0.19 ± 0.11
|
Slovenia
|
2
|
+ 0.14 ± 0.08
|
Spain
|
12
|
+ 0.36 ± 0.24
|
Sweden
|
3
|
+ 0.37 ± 0.10
|
Switzerland
|
11
|
+ 0.28 ± 0.11
|
United Kingdom
|
12
|
+ 0.21 ± 0.12
|
France
|
1999–2012
|
Sicard et al., 2016b
|
179
|
+ 0.14 ± 0.19
|
France
|
2000–2010
|
Kulkarni et al., 2015
Sicard et al., 2013
|
29
|
+ 0.10 ± 0.30
|
Greece
|
3
|
+ 0.41 ± 0.15
|
Italy
|
20
|
+ 0.04 ± 0.30
|
Portugal
|
8
|
+ 0.40 ± 0.33
|
Spain
|
14
|
+ 0.48 ± 0.53
|
Europe
|
2000–2014
|
Chang et al., 2017
|
260
|
+ 0.05 ± 0.13
|
Belgium
|
2005–2014
|
Sicard et al., 2020a
|
2
|
+ 0.42 ± 0.05
|
France
|
136
|
+ 0.31 ± 0.42
|
Germany
|
79
|
+ 0.09 ± 0.17
|
Greece
|
4
|
+ 0.85 ± 0.43
|
Italy
|
50
|
+ 0.43 ± 0.84
|
Portugal
|
2
|
+ 0.48 ± 0.12
|
Spain
|
77
|
+ 0.54 ± 0.73
|
United Kingdom
|
29
|
− 0.18 ± 0.34
|
Germany
|
2005–2018
|
Sicard et al., 2020a
|
79
|
+ 0.18 ± 0.15
|
Trends in national mortality from exposure to ambient PM2.5 and O3 levels
At present compared to other air pollutants, PM2.5 poses the most serious health risk in the EU-28 cities, associated with premature deaths and increased morbidity, followed by ground-level O3 (Pascal et al., 2013; Cohen et al., 2017). In the EU-28, the number of deaths due to ambient PM2.5 levels decreased by on average 4.85 per 1,000,000 inhabitants annually between 2000 and 2017 (Table 4). The highest annual decreases were observed in the United Kingdom and Estonia (− 11.74 and − 10.46 deaths per 106 inhabitants, respectively) while a slighter reduction was found in Portugal (− 0.50 deaths per 106 inhabitants). In Greece and Lithuania, an increase of annual mortality due to ambient PM2.5 levels was observed (+ 1.22 and + 1.72 deaths per 106 inhabitants, respectively). In line with rising O3 levels in cities (Sicard et al., 2018, 2020a), the annual O3-related number of premature deaths increased in the EU-28 (on average + 0.55 deaths per 106 inhabitants). The highest annual decrease of mortality was observed in Greece (+ 2.41 deaths per 106 inhabitants), Hungary (+ 2.05 deaths per 106 inhabitants) and Czech Republic (+ 1.40 deaths per 106 inhabitants), while a non-significant increase was found in Spain (+ 0.03 deaths per 106 inhabitants). Between 2000 and 2017, the annual number of deaths attributed to O3 declined mostly in Northern Europe (e.g. Belgium: − 0.24; Ireland: − 0.30; Lithuania: − 0.23 deaths per 106 inhabitants per year) where lower background O3 levels (annual mean < 20 ppb) were observed (Araminienė et al., 2019; Sicard et al., 2020a).
Table 4
Annual trends of mortality (number of deaths per 1,000,000 inhabitants per year) due to ambient particulate matter with an aerodynamic diameter lower than 2.5 µm (PM2.5) and tropospheric ozone (O3) over the time period 2000–2017 in the 28 European Union countries (EU-28) with associated significance level p (Mann-Kendall *** p < 0.001; ** p < 0.01; * p < 0.05; + p < 0.1 and p > 0.1).
EU-28 Countries
|
PM2.5
|
p level
|
O3
|
p level
|
Austria
|
− 6.00
|
***
|
0.18
|
**
|
Belgium
|
− 8.80
|
***
|
− 0.24
|
*
|
Bulgaria
|
− 2.73
|
*
|
0.56
|
***
|
Croatia
|
− 2.27
|
+
|
1.18
|
***
|
Cyprus
|
− 9.07
|
***
|
0.14
|
|
Czech Republic
|
− 4.56
|
***
|
1.40
|
***
|
Denmark
|
− 9.42
|
***
|
0.18
|
|
Estonia
|
− 10.46
|
***
|
0.20
|
***
|
Finland
|
− 6.55
|
***
|
0.22
|
***
|
France
|
− 3.55
|
***
|
0.09
|
|
Germany
|
− 3.11
|
***
|
1.19
|
***
|
Greece
|
1.22
|
*
|
2.41
|
***
|
Hungary
|
− 1.39
|
|
2.05
|
***
|
Ireland
|
− 9.05
|
***
|
− 0.30
|
+
|
Italy
|
− 2.28
|
**
|
0.75
|
***
|
Latvia
|
− 5.40
|
*
|
0.20
|
***
|
Lithuania
|
1.72
|
+
|
− 0.23
|
***
|
Luxembourg
|
− 8.05
|
***
|
− 0.17
|
*
|
Malta
|
− 0.38
|
|
0.32
|
***
|
Netherlands
|
− 8.76
|
***
|
0.24
|
*
|
Poland
|
− 9.56
|
***
|
0.45
|
***
|
Portugal
|
− 0.50
|
|
0.37
|
***
|
Romania
|
− 4.04
|
***
|
0.37
|
***
|
Slovakia
|
− 7.56
|
***
|
0.42
|
***
|
Slovenia
|
− 5.74
|
***
|
− 0.67
|
***
|
Spain
|
− 5.04
|
***
|
0.03
|
|
Sweden
|
− 8.44
|
***
|
0.32
|
***
|
United Kingdom
|
− 11.74
|
***
|
0.08
|
|
EU-28
|
− 4.85
|
***
|
0.55
|
***
|