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CONTRIBUTION OF TRAFFIC TO ANNUAL AIR POLLUTION WITH NITROGEN DIOXIDE OVER STARA ZAGORA, BULGARIA Nikolay P. Takuchev Trakia University, Stara Zagora 6000, Bulgaria Abstract Introduction. Stara Zagora (42,4283 N; 25,6559 E, population 150000) is a densely populated town with developed industry and heavy traffic, subjected to the above-threshold pollution by nitrogen dioxide. Aim. To estimate the contribution of the city traffic to the annual urban air pollution with NOx. Material and methods. The number of vehicles registered in Stara Zagora municipality in 2012 and the fuel (gasoline, auto gas, natural gas) sold in 2012 in Stara Zagora area, were received through requests for access to public information. Results and discussion. The appraisal for the city traffic emissions of nitrogen oxides into the urban air for 2012 is total 201 t/y. The traffic emits about 2/3 from all annual city emissions of NOx in Stara Zagora. Key words:urban air pollution, NOx, Traffic, Stara Zagora 1. INTRODUCTION Stara Zagora is a densely populated town with developed industry, heavy traffic and without centralized heating. The town is located in the foothills of the southern slopes of the Sredna Gora Mountain. The combination between the compact city layout with heavy traffic added to the industrial sources of pollution and the thousands of closely spaced polluting sources households, determines the local environmental problems associated with urban air pollution. The environmental problems with the urban air pollution of the city have long history. Several events of above-threshold pollution of nitrogen dioxide occur over recent years, mainly in November. The aim of the paper is to estimate the contribution of city traffic to the annual urban NOx emission (harmful NO 2 + harmless NO, which converts to NO 2 in the presence of volatile organic compounds in the ambient air). 2. MATERIAL AND METHODS In a stationary situation the flow leaving the city motor vehicles equals the flow entering the city vehicles, i.e. in average the annual number of vehicles in the city is constant. It slowly changes over the years. Vehicles consume relatively constant amount of fuel and consequently emit relatively constant amount of nitrogen oxides in the air per year. In a stationary situation, fuel burned in the city has purchased from fuel stations in the city, i.e. if the fuel sold in the city is known the air pollution with nitrogen oxides can be evaluated. From April 2012 the National Revenue Agency (NRA) controls online sales of fuels, in particular those in the territory of Stara Zagora. By request for access to public information the monthly sales from the fuel stations in the territory of Stara Zagora for 2012 by fuel type, were received from the NRA. Additional data for monthly methane consumption from methane stations in the city for the entire 2012 was received from the supplier OVERGAS AD. 3. RESULTS AND DISCUSSION The volume of the sold fuels is given in table 1. Since the calculation of the NOx emissions due to the combustion process in the vehicle engines requires the fuel to be expressed in mass units, in the table are given also the masses of the fuels, calculated by their densities. The density of gasoline (730 kg/m 3 ) was taken at 15 C. Diesel density (835 kg/m 3 ) was taken at 15 C. The density of autogas is calculated as the average of the densities of propane (510 kg/m 3 ), butane (580 kg/m 3 ) and isobutane (557,3 kg/m 3 ) at 15 C and atmospheric pressure. (Source: Characteristic properties of the gas mixture LPG (LPG), 2013.) Density (416 kg/m 3 ) of the compressed methane (natural gas) is taken at 0 C. (Source: Methane, 2013. Also: Greenhouse Gas Conversion Factors, 2013). 606

Type of energy source Sales for April-December 2012 Annual sales for 2012 Gasoline, l (liter) 9346672 12459114 Diesel, l 19888184 26510949 Autogas (LPG), l 10663352 14214248 Methane (CNG), l 6145266 8191640 Gasoline, kg 6823071 9095153 Diesel, kg 16606634 22136642 Autogas, kg 5854180 7803622 Methane, kg 2556431 3407722 Table 1. Sales of fuel stations of Stara Zagora from April to December 2012 and for the year as a whole (the sales for missing months are replaced by the average of the available data). The density of autogas is calculated as average of the densities of propane, butane and isobutane at 15 C and atmospheric pressure. Monthly data are shown graphically in figure 1. It can be seen that the distribution is more or less evenly throughout the year, i.e., is groundless to assert that the November gassing with nitrogen dioxide in 2012 were due to increased traffic, more so in November 2012 the sales of fuels were weakest in the year. Available data from the NRA show a weak trend of probably decreasing sales of fuel at the beginning of the year (the first three months). An additional argument in favor of such an assumption is the fact that at the beginning of the year sales of methane (the information is available for whole year) were slightly higher. Since the methane is the fuel used of part of public transport and taxis, increased methane sales indicate an increased flow of users of public transport in winter, i.e. reduced flow of personal vehicles and reduced sales of other types of fuel at the beginning of the year. I.e. the missing data on fuel purchased in the first three months of the year can be replaced with monthly averages calculated from the other months, without risk to underestimate the annual emissions of nitrogen oxides originating from traffic (right column of table 1). Sold fuels in the teritory of Stara Zagora, 2012 3000000 1000000 Volume, l, (gasoline, Diesel, autogas) 2500000 2000000 1500000 1000000 500000 0 gasoline, l autogas, l 900000 800000 700000 600000 500000 400000 300000 200000 100000 0 Jan 2012 Feb 2012 Mar 2012 Apr 2012 May 2012 Jun 2012 Jul 2012 Aug 2012 Sept 2012 Oct 2012 Nov 2012 Dec 2012 Diesel, l Methane, Nm3 Volume, Nm 3, methane Figure 1. Distribution of fuel stations sales during the year 2012 on the territory of Stara Zagora. In November 2012, when there were above-threshold nitrogen dioxide pollution events and accusations that the traffic is guilty for it, no oversold automotive fuels were observed, by contrast, there is a slight decline in sales. 607

Data for the vehicle fleet of Stara Zagora District received from the District Police Directorate, are shown in table 2. to 1.1.2012 First registration: Type of vehicle to 1990 24747 1416 2014 354 1509 between 1991 and 1995 31717 1773 1074 240 871 between 1996 and 2000 28352 1782 865 184 945 after 2000 12383 1878 901 191 1749 Total 97199 6849 4854 969 5074 Shares,% 85 6 4 1 4 Table 2. Vehicles registered in Stara Zagora district. In Stara Zagora municipality "Program of reducing levels of nitrogen dioxide and reaching the established norms in Stara Zagora for the period 2013-2015", are given the total number of vehicles, registered in the municipality in 2010 and shares of vehicles by type divided into three groups. The number of vehicles in the municipality of Stara Zagora was calculated on these data where the missing data from the municipality information on the distribution of light duty, heavy duty vehicles and busses is calculated according to their share as it is shown in table 2. The final data is shown in table 3. Number: 80914 at the end of 2010 Type of vehicle Shares,% 87 Total 10 3 Number 70395 4413 2942 736 2427 Table 3. Vehicles registered in Stara Zagora municipality. The approximate ratios of the number of vehicles registered in the municipality by type of fuel, are given in the same source: gasoline: diesel: auto gas = 50:30:20. It can be assumed that the heavy duty trucks and buses use 100% diesel. The motorcycles use gasoline. This gives the data in a table 4. Type of vehicle Shares,% Gasoline 50 50 100 Diesel 30 30 100 100 Auto gas 20 20 Number Gasoline 35198 2207 2427 Diesel 21119 1324 2942 736 Auto gas 14079 883 Table 4. Distribution of motor vehicles registered in the municipality of Stara Zagora by type and by fuel used. 608

The result of vehicles counting per day in a city street with heavy traffic (November 2010) is shown in table 5. Number: 11985 November 12, 2010 Type of vehicle Shares,% 89,9 7,6 2,0 0,3 0,2 Number 10773 910 236 39 27 Table 5. Distribution by type of the vehicles passed per day along the counting point in November 12, 2010. Shares of vehicles types in the municipality derived from the above mentioned three independent sources (table 3, table 4 and table 5), are close in value, which confirms the reliability of the data in table 4 used in the calculations below. Tier 1 method (recommended by European Environmental Agency (EEA), EMEP/EEA emission inventory guidebook 2013 1.A.3.b Road transport) was used to estimate the emissions of nitrogen oxides from the vehicles in Stara Zagora. The method is consistent with the legal and technical requirements for the vehicle fleet of Europe in 1995, which corresponds to the specificity of the vehicle fleet of Bulgaria at the time. As shown in table 1, in Stara Zagora prevail cars manufactured between 1991 and 1995. The number of more new cars gradually increases which reduces the emissions and the real input of the traffic to the air pollution of the city is probably smaller than the obtained by the above mentioned method. A typical fuel consumption in grams per kilometer by vehicle type and by fuel used, is shown in table 6. Fuel Consumption, g/km, by type of vehicle Gasoline 70 100 35 Diesel 60 80 240 240 Auto gas 57,5 Table 6. Fuel consumption per kilometer for vehicle type. (Source : EMEP / EEA emission inventory guidebook 2013 1.A.3.b Road transport, Tier 1 method, page 29, table 3-14). The fuel in kilograms, which all vehicles in the city would burn covering 1 km of city streets can be calculated by multiplication of relevant data from tables 4 and 6, divided by 1000. The result is given in table 7. Burned fuel in kg per 1 km mileage by type of vehicle Gasoline 2464 221 85 Diesel 1267 106 706 177 Auto gas 810 Table 7. Fuel burnt by all vehicles in the city of Stara Zagora, in kilograms per kilometer. If the distribution of vehicles on their annual mileage in city conditions is known, equivalent kilometers run in the city of vehicles of a given type can be calculated from fuel data burnt per kilometer of a given type vehicles (table 7), and data on fuel purchased from the fuel stations (table 1). 609

Data on the average mileage of the vehicles in urban conditions for the country (Bulgaria) by category, is presented in a report to the Metropolitan municipality on "Inventory of emissions of CO 2, released into the atmosphere as a result of energy consumption on the territory of Sofia Municipality", 2012, page 19, table 19. The data are given in table 8. The calculations below are based on the assumption that these data are representative for Stara Zagora as a proportion between the annual mileage of different types of vehicles. Average mileage in city conditions: 3393 km Average mileage in the city, km/y, per vehicle Total Gasoline 2693 3151 686 6530 Diesel 3895 4193 4410 4410 16908 Auto gas 2693 2693 Table 8. Average mileage of a vehicle in an urban environment in Bulgaria in 2011 (Source: "Inventory of emissions of CO 2, released into the atmosphere as a result of energy consumption on the territory of Sofia Municipality" prepared by the international consulting company in the field of ecology "Denkstatt" p.19, table 19) The absolute average annual mileage of a motor vehicle for Stara Zagora, probably differs from the values in table 8. It depends mostly on the size of the settlement on which depend the distances to work, shops, medical facilities, etc. All these distances are proportional to the size of the settlement and determine the absolute value of the average annual mileage of different types vehicles in the settlement the mileage is longer in larger settlements and vice versa. For each type of vehicle was calculated the relative average mileage in city conditions as a percentage of the mileage for a given type of vehicle compared to the cumulative absolute mileage of all types of vehicles using a particular fuel type. The result is given in table 9. Relative average annual mileage by type of vehicle Gasoline 0,412 0,483 0,105 Diesel 0,230 0,248 0,261 0,261 Auto gas 1,000 Table 9. Relative average mileage per a vehicle type by fuel type for urban conditions in Bulgaria. Unlike the average mileage in absolute terms, the relative average mileage of a vehicle (for a given fuel type) does not depend on the size of the settlement, if other conditions like economy, population density, distribution of jobs, etc being equal. Below this independence is used to evaluate the absolute value of the average annual mileage per type of vehicle for Stara Zagora. As far as the above mentioned conditions are not the same for all locations in the country, the independence of the relative average mileage of a vehicle for a particular fuel type on the size of the settlement is rather approximate. The total mass of fuel of a particular type sold by the fuel stations on the territory of Stara Zagora per year is known (table 1). The same mass is proportional on a function (polynomial) calculated as a sum of multiplications between the fuel of the same type burnt per year by all vehicles of a given type in the city of Stara Zagora (table 7) and the relative average mileage per a vehicle type by fuel type for urban conditions in Bulgaria (table 9). For the three above mentioned types of fuel three such functions were calculated. Each of the terms of each of the three functions has to be multiplied by the same unknown coefficient, to coincide with the annual sales of the corresponding type of fuel. Goal Seek function of MS Excel was used to obtain the coefficient for each of the functions. The results are given in table 10. 610

Fuel type Coefficient, y -1.km -1 Gasoline 8043 Diesel 40383 Auto gas 9634 Table 10. Values of the unknown coefficient in the above mentioned functions. The annual mileage of each type of vehicle and type of used fuel is obtained by multiplying the appropriate fuel type coefficient (table 10) to the relative average mileage per a vehicle type for urban conditions in Bulgaria, taken from table 9. The results are given in table 11. Average annual mileage, km, by type of vehicle Gasoline 3314 3885 845 Diesel 9288 10015 10540 10540 Auto gas 9634 Table 11. Average mileage per vehicle per year in the city of Stara Zagora. Part of the fuel purchased from the stations in Stara Zagora is spent out of town and does not contribute to pollution in the city. The part of the fuel burned in the city boundary can be assessed by comparing the average mileage in the city streets for Bulgaria (table 8) with the average mileage, regardless of the type of road for Bulgaria. The average annual mileage of vehicles in the country for all types of roads, is given in table 12. Type of Vehicle Fuel Technology Average annual mileage, km Number of cars Passenger cars, from 0.8 to > 2l, three gasoline classes gasoline PC Euro 2 и 4 5976 499433 Passenger cars, from 1.4 to > 2l, two diesel classes Diesel PC Euro 4-98/69/EC Stage2005 11738 457104 Passenger cars LPG PC Euro 2-94/12/EEC 66348 26768 Passenger cars CNG PC Euro 4-98/69/EC Stage2005 60178 15183 Light duty <3,5 t gasoline LD Euro 4-98/69/EC Stage2005 8645 7274 Light duty <3,5 t Diesel LD Euro 4-98/69/EC Stage2005 12522 101604 Heavy duty Rigid <=7,5 t Diesel HD Euro II - 91/542/EEC Stage II 15597 4546 Bus City Standard, 15-18 t Diesel HD Euro III - 2000 Standards 30878 1119 City Bus CNG HD Euro III - 2000 Standards 122748 0 Motorcycles, from under 50 to under 250 cm3 gasoline Mop - Euro II, Mot - Euro I 1545 58720 Table 12. Average mileage per vehicle for Bulgaria, 2011 (Source: United Nation Framework Convention of Climate Change, 2013). The ratio between the data in table 8 and those in table 12 shows the proportion of the fuel, burned in urban environments. The values of the ratio are shown in table 13. 611

Average annual mileage, share by type of vehicle Gasoline 0,451 0,364 0,444 Diesel 0,332 0,335 0,283 0,143 Auto gas 0,041 Table 13. Share of average city mileage for vehicles by type in Bulgaria for 2011 compared with the average total mileage. To obtain the average city mileage of a vehicle for Stara Zagora, the data in table 11 were multiplied by those in table 13. The result is shown in table 14. Average annual mileage, km, by type of vehicle Gasoline 1493 1416 375 Diesel 3082 3354 2980 1505 Auto gas 391 Table 14. Average annual city mileage for vehicles in Stara Zagora. The product of relevant data from tables 4, 6 and 14, divided into 1000 gives annual fuel consumption in kilograms of the vehicles on the territory of Stara Zagora. The result is given in table 15. Fuel consumption, kg, by type of vehicle Gasoline 3679546 312519 31862 Diesel 3905369 355206 2104224 265900 Auto gas 316559 Table 15. Fuel consumption in urban conditions from the vehicles of Stara Zagora. The emission factors for NOx by fuel and vehicle type are given in table 16. Emission factor for NOx, g/kg, by type of vehicle Gasoline 29,89 25,46 10,73 Diesel 13,88 18,43 38,29 38,29 Auto gas 34,30 Table 16. Emission factors for nitrogen oxides in g/kg by fuel and vehicle type according to the method Tier 1. (Source: EMEP/EEA emission inventory guidebook 2013 1.A.3.b Road transport, Tier 1 method, p.26 table 3-6) The product of relevant data from tables 15 and 16, divided by 1,000,000 gives in Mg the emitted nitrogen oxides from the traffic in the city of all vehicles per year. The result is given in table 17. 612

General issue: 280,6 t/y Emissions of NOx, Mg/y, by type of vehicle Gasoline 110,0 8,0 0,3 Diesel 54,2 6,5 80,6 10,2 Auto gas 10,9 Table 17. NOx emissions from all vehicles in the city of Stara Zagora in Mg per year. 4. CONCLUSIONS Regulation of traffic in the city of Stara Zagora deviates the trucks from the central part of Stara Zagora, so their contribution to the emission of nitrogen oxides can be ignored, i.e. the above calculations show that for the year traffic in Stara Zagora emits 201 Mg of NOx, which is about 2/3 of all NOx emissions from the city. REFERENCES Characteristic properties of the gas mixture LPG (LPG), 2013. Last visited: 14.1.2014 г. (Bulgarian). http://www.gastradebg.com/pagebg.php?p=2&sp=33 EMEP/EEA emission inventory guidebook 2013 1.A.3.b Road transport, method Tier 1, p.26, table 3-6. Last visited: 14.1.2014 г. http://www.eea.europa.eu/publications/emep-eea-guidebook-2013 EMEP / EEA emission inventory guidebook 2013 1.A.3.b Road transport, Tier 1 method, page 29, table 3-14. Last visited: 14.1.2014 г. http://www.eea.europa.eu/publications/emep-eea-guidebook-2013 Greenhouse Gas Conversion Factors, 2013. Pb13773-ghg-conversionfactors2012.xls, Fuel Properties. Last visited: 14.1.2014 г. https://www.gov.uk/government/publications/2012-greenhouse-gas-conversion-factors-forcompany-reporting Inventory of emissions of CO 2, released into the atmosphere as a result of energy consumption on the territory of Sofia Municipality", 2012, page 19, table 19. Last visited: 14.1.2014 г. http://www.sofia.bg/strategii.asp Methane, 2013. Last visited: 14.1.2014 г. (Bulgarian). http://bg.wikipedia.org Program of reducing levels of nitrogen dioxide and reaching the established norms in Stara Zagora for the period 2013-2015. last visited: 15.1.2013 г. (Bulgarian). http://www.starazagora.bg/bg/administrativni-aktove/programi United Nation Framework Convention of Climate Change, 2013. Page. 533, table 262, page 549, table 264. http://unfccc.int/national_reports/annex_i_ghg_inventories/national_inventories_submissions/items/7383.php 613