Geochemical Journal, Vol. 51, pp. 485 to 494, 2017 doi:10.2343/geochemj.2.0480

Emission inventory and distribution characteristics of atmospheric polycyclic aromatic hydrocarbons in a coking industry city in Northern

WEI LIU,1,2 ZHONGHUAN XIA1,2,3,4* and HAO YANG2,3,4

1Jiangsu Provincial Key Laboratory of Materials Cycling and Pollution Control, School of Environment, Nanjing Normal University, Nanjing 210023, China 2Key Laboratory of Virtual Geographic Environment (Nanjing Normal University), Ministry of Education, Nanjing 210023, China 3Jiangsu Center for Collaborative Innovation in Geographical Information Resource Development and Application, Nanjing 210023, China 4State Key Laboratory Cultivation Base of Geographical Environment Evolution (Jiangsu Province), Nanjing 210023, China

(Received August 25, 2016; Accepted April 5, 2017)

The sources of 16 polycyclic aromatic hydrocarbons (PAHs) in , a coking industry city in Northern China, were studied. The overall emission amount for these 16 PAHs in 2013 in Linfen was 825.12 t, with 149.22 t identified as carcinogenic PAHs. The emission intensity of PAHs in 2013 was about 40.7 kg/km2 in Linfen, which was much higher than the average intensity found in China in 2013. Most of the PAHs were generated from the combustion of domestic, industrial, and coke-production coal, accounting for 78.6% of the total emission amount. Among the emissions of these 16 PAHs, two- and three-ring PAHs made up the majority (68.15%). In the different areas (17 in total) of Linfen, the PAH emissions ranged from 143.35 t in Hongdong County to 2.64 t in Daning County. There was a positive correlation between the rural population and total PAH emissions (R2 = 0.794). The estimated 16 PAH emissions in Linfen from 1995 to 2013 based on historical energy consumption data showed that the amount of PAH emissions has been gradually increasing.

Keywords: PAHs, emission inventory, Linfen, source apportionment, uncertainty analysis

tion was the most important source globally, whereas the INTRODUCTION domination of PAH emissions from residential biomass As a group of persistent organic pollutants (POPs), burning led to relatively high percentages of high mo- polycyclic aromatic hydrocarbons (PAHs) are of great lecular weight PAHs in developing countries. Berdowski concern because of their widespread occurrence and toxic et al. (1997) estimated that the total emissions of six kinds effects on ecosystems and human health (Laflamme and of polycyclic aromatic hydrocarbons in 23 countries and Hites, 1978; Perera, 1997). PAHs are formed mainly by regions in Europe equaled 12500 t, and indicated that these anthropogenic processes, including biomass burning, coal PAHs could mainly be traced to non-industrial emission and petroleum combustion, and coke and metal produc- sources (45.2%). Wild and Jones (1995) estimated that tion (Baek et al., 1991). Natural processes such as forest the annual PAH emissions in the UK were approximately fires and volcanic eruptions also produce PAHs. 1000 t, with 95% of these attributed to domestic coal burn- The establishment of a PAH emission inventory is very ing, motor vehicles, and conflagrations. Jiang et al. (2013) important for assessing their health impact (Zhang et al., estimated that the annual PAH emissions in , 2009) and reducing PAH emissions. PAH emission inven- China in 2010 were 332.10 t, with domestic and coking tories have been developed for several countries (includ- coal burning being the main PAH emission sources. The ing developed and developing countries) and regions, in- spatial distribution of emissions was closely related to cluding the former USSR (EMEP, 2011), Europe (Van der the regional population and economic development of Gon et al., 2007) and North America (Galarneau et al., Taiyuan. 2007). Shen et al. (2013) estimated the annual total PAH As a coking industry city, Linfen is one of the most emissions of the entire world, developing countries, and polluted cities in China because of the high concentra- developed countries in 2007, indicating that transporta- tion of pollutant emissions and adverse weather condi- tions (Zhang et al., 2009). Thus, obtaining the present emission inventory and distribution characteristics of *Corresponding author (e-mail: [email protected]) PAHs in Linfen and analyzing its historical change is es- Copyright © 2017 by The Geochemical Society of Japan. sential for effective environmental management. How-

485 Table 1. Emission factors for different sources (mg/kg)

Component Indoor biomass Outdoor Coal Oil Natural gas burning biomass burning Straw Firewood Wheat Corn Domestic Industrial Coking Transport Industrial Petrol Diesel Nap 14.63 50.30 44.00 1.50 10.90 0.52 4.90 3.63 1.26 0.51 5.20E+04 Acy 3.17 24.88 0.33 0.63 25.60 0.02 0.75 6.86 7.82 0.00 4.01E+03 Ace 2.69 8.94 0.70 0.50 10.00 0.10 0.13 1.62 0.43 0.00 7.24E+04 Flo 0.38 3.77 0.25 0.06 16.10 0.02 0.44 4.67 2.39 0.00 2.25E+02 Phe 6.91 15.03 4.80 1.80 44.20 0.04 1.47 4.00 16.97 0.01 6.39E+02 Ant 1.12 3.67 1.50 0.27 10.50 0.01 0.13 1.00 1.46 0.00 1.96E+01 Fla 3.15 6.58 6.70 0.76 14.10 0.14 0.70 1.74 2.57 0.01 3.90E+02 Pyr 3.00 4.29 3.30 0.79 10.60 0.01 0.54 2.16 2.69 0.00 1.54E+03 BaA 0.60 1.53 2.30 0.08 9.61 0.00 0.17 0.16 0.45 0.01 6.26E+02 Chr 0.88 1.21 2.30 0.15 14.00 0.00 0.13 0.20 0.47 0.00 2.28E+01 BbF 0.16 0.78 0.99 0.03 18.40 0.01 0.13 0.11 0.29 0.00 2.11E+02 BkF 0.74 0.62 0.53 0.18 11.70 0.01 0.07 0.14 0.36 0.00 5.23E+02 BaP 0.11 0.83 0.28 0.02 7.98 0.00 0.24 0.22 0.21 0.00 1.44E+02 DahA 0.00 0.34 0.67 0.00 6.21 0.01 0.02 0.03 0.09 0.00 3.77E+01 IcdP 0.00 0.16 0.00 0.00 9.04 0.00 0.08 0.14 0.14 0.00 1.11E+02 BghiP 0.00 0.35 1.00 0.00 11.50 0.02 0.11 0.27 0.21 0.00 1.59E+02

Note: Natural gas: g/108 m3.

Table 2. Energy Consumption Data of Linfen (104 t) in 2013

Counties Indoor biomass Outdoor straw Coal Oil Natural gas burning (104 m3) Crop Firewood Wheat Corn Domestic Industrial Coking Traffic Industrial Petrol Diesel Total 23.93 120.26 8.15 21.53 150.60 811.60 2937.80 11.43 22.16 12.59 27396.00 Yaodu 3.35 16.81 1.21 1.97 21.09 113.68 411.50 2.40 4.65 2.64 5988.80 Quwo County 1.57 7.87 0.70 1.75 0.00 0.00 0.00 0.91 1.76 1.00 1505.89 Yicheng County 2.10 10.54 0.90 1.51 13.28 71.58 259.11 0.82 1.60 0.91 1974.00 2.90 14.59 1.72 3.55 0.00 0.00 0.00 1.15 2.24 1.27 2813.40 Hongdong County 4.65 23.38 1.76 3.24 25.47 137.25 496.82 1.59 3.08 1.75 4651.78 0.59 2.97 0.16 0.61 17.55 94.58 342.37 0.50 0.98 0.55 583.87 Anze County 0.53 2.66 0.03 1.58 20.13 108.46 392.59 0.46 0.89 0.50 520.61 Fushan County 0.85 4.29 0.35 0.96 0.57 3.06 11.06 0.44 0.85 0.49 809.56 Ji County 0.75 3.76 0.07 0.52 5.44 29.29 106.02 0.13 0.25 0.14 676.23 Xiangning County 1.61 8.10 0.34 0.67 28.84 155.44 562.64 0.85 1.65 0.93 1482.08 Daning County 0.39 1.96 0.00 0.56 0.00 0.00 0.00 0.03 0.06 0.03 410.11 Xi County 0.63 3.17 0.00 1.17 0.00 0.00 0.00 0.08 0.16 0.09 658.05 Yonghe County 0.40 2.03 0.01 0.81 0.00 0.00 0.00 0.04 0.07 0.04 404.01 0.63 3.17 0.00 0.87 18.23 98.26 355.69 0.51 0.99 0.56 682.60 Fenxi County 0.88 4.43 0.17 0.58 0.00 0.00 0.00 0.16 0.32 0.18 918.54 Houma County 0.94 4.72 0.33 0.70 0.00 0.00 0.00 0.82 1.59 0.90 1522.10 County 1.16 5.81 0.39 0.47 0.00 0.00 0.00 0.53 1.04 0.59 1794.35

ever, no such information is currently available, leaving anthracene (BaA), chrysene (CHR), benzo(b)fluoranthene a large information gap. (BbF), benzo(k)fluoranthene (BkF), benzo(a)pyrene The objective of this study was to estimate the emis- (BaP), dibenz(a,h)anthracene (DahA), indeno(l,2,3- sions of individual PAH species, as well as the total for cd)pyrene (IcdP), and benzo(g,h,i)perylene (BghiP). 16 PAHs, and depict their distribution characteristics in Linfen. The 16 PAHs included in the inventory were naph- MATERIAL AND METHODS thalene (NAP), acenaphthylene (ACY), acenaphthene (ACE), fluorine (FLO), phenanthrene (PHE), anthracene Site description (ANT), fluoranthene (FLA), pyrene (PYR), benz(a)- Linfen is situated in the southwestern part of

486 W. Liu et al. Table 3. Total emissions of 16 PAHs in Linfen (t) in 2013

PAHs Indoor biomass Outdoor straw Coal Oil Natural gas Total burning Crop Firewood Wheat Corn Domestic Industrial Coking Traffic Industrial Petrol Diesel Nap 3.50 60.49 3.59 0.32 16.42 4.22 143.95 0.43 0.29 0.06 0.14 233.41 Acy 0.76 29.92 0.03 0.14 38.55 0.16 22.03 0.80 1.79 0.00 0.01 94.18 Ace 0.64 10.75 0.06 0.11 15.06 0.81 3.82 0.19 0.10 0.00 0.20 31.54 Flo 0.09 4.53 0.02 0.01 24.25 0.16 12.93 0.55 0.55 0.00 0.00 43.09 Phe 1.65 18.08 0.39 0.39 66.57 0.32 43.19 0.47 3.88 0.00 0.00 134.93 Ant 0.27 4.41 0.12 0.06 15.81 0.08 3.82 0.12 0.33 0.00 0.00 25.03 Fla 0.75 7.91 0.55 0.16 21.23 1.14 20.56 0.20 0.59 0.00 0.00 53.10 Pyr 0.72 5.16 0.27 0.17 15.96 0.08 15.86 0.25 0.62 0.00 0.00 39.09 BaA 0.14 1.84 0.19 0.02 14.47 0.00 4.99 0.02 0.10 0.00 0.00 21.78 Chr 0.21 1.46 0.19 0.03 21.08 0.00 3.82 0.02 0.11 0.00 0.00 26.92 BbF 0.04 0.94 0.08 0.01 27.71 0.08 3.82 0.01 0.07 0.00 0.00 32.75 BkF 0.18 0.75 0.04 0.04 17.62 0.08 2.06 0.02 0.08 0.00 0.00 20.86 BaP 0.03 1.00 0.02 0.01 12.02 0.00 7.05 0.03 0.05 0.00 0.00 20.19 DahA 0.00 0.41 0.05 0.00 9.35 0.08 0.59 0.00 0.02 0.00 0.00 10.51 IcdP 0.00 0.19 0.00 0.00 13.61 0.00 2.35 0.02 0.03 0.00 0.00 16.21 BghiP 0.00 0.42 0.08 0.00 17.32 0.16 3.23 0.03 0.05 0.00 0.00 21.29 Total 8.98 148.26 5.68 1.47 347.04 7.39 294.07 3.16 8.65 0.06 0.36 825.12

Province, China, and includes a metropolitan area and 16 the latest parameters, including the total and rural counties. The city is surrounded by mountains on three populations and total secondary and tertiary GDPs sides. Thus, the urban area is located in a three quarters- (GDP23) (Wang et al., 2011). The emissions from open closed basin. The total area of Linfen is 20275 km2, with crop residue burning were estimated by the yield of the 4.391 million residents. A semiarid and semi-humid tem- staple crops (Galarneau et al., 2007), including wheat and perate continental climate prevails in this area, with a maize. According to the Global Fire Emissions Database prevailing northwestern wind in winter and southern wind (2013), there were no forest fires in 2013 (Table 2). in summer. Linfen is a typical coking industrial city, with The PAH emissions were calculated as follows: a large number of industrial facilities such as coal mines, steel mills, and coking plants located in the city. These QtTi()= Q ()1 cause serious pollution by PAHs, which pose a severe Âi threat to human health. Qt Q 2 Emission inventory establishment iij()= , () Âj The local emission inventories of 16 priority PAHs were derived from the emission factors, as well as the Qt Q energy consumption structure and composition. ij, ()= Â ijk,, ()3 The emission factors (the mass of PAHs emitted per k unit mass of fuel burned) corresponding to China have been presented in previous studies (Shen et al., 2013; -2 QtFRijk,,()=¥ ijk ,, ijk ,, 10() 4 Zhang et al., 2007; Liu et al., 2015; Chen et al., 2005; Wang et al., 2013) and were adopted in this study (Table where Q (t/a) represents the PAH emissions; F (104 t/a) 1). The major emission sources of PAHs in Linfen are the is the energy consumption; R (mg/kg) is the emission fac- combustion of fossil fuels; petroleum used for transpor- tors; and t, i, j, k, and T denote the year (2013), district of tation; burning of biomass, including straw and firewood; Linfen, type of energy, type of PAH, and total emissions combustion for heating in homes and businesses; and pro- of the city, respectively. duction of coke. Among these, the amounts of domestic coal, industrial coal, and coking coal consumed in 2013 were derived from the Linfen Statistical Yearbook. The RESULTS AND DISCUSSION amounts of indoor biomass (straw and firewood), traffic Energy consumption data petroleum, and industrial petroleum consumed were esti- Table 2 shows the energy consumption of all the dis- mated using a regression model (Zhang et al., 2007) with tricts and counties of Linfen. Domestic coal (150.60 ¥

Emission inventory of PAHs in industry city 487 Fig. 1. Locations of Linfen.

4 4 10 t), industrial coal (811.60 ¥ 10 t), and coking coal tors (Shen et al., 2013; Zhang et al., 2007; Liu et al., 4 (2937.80 ¥ 10 t) accounted for 3.86%, 20.8%, and 75.3% 2015; Chen et al., 2005; Wang et al., 2013), which indi- 3 of the total coal consumption (3.9 ¥ 10 t), respectively. cated that Linfen was one of the most polluted cities in The gasoline and diesel consumptions (traffic petroleum) China. 4 4 were 11.43 ¥ 10 t and 22.16 ¥ 10 t, respectively, and Figure 2 shows the relative contributions of various 4 the industrial petroleum consumption was 12.59 ¥ 10 t. sources to the total emissions in Linfen. Coal burning, The indoor and outdoor biomass fuel quantities consumed including domestic coal, coking coal, and industrial coal, 4 4 for residential uses were 144.19 ¥ 10 t and 29.68 ¥ 10 t, was undoubtedly the major PAH emission source, con- respectively. In addition, the total natural gas consump- tributing 78.6% of the total PAH emissions. Indoor 4 3 tion was 2.7 ¥ 10 m , whereas other energy consump- biomass burning and open crop residue burning were also tion values were negligible. important PAH emission sources. Indoor biomass burn- ing, including firewood and crop residues, contributed Total emission and source profile 19.05% of the total emissions, whereas open crop resi- Table 3 lists the estimated emission inventory of PAHs due burning contributed 0.86% of the total. In addition, from different sources in Linfen, which were calculated traffic petroleum contributed 1.43% of the total emissions. using Eqs. (1)–(4). In 2013, the total annual atmospheric The total PAH emissions in China in 2013 were esti- emissions of the 16 PAHs in Linfen was 825.12 t, which mated to be 83378.8 t. Although the area of Linfen City was equivalent to 188 g per capita per year. This was ap- occupies approximately 0.2% of the total land area of proximately three times the average for China (61.3 g) in China, its PAH emissions contributed 0.99% of China’s 2013 estimated using the nationwide energy consump- total emissions, and Linfen’s PAH emission concentra- tion data for 2013 (Linfen Bureau of Statistics, Linfen tion (40.7 kg/km2) was 4.7 times higher than that of China Statistical Yearbook, 2015), along with the emission fac- (8.7 kg/km2). There were some differences in the PAH

488 W. Liu et al. Fig. 2. Source of profiles of PAH emissions (t) in Linfen in 2013.

source profiles between Linfen City and China as a whole. population in Linfen. The PAH emission factors of in- Indoor biomass burning and coal consumption contrib- door biomass burning and domestic coal burning were uted 19.1% and 78.6% of the total emissions in Linfen, significantly higher than that of industrial coal burning respectively, whereas they occupied 49.8% and 36.6% of (Table 1), because badly equipped biomass and coal stoves the total emissions in China, respectively. The total PAH were used in rural areas (Jiang et al., 2013). Burning stalks emissions of Linfen (825.12 t) were two times higher than in fields was a universal phenomenon in the rural areas the nearby coking industry city of Taiyuan, China (332.10 of Linfen, resulting in high PAH emissions. t), whereas the PAH emission concentration of Linfen was slightly lower than that of Taiyuan (44.62 kg/km2) (Jiang Composition profile et al., 2013). The two cities have the same major emis- Figure 3 shows the PAH emission composition pro- sion sources—domestic coal burning and coking coal con- files of Linfen City in 2013. NAP was the highest emis- sumption, which accounted for 42.09% and 35.67% of sion of the 16 PAHs, accounting for 28.6% of the total, the total emissions in Linfen, respectively, and for 35.25% followed by PHE (16.3%) and ACY (11.4%). The low and 30.23% of the total emissions in Taiyuan, respectively. molecular weight compounds (two- and three-ring PAHs) The industrial and energy structure, as well as the accounted for the majority of the total emissions population status, are likely to be the reasons for the high (68.15%), followed by the middle molecular (four-ring) PAH emissions in Linfen. Industry dominates the GDP (17.08%) and high molecular (five- and six-ring) com- of Linfen, with its proportion reaching 60.63% of the to- pounds (14.77%). tal output of three industries (the primary, secondary, and Different PAH contributions were found among the tertiary industries) of the area in 2013, and industrial coal various sources. Figure 4 shows that natural gas, indoor consumption accounted for 98.8% of the total coal con- firewood, traffic petroleum, and diesel combustion emit- sumption. Moreover, a long heating period in Linfen also ted mainly two- and three-ring PAHs, accounting for more led to a large coal consumption. It is important to note than 80% of the various ring compounds. Additionally, that the rural population accounts for 54.3% of the total indoor and outdoor biomass, domestic coal, industrial,

Emission inventory of PAHs in industry city 489 Fig. 3. PAH emission profiles in Linfen in 2013.

Fig. 4. Emissions ratios of different PAH rings of various emission sources in Linfen in 2013.

and coking coal contributed more middle and high mo- being nearly 2.65 times the latter. To control the carcino- lecular compounds, occupying more than 20% of the to- genic compounds, we should focus on reducing the emis- tal compounds. It should be noted that the emissions of sions of domestic and coking coal burning, such as by middle and high weight carcinogenic compounds (BaA, optimizing the management and technique of the coking CHR, BbF, BkF, BaP, IcdP, and DahA) were 149.22 t and process and improving dust treatment technology. At the accounted for 18.08% of the overall emission amounts of same time, new and clean energy must be developed, and the 16 PAHs. They were mainly from domestic (64.86%) its use must be encouraged to improve the combustion and coking (24.49%) coal consumption, with the former efficiency.

490 W. Liu et al. Fig. 5. Source profiles of BaPeq emissions in Linfen in 2013.

Fig. 6. Emissions of 16 PAHs in different areas of Linfen in 2013.

To describe the combined toxicities of the emissions individual PAHs (Nisbet and LaGoy, 1992) and emission of the 16 PAHs from various sources, the BaP toxic profiles. On a city scale, the average BaPeq/u value from equivalent quantity (g) per unit mass emission (kg) val- all the PAH emission sources was 20.3 g/kg in Linfen in ues from individual sources (BaPeq/u) were defined and 2013, which was slightly more than the global average calculated based on the toxicity equivalent factors of the BaPeq/u value (15.0 g/kg) in 2007 (Shen et al., 2013). In

Emission inventory of PAHs in industry city 491 Fig. 7. Relationship between rural population and 16 PAH emissions.

Fig. 8. Trends of total PAH emissions and emissions of various sources for 1995–2013 in Linfen.

492 W. Liu et al. Linfen, the most toxic sources in terms of the PAH com- ers could be a potential measure in this regard. position were domestic coal consumption (89.4 g/kg), Figure 7 also shows that with the adjustment of the coking production (32.7 g/kg), outdoor crop residue burn- energy industry and reduction of the rural population, PAH ing (31.3 g/kg), and motor vehicles (26.9 g/kg). Sources emissions from the combustion of indoor crop residue and with relatively low BaPeq/u values included industrial oil firewood have decreased in recent years. Because most burning (2.83 g/kg), natural gas burning (3.58 g/kg), and stoves used in rural areas have relatively low efficiencies, industrial coal consumption (16.43 g/kg). there is still room for improvement if the replacement of Based on the calculated BaPeq/u values and total PAH these out-of-date facilities is encouraged by economic emission mass, BaP toxic equivalent quantities were cal- incentives. culated as indicators of the relative health effect poten- tial of all the individual sources (Fig. 5). Because of sig- Uncertainty analysis nificant differences in their BaPeq/u values, sources with The uncertainty of the PAH emission estimates mainly high BaPeq/u values, such as domestic coal consumption lies in the accuracy of the data for the energy consump- and coking production, contributed much more to the tion and emission factors. The energy consumption data health effect potential than other sources. such as for the burning of open crop residues, coal con- sumption, and natural gas consumption were mainly sta- Spatial distribution tistical data, but accounted for 79.5% of the total PAH Because of differences in economic development and emissions in Linfen. In addition, the burning of indoor population density, the counties in Linfen had different biomass and oil consumption were estimated using a fit- emission rates and patterns. The annual emissions for the ting method function derived from a statistical analysis 16 PAHs ranged from 143.35 t in Hongdong County to and mass balance under reasonable assumptions, which 2.64 t in Daning County (Fig. 6), with the top three areas may have caused some uncertainty. There were differences being Hongdong County (143.40 t), Xiangning County in the annual mileage and oil consumption values of dif- (135.97 t), and (116.36 t). There was a ferent kinds of motor vehicles, resulting in high uncer- positive relationship between the total emissions and ru- tainty in the petrol and diesel consumption values. The ral population of different areas (R2 = 0.7937) (Fig. 7). emission factors were collected from different studies, in This might have been because of the use of high emis- which the measured data were from different laborato- sion fuels by the majority of rural families, as well as the ries, leading to some uncertainty. Thus, in the future, it is low combustion efficiency for domestic coal-fired boil- necessary to obtain more accurate emission factors for ers. different sources by making precise measurements.

Historical time trends CONCLUSION The available historical fuel consumption data and emission factors of different sources were used to calcu- The emission concentration of PAHs in Linfen was late the annual PAH emissions in Linfen from 1995 to much higher than the average concentration in China. The 2013 (the emission data for 1996–1999 were skipped be- PAH emissions were dominated by low molecular weight cause the fuel consumption data for 1996–1999 were una- compounds, with NAP being the largest among the 16 vailable) (Fig. 8). During the period from 1995 to 2013, PAHs. The highest contribution to the total emissions for the total emissions increased 37.5%, primarily as a result the 16 PAHs came from coal burning, with domestic coal of the increasing consumption of coking coal and domes- consumption and coking production contributing much tic coal, as well as the rapid increase in motor vehicles more to the health effect potential than other sources. The and crop yields (Bureau, Linfen Statistics, 2014). A com- quantity of PAHs emitted from Hongdong County was parison with the results of Shen et al. (2013) shows that the largest among the various areas in Linfen, followed even though the annual total emissions in developing by Xiangning County and Yaodu District. The total PAH countries have declined since 2000, the emission amounts emissions in different areas had a positive relationship in some cities are still on the rise. with the rural population. The annual PAH emissions in Coke production contributed to a large share of the Linfen showed a gradually growing trend from 1995 to PAH emissions. Driven by the demands in national mar- 2013. kets, the consumption of coking coal remained high dur- ing the past decade in Linfen (Bureau, Linfen Statistics, Acknowledgments—This study was jointly supported by the 2014). Obviously, the emission of PAHs from the coke National Natural Science Foundation of China (41001344 and industry will remain high if no measures are taken to re- 41673108), China Postdoctoral Science Foundation Funded duce either the production or emissions during manufac- Project (2013M541696), Jiangsu Planned Projects for turing. The imposition of PAH emission fees on coke us- Postdoctoral Research Funds (1301040C), Program of Natural Science Research of Jiangsu Higher Education Institutions of

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