1. Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China 2. State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
• The sampling was conducted in city on the Yunnan-Guizhou Plateau for one year.
• The groups of PAHs revealed their different environmental fates and migration paths.
• Seasonal biomass burning could affect the concentration by long-distance transport.
• Industrial sources and traffic emissions were the main contributor of PAHs.
• Living in industrial areas or winter had higher health risk by exposure PAHs in PM2.5.
Monthly particle-phase ambient samples collected at six sampling locations in Yuxi, a high-altitude city on the edge of Southeast Asia, were measured for particle-associated PAHs. As trace substances, polycyclic aromatic hydrocarbons (PAHs) are susceptible to the influences of meteorological conditions, emissions, and gas-particulate partitioning and it is challenging job to precise quantify the source and define the transmission path. The daily concentrations of total PM2.5-bound PAHs ranged from 0.65 to 80.76 ng/m3, with an annual mean of 11.94 ng/m3. Here, we found that the concentration of PM2.5-bound PAHs in winter was significantly higher than that in summer, which was mainly due to source and meteorology influence. The increase of fossil combustion and biomass burning in cold season became the main contributors of PAHs, while precipitation and low temperature exacerbated this difference. According to the concentration variation trend of PM2.5-bound PAHs and their relationship with meteorological conditions, a new grouping of PAHs is applied, which suggested that PAHs have different environmental fates and migration paths. A combination of source analysis and trajectory model supported local sources from combustion of fossil fuel and vehicle exhaust contributed to the major portion on PAHs in particle, but on the Indochina Peninsula the large number of pollutants emitted by biomass burning during the fire season would affect the composition of PAHs through long-range transporting. Risk assessment in spatial and temporal variability suggested that citizens living in industrial areas were higher health risk caused by exposure the PM2.5-bound PAHs than that in other regions, and the risk in winter was three times than in summer.
Dayana Milena Agudelo-Castañeda, Elba Calesso Teixeira (2014). Seasonal changes, identification and source apportionment of PAH in PM1.0. Atmospheric Environment, 96: 186–200 https://doi.org/10.1016/j.atmosenv.2014.07.030
2
ATSDR (2009). Agency for Toxic Substances and Disease Registry (ATSDR). Case Studies in Environmental Medicine. Toxicity of Polycyclic Aromatic Hydrocarbons (PAHs). Agency for Toxic Substances and Disease Registry
3
K R Baker, S N Koplitz, K M Foley, L Avey, A Hawkins (2019). Characterizing grassland fire activity in the Flint Hills region and air quality using satellite and routine surface monitor data. Science of the Total Environment, 659: 1555–1566 https://doi.org/10.1016/j.scitotenv.2018.12.427
pmid: 31096365
4
B A M Bandowe, H Meusel, R J Huang, K Ho, J Cao, T Hoffmann, W Wilcke (2014). PM2.5-bound oxygenated PAHs, nitro-PAHs and parent-PAHs from the atmosphere of a Chinese megacity: Seasonal variation, sources and cancer risk assessment. Science of the Total Environment, 473– 474: 77–87 https://doi.org/10.1016/j.scitotenv.2013.11.108
pmid: 24361780
5
A I Barrado, S Garcia, E Barrado, R M Perez (2012). PM2.5-bound PAHs and hydroxy-PAHs in atmospheric aerosol samples: Correlations with season and with physical and chemical factors. Atmospheric Environment, 49(3): 224–232 https://doi.org/10.1016/j.atmosenv.2011.11.056
6
BCS (2019). China Statistical Yearbook. Beijing: Statistics Bureau of the People’s Republic of China (in Chinese)
7
L Bi, J Hao, P Ning, J Shi, Z Shi, X Xu (2015). Characteristics and sources apportionment of PM2.5-bound PAHs in Kunming. China. Environmental Sciences (Ruse), 35(3): 659–667
8
C Bourotte, M C Forti, S Taniguchi, M C Bícego, P A Lotufo (2005). A wintertime study of PAHs in fine and coarse aerosols in Sáo Paulo City, Brazil. Atmospheric Environment, 39(21): 3799–3811 https://doi.org/10.1016/j.atmosenv.2005.02.054
9
N Domínguez-Morueco, M Schuhmacher, J Sierra, M Nadal, J L Domingo (2016). Assessment of PAH loss in passive air samplers by the effect of temperature. Atmospheric Pollution Research, 7(1): 142–146 https://doi.org/10.1016/j.apr.2015.08.005
10
R Draxler, B Stunder, G Rolph, A Stein, A Taylor (2014). HYSPLIT4 User’s Guide. US Department of Commerce, National Oceanic and Atmospheric Administration, Environmental Research Laboratories, Air Resources Laboratory.
11
I Durre, R S Vose, D B Wuertz (2008). Robust automated quality assurance of radiosonde temperatures. Journal of Applied Meteorology and Climatology, 47(8): 2081–2095 https://doi.org/10.1175/2008JAMC1809.1
12
A Dvorská, G Lammel, J Klánová (2011). Use of diagnostic ratios for studying source apportionment and reactivity of ambient polycyclic aromatic hydrocarbons over central Europe. Atmospheric Environment, 45(2): 420–427 https://doi.org/10.1016/j.atmosenv.2010.09.063
13
G C Fang, Y S Wu, J C Chen, C N Chang, T T Ho (2006). Characteristic of polycyclic aromatic hydrocarbon concentrations and source identification for fine and coarse particulates at Taichung Harbor near Taiwan Strait during 2004–2005. Science of the Total Environment, 366(2–3): 729–738 https://doi.org/10.1016/j.scitotenv.2005.09.075
pmid: 16343600
14
GB3095-2012 (2012). Ambient air quality standard. Standard.Beijing: Ministry of Environmental Protection of the People’s Republic of China (in Chinese)
15
C Geng, J Chen, X Yang, L Ren, B Yin, X Liu, Z Bai (2014). Emission factors of polycyclic aromatic hydrocarbons from domestic coal combustion in China. Journal of Environmental Sciences (China), 26(1): 160–166 https://doi.org/10.1016/S1001-0742(13)60393-9
pmid: 24649702
16
C W Götz, M Scheringer, M MacLeod, F Wegmann, K Hungerbühler. (2008). Regional differences in gas–particle partitioning and deposition of semivolatile organic compounds on a global scale. Atmospheric Environment, 42(3): 554–567 https://doi.org/10.1016/j.atmosenv.2007.08.033
17
H Guo, S C Lee, K F Ho, X M Wang, S C Zou (2003). Particle-associated polycyclic aromatic hydrocarbons in urban air of Hong Kong. Atmospheric Environment, 37(38): 5307–5317 https://doi.org/10.1016/j.atmosenv.2003.09.011
18
R M Harrison, D J T Smith, L Luhana (1996). Source apportionment of atmospheric polycyclic aromatic hydrocarbons collected from an urban location in Birmingham, UK. Environmental Science & Technology, 30(3): 825–832 https://doi.org/10.1021/es950252d
IARC (2008). Monographs on the Evaluation of Carcinogenic Risk to Human: Air Pollution, Part 1. In: Some Non-Heterocyclic PAHs and Related Industrial Exposures, Vol.92. Washington, DC: World Health Organization International Agency for Research on Cancer
21
G Karavalakis, G Fontaras, D Ampatzoglou, M Kousoulidou, S Stournas, Z Samaras, E Bakeas (2010). Effects of low concentration biodiesel blends application on modern passenger cars. Part 3: Impact on PAH, nitro-PAH, and oxy-PAH emissions. Environmental Pollution, 158(5): 1584–1594 https://doi.org/10.1016/j.envpol.2009.12.017
pmid: 20083330
22
K Kashiwa, M Arai, Y Kobayashi (2020). Oxygen effect on PAH and PM formation in low temperature benzene pyrolysis. Fuel, 262:116–429
23
I G Kavouras, P Koutrakis, M Tsapakis, E Lagoudaki, E G Stephanou, D Von Baer, P Oyola (2001). Source apportionment of urban particulate aliphatic and polynuclear aromatic hydrocarbons (PAHs) using multivariate methods. Environmental Science & Technology, 35(11): 2288–2294 https://doi.org/10.1021/es001540z
pmid: 11414034
24
N Khalili, P Scheff, T Holsen (1995). PAH source fingerprints for coke ovens, diesel and gasoline engines, highway tunnels, and wood combustion emissions. Atmospheric Environment, 29(4): 533–542 https://doi.org/10.1016/1352-2310(94)00275-P
25
M F Khan, M T Latif, C H Lim, N Amil, S A Jaafar, D Dominick, M S Mohd Nadzir, M Sahani, N M Tahir (2015). Seasonal effect and source apportionment of polycyclic aromatic hydrocarbons in PM2.5. Atmospheric Environment, 106(178): 178–190 https://doi.org/10.1016/j.atmosenv.2015.01.077
26
D J Kielhorn, U Wahnschaffe, I Mangelsdorf (2003). Selected nitro- and nitro- oxy- polycyclic aromatic hydrocarbons. Environmental Health Criteria: 229
27
R K Larsen 3rd, J E Baker (2003). Source apportionment of polycyclic aromatic hydrocarbons in the urban atmosphere: A comparison of three methods. Environmental Science & Technology, 37(9): 1873–1881 https://doi.org/10.1021/es0206184
pmid: 12775060
28
A R Lea-Langton, A B Ross, K D Bartle, G E Andrews, J M Jones, H Li, M Pourkashanian, A Williams. (2013). Low temperature PAH formation in diesel combustion. Journal of Analytical and Applied Pyrolysis, 103: 119–125 https://doi.org/10.1016/j.jaap.2012.10.009
29
J Li, G Zhang, S Qi (2004). Characteristics and seasonal variations and influence factors on polycyclic aromatic hydrocarbon in Guangzhou City. Environmental Sciences, 25(3): 7–13
30
R J Li, X J Kou, H Geng, C Dong, Z W Cai (2014). Pollution characteristics of ambient PM2.5-bound PAHs and NPAHs in a typical winter time period in Taiyuan. Chinese Chemical Letters, 25(5): 663–666 https://doi.org/10.1016/j.cclet.2014.03.032
31
W Li, Y Peng, J Shi, W Qiu, J Wang, Z Bai (2011). Particulate polycyclic aromatic hydrocarbons in the urban northeast region of China: Profiles, distributions and sources. Atmospheric Environment, 45(40): 7664–7671 https://doi.org/10.1016/j.atmosenv.2011.04.004
32
Z Li, E N Porter, A Sjodin, L L Needham, S Lee, A G Russell, J A Mulholland (2009). Characterization of PM2.5−bound polycyclic aromatic hydrocarbons in atlantad-seasonal variations at urban, suburban, and rural ambient air monitoring sites. Atmospheric Environment, 43(27): 4187–4193 https://doi.org/10.1016/j.atmosenv.2009.05.031
33
L Ma, B Li, Y Liu, X Sun, D Fu, S Sun, S Thapa, J Geng, H Qi, A Zhang, C Tian (2020a). Characterization, sources and risk assessment of PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) and nitrated PAHs (NPAHs) in Harbin, a cold city in northern China. Journal of Cleaner Production, 264: 118296 https://doi.org/10.1016/j.jclepro.2020.121673
34
W Ma, L Liu, H Jia, M Yang, Y Li (2018). PAHs in Chinese atmosphere part i: Concentration, source and temperature dependence. Atmospheric Environment, 173: 330–337 https://doi.org/10.1016/j.atmosenv.2017.11.029
35
W L Ma, F J Zhu, P T Hu, L N Qiao, Y F Li (2020b). Gas/particle partitioning of PAHs based on equilibrium-state model and steady-state model. Science of the Total Environment, 706: 136029 https://doi.org/10.1016/j.scitotenv.2019.136029
pmid: 31855629
36
T Martellini, M Giannoni, L Lepri, A Katsoyiannis, A Cincinelli (2012). One year intensive PM2.5 bound polycyclic aromatic hydrocarbons monitoring in the area of Tuscany, Italy. Concentrations, source understanding and implications. Environmental Pollution, 164(1): 252–258 https://doi.org/10.1016/j.envpol.2011.12.040
pmid: 22377904
37
P Masclet, G Mouvier, K Nikolaou (1986). Relative decay index and sources of polycyclic aromatic hydrocarbons. Atmospheric Environment, 20(3): 439–446 https://doi.org/10.1016/0004-6981(86)90083-1
38
A Mastral, M Callen, J Lopez, R Murillo, T Garcıa, M Navarro (2003). Critical review on atmospheric PAH: Assessment of reported data in the Mediterranean Basin. Fuel Processing Technology, 80(2): 183–193 https://doi.org/10.1016/S0378-3820(02)00249-7
39
A M Mastral, M Call’en, R Murillo (1996). Assessment of PAH emissions as a function of coal combustion variables. Fuel, 75(13): 1533–1536 https://doi.org/10.1016/0016-2361(96)00120-2
40
J L Mumford, X Li, F Hu, X B Lu, J C Chuang (1995). Human exposure and dosimetry of polycyclic aromatic hydrocarbons in urine from Xuan Wei, China with high lung cancer mortality associated with exposure to unvented coal smoke. Carcinogenesis, 16(12): 3031–3036 https://doi.org/10.1093/carcin/16.12.3031
pmid: 8603481
41
I C T Nisbet, P K LaGoy (1992). Toxic equivalency factors (TEFs) for polycyclic aromatic hydrocarbons (PAHs). Regulatory Toxicology and Pharmacology: RTP, 16(3): 290–300 https://doi.org/10.1016/0273-2300(92)90009-X
pmid: 1293646
42
N T Kim Oanh, D A Permadi, P K Hopke, K R Smith, N P Dong, A N Dang. (2018). Annual emissions of air toxics emitted from crop residue open burning in southeast Asia over the period of 2010–2015. Atmospheric Environment, 187: 163–173 https://doi.org/10.1016/j.atmosenv.2018.05.061
43
B Panther, M Hooper, N Tapper (1999). A comparison of air particulate matter and associated polycyclic aromatic hydrocarbons in some tropical and temperate urban environments. Atmospheric Environment, 33(24-25): 4087–4099 https://doi.org/10.1016/S1352-2310(99)00150-8
44
S Ramachandran, T A Rajesh, S Kedia (2019). Influence of relative humidity, mixed layer height, and mesoscale vertical-velocity variations on column and surface aerosol characteristics over an urban region. Boundary-Layer Meteorology, 170(1): 161–181 https://doi.org/10.1007/s10546-018-0384-0
45
K Ravindra, L Bencs, E Wauters, J de Hoog, F Deutsch, E Roekens, N Bleux, P Berghmans, R Van Grieken. (2006). Seasonal and site-specific variation in vapour and aerosol phase PAHs over Flanders (Belgium) and their relation with anthropogenic activities. Atmospheric Environment, 40(4): 771–785 https://doi.org/10.1016/j.atmosenv.2005.10.011
46
J Ringuet, A Albinet, E Leoz-Garziandia, H Budzinski, E Villenave (2012). Reactivity of polycyclic aromatic compounds (PAHs, NPAHs and OPAHs) adsorbed on natural aerosol particles exposed to atmospheric oxidants. Atmospheric Environment, 61: 15–22 https://doi.org/10.1016/j.atmosenv.2012.07.025
47
W F Rogge, L M Hildemann, M A Mazurek, G R Cass, B R T Simoneit (1993). Sources of fine organic aerosol. 2. Non-catalyst and catalyst-equipped automobiles and heavy duty diesel trucks. Environmental Science & Technology, 27(4): 636–651 https://doi.org/10.1021/es00041a007
48
N E Sánchez, Á Millera, R Bilbao, M U Alzueta (2013). Polycyclic aromatic hydrocarbons (PAH), soot and light gases formed in the pyrolysis of acetylene at different temperatures: Effect of fuel concentration. Journal of Analytical and Applied Pyrolysis, 103: 126–133 https://doi.org/10.1016/j.jaap.2012.10.027
49
O Sevimoğlu , W F Rogge (2019). Seasonal variations of PM10–trace elements, PAHs and levoglucosan: Rural sugarcane growing area versus coastal urban area in southeastern Florida, USA. Part Ⅱ: Elemental concentrations. Particuology, 46: 99–108 https://doi.org/10.1016/j.partic.2019.05.001
50
J Shi, Y Peng, W Li, W Qiu, Z Bai, S Kong, T Jin (2010). Characterization and source identification of PM10-bound polycyclic aromatic hydrocarbons in urban air of Tianjin, China. Aerosol and Air Quality Research, 10(5): 507–518 https://doi.org/10.4209/aaqr.2010.06.0050
51
M D R Sienra, N G Rosazza, M Préndez (2005). Polycyclic aromatic hydrocarbons and their molecular diagnostic ratios in urban atmospheric respirable particulate matter. Atmospheric Research, 75(4): 267–281 https://doi.org/10.1016/j.atmosres.2005.01.003
52
M F Simcik, S J Eisenreich, P J Lioy (1999). Source apportionment and source/sink relationships of PAHs in the coastal atmosphere of Chicago and lake Michigan. Atmospheric Environment, 33(30): 5071–5079 https://doi.org/10.1016/S1352-2310(99)00233-2
53
H Tao, HY Wang, W Ren, K CLin (2019). Kinetic mechanism for modeling the temperature effect on PAH formation in pyrolysis of acetylene. Fuel, 255: 115, 796
54
E C Teixeira, D M Agudelo-Castañeda, J M G Fachel, K A Leal, K O Garcia, F Wiegand. (2012). Source identification and seasonal variation of polycyclic aromatic hydrocarbons associated with atmospheric fine and coarse particles in the metropolitan area of Porto Alegre, RS, Brazil. Atmospheric Research, 118: 390–403 https://doi.org/10.1016/j.atmosres.2012.07.004
55
S Tomaz, P Shahpoury, J L Jaffrezo, G Lammel, E Perraudin, E Villenave, A Albinet (2016). One-year study of polycyclic aromatic compounds at an urban site in Grenoble (France): Seasonal variations, gas/particle partitioning and cancer risk estimation. Science of the Total Environment, 565: 1071–1083 https://doi.org/10.1016/j.scitotenv.2016.05.137
pmid: 27261422
56
USEPA (1999). Compendium of methods for the determination of toxic organic compounds in ambient air: determination of polycyclic aromatic hydrocarbons (PAHs) in ambient air using gas chromatograph/mass spectrometer (GC/MS). method to –13a. Washington, DC: Environmental Protection Agency. U.S. Government Printing Office
57
A Valavanidis, K Fiotakis, T Vlahogianni, E B Bakeas, S Triantafillaki, V Paraskevopoulou, M Dassenakis (2006). Characterization of atmospheric particulates, particle-bound transition metals and polycyclic aromatic hydrocarbons of urban air in the centre of Athens (Greece). Chemosphere, 65(5): 760–768 https://doi.org/10.1016/j.chemosphere.2006.03.052
pmid: 16674985
58
QT Vuong, PQ Thang, TNT Nguyen, T Ohura, SD Choi (2020). Seasonal variation and gas/particle partitioning of atmospheric halogenated polycyclic aromatic hydrocarbons and the effects of meteorological conditions in Ulsan, South Korea. Environmental Pollution, 263:114–592
59
J Wang, N B Geng, Y F Xu, W D Zhang, X Y Tang, R Q Zhang (2014). PAHs in PM2.5 in Zhengzhou: Concentration, carcinogenic risk analysis, and source apportionment. Environmental Monitoring and Assessment, 186(11): 7461–7473 https://doi.org/10.1007/s10661-014-3940-1
pmid: 25060861
60
Y Wang, M Bao, Y Zhang, F Tan, H Zhao, Q Zhang, Q Li (2020). Polycyclic aromatic hydrocarbons in the atmosphere and soils of Dalian, China: Source, urban-rural gradient, and air-soil exchange. Chemosphere, 244: 125–518
61
C Wiedinmyer, S K Akagi, R J Yokelson, L K Emmons, J A Al-Saadi, J J Orlando, A J Soja. (2011). The Fire INventory from NCAR (FINN): A high resolution global model to estimate the emissions from open burning. Geoscientific Model Development, 4(3): 625–641 https://doi.org/10.5194/gmd-4-625-2011
62
K Yang, Y Huang, G Zhao, Y Lei, K Wang (2010). The expression of PAH-DNA adducts in lung tissues of Xuanwei female lung cancer patients. The Chinese-German Journal of Clinical Oncology. 9: 497–501 https://doi.org/10.1007/s10330-010-0669-3
pmid: 20677652
