Abstract
To develop effective mitigation policies, a comprehensive understanding of the evolution of the chemical composition, formation mechanisms, and the contribution of sources at different pollution levels is required. PM2.5 samples were collected for 1 year from August 2016 to August 2017 at an urban site in Zibo, then chemical compositions were analyzed. Secondary inorganic aerosols (SNA), anthropogenic minerals (MIN), and organic matter (OM) were the most abundant components of PM2.5, but only the mass fraction of SNA increased as the pollution evolved, implying that PM2.5 pollution was caused by the formation of secondary aerosols, especially nitrate. A more intense secondary transformation was found in the heating season (from November 15, 2016, to March 14, 2017), and a faster secondary conversion of nitrate than sulfate was discovered as the pollution level increased. The formation of sulfate was dominated by heterogeneous reactions. High relative humidity (RH) in polluted periods accelerated the formation of sulfate, and high temperature in the non-heating season also promoted the formation of sulfate. Zibo city was under ammonium-rich conditions during polluted periods in both seasons; therefore, nitrate was mainly formed through homogeneous reactions. The liquid water content increased significantly as the pollution levels increased when the RH was above 80%, indicating that the hygroscopic growth of aerosol aggravated the PM2.5 pollution. Source apportionment showed that PM2.5 was mainly from secondary aerosol formation, road dust, coal combustion, and vehicle emissions, contributing 36.6%, 16.5%, 14.7%, and 13.1% of PM2.5 mass, respectively. The contribution of secondary aerosol formation increased remarkably with the deterioration of air quality, especially in the heating season.
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Data availability
All relevant data are within the manuscript and available from the corresponding author upon request.
Abbreviations
- BTH:
-
Beijing–Tianjin–Hebei
- C:
-
Clean days
- HP:
-
Heavily polluted
- LWC:
-
Liquid water content
- MDL:
-
Method detection limit
- MIN:
-
Minerals
- MP:
-
Moderately polluted
- NOR:
-
Nitrogen oxidation ratio
- OM:
-
Organic matter
- PMF:
-
Positive matric factorization
- RH:
-
Relative humidity
- SNA:
-
Secondary inorganic aerosols
- SOR:
-
Sulfur oxidation ratio
- SP:
-
Slightly polluted
- T:
-
Temperature
- TE:
-
Trace elements
- UM:
-
Unidentified matter
- WS:
-
Wind speed
References
Bao Z, Chen L, Li K, Han L, Wu X, Gao X, Azzi M, Cen K (2019) Meteorological and chemical impacts on PM2.5 during a haze episode in a heavily polluted basin city of eastern China. Environ Pollut 250:520–529. https://doi.org/10.1016/j.envpol.2019.04.045
Bei N, Li X, Tie X, Zhao L, Wu J, Li X, Liu L, Shen Z, Li G (2020) Impact of synoptic patterns and meteorological elements on the wintertime haze in the Beijing-Tianjin-Hebei region, China from 2013 to 2017. Sci Total Environ 704:135210. https://doi.org/10.1016/j.scitotenv.2019.135210
Cesari D, Donateo A, Conte M, Merico E, Giangreco A, Giangreco F, Contini D (2016) An inter-comparison of PM2.5 at urban and urban background sites: chemical characterization and source apportionment. Atmos Res 174–175:106–119. https://doi.org/10.1016/j.atmosres.2016.02.004
Chang X, Wang S, Zhao B, Cai S, Hao J (2018) Assessment of inter-city transport of particulate matter in the Beijing–Tianjin–Hebei region. Atmos Chem Phys 18(7):4843–4858. https://doi.org/10.5194/acp-18-4843-2018
Chang X, Wang S, Zhao B, Xing J, Liu X, Wei L, Song Y, Wu W, Cai S, Zheng H, Ding D, Zheng M (2019) Contributions of inter-city and regional transport to PM2.5 concentrations in the Beijing-Tianjin-Hebei region and its implications on regional joint air pollution control. Sci Total Environ 660:1191–1200. https://doi.org/10.1016/j.scitotenv.2018.12.474
Chen L, Watson JG, Chow JC, Green MC, Inouye D, Dick K (2012) Wintertime particulate pollution episodes in an urban valley of the Western US: a case study. Atmos Chem Phys 12(21):10051–10064. https://doi.org/10.5194/acp-12-10051-2012
Chen C, Zhang H, Li H, Wu N, Zhang Q (2020) Chemical characteristics and source apportionment of ambient PM1.0 and PM2.5 in a polluted city in North China plain. Atmos Environ 242:117867. https://doi.org/10.1016/j.atmosenv.2020.117867
Cheng N, Li Y, Cheng B, Wang X, Meng F, Wang Q, Qiu Q (2018) Comparisons of two serious air pollution episodes in winter and summer in Beijing. J Environ Sci 69:141–154. https://doi.org/10.1016/j.jes.2017.10.002
Cheung K, Daher N, Kam W, Shafer MM, Ning Z, Schauer JJ, Sioutas C (2011) Spatial and temporal variation of chemical composition and mass closure of ambient coarse particulate matter (PM10–2.5) in the Los Angeles area. Atmos Environ 45(16):2651–2662. https://doi.org/10.1016/j.atmosenv.2011.02.066
Dong Z, Wang S, Xing J, Chang X, Ding D, Zheng H (2020) Regional transport in Beijing-Tianjin-Hebei region and its changes during 2014–2017: the impacts of meteorology and emission reduction. Sci Total Environ 737:139792. https://doi.org/10.1016/j.scitotenv.2020.139792
Fu Q, Zhuang G, Wang J, Xu C, Huang K, Li J, Hou B, Lu T, Streets DG (2008) Mechanism of formation of the heaviest pollution episode ever recorded in the Yangtze River Delta, China. Atmos Environ 42(9):2023–2036. https://doi.org/10.1016/j.atmosenv.2007.12.002
Gao J, Wang K, Wang Y, Liu S, Zhu C, Hao J, Liu H, Hua S, Tian H (2018) Temporal-spatial characteristics and source apportionment of PM2.5 as well as its associated chemical species in the Beijing-Tianjin-Hebei region of China. Environ Pollut 233:714–724. https://doi.org/10.1016/j.envpol.2017.10.123
Guo B, Wang Y, Zhang X, Che H, Zhong J, Chu Y, Cheng L (2020) Temporal and spatial variations of haze and fog and the characteristics of PM2.5 during heavy pollution episodes in China from 2013 to 2018. Atmos Pollut Res 11(10):1847–1856. https://doi.org/10.1016/j.apr.2020.07.019
Guo Y, Cao Z, Jiao X, Ba D, Zhang Y, Hua J, Liu W, Teng X (2021) Pre-pregnancy exposure to fine particulate matter (PM2.5) increases reactive oxygen species production in oocytes and decrease litter size and weight in mice. Environ Pollut 268:115858. https://doi.org/10.1016/j.envpol.2020.115858
Han L, Xiang X, Zhang H, Cheng S, Wang H, Wei W, Wang H, Lang J (2019) Insights into submicron particulate evolution, sources and influences on haze pollution in Beijing, China. Atmos Environ 201:360–368. https://doi.org/10.1016/j.atmosenv.2018.12.045
Hu Q, Fu H, Wang Z, Kong L, Chen M, Chen J (2016) The variation of characteristics of individual particles during the haze evolution in the urban Shanghai atmosphere. Atmos Res 181:95–105. https://doi.org/10.1016/j.atmosres.2016.06.016
Ianniello A, Spataro F, Esposito G, Allegrini I, Hu M, Zhu T (2011) Chemical characteristics of inorganic ammonium salts in PM2.5 in the atmosphere of Beijing (China). Atmos Chem Phys 11:10803–10822. https://doi.org/10.5194/acp-11-10803-2011
Jiang P, Chen X, Li Q, Mo H, Li L (2020) High-resolution emission inventory of gaseous and particulate pollutants in Shandong Province, eastern China. J Clean Prod 259:120806. https://doi.org/10.1016/j.jclepro.2020.120806
Khan MF, Hirano K, Masunaga S (2010) Quantifying the sources of hazardous elements of suspended particulate matter aerosol collected in Yokohama, Japan. Atmos Environ 44(21–22):2646–2657. https://doi.org/10.1016/j.atmosenv.2010.03.040
Kim YH, Krantz QT, McGee J, Kovalcik KD, Duvall RM, Willis RD, Kamal AS, Landis MS, Norris GA, Gilmour MI (2016) Chemical composition and source apportionment of size fractionated particulate matter in Cleveland, Ohio, USA. Environ Pollut 218:1180–1190. https://doi.org/10.1016/j.envpol.2016.08.073
Li H, Ma Y, Duan F, He K, Zhu L, Huang T, Kimoto T, Ma X, Ma T, Xu L, Xu B, Yang S, Ye S, Sun Z, An J, Zhang Z (2017) Typical winter haze pollution in Zibo, an industrial city in China: characteristics, secondary formation, and regional contribution. Environ Pollut 229:339–349. https://doi.org/10.1016/j.envpol.2017.05.081
Li W, Liu X, Zhang Y, Sun K, Wu Y, Xue R, Zeng L, Qu Y, An J (2018) Characteristics and formation mechanism of regional haze episodes in the Pearl River Delta of China. J Environ Sci 63:236–249. https://doi.org/10.1016/j.jes.2017.03.018
Li R, Wang Z, Cui L, Fu H, Zhang L, Kong L, Chen W, Chen J (2019) Air pollution characteristics in China during 2015–2016: spatiotemporal variations and key meteorological factors. Sci Total Environ 648:902–915. https://doi.org/10.1016/j.scitotenv.2018.08.181
Li M, Wu L, Zhang X, Wang X, Bai W, Ming J, Geng C, Yang W (2020a) Comparison of PM2.5 chemical compositions during haze and non-haze days in a heavy industrial city in North China. Aerosol Air Qual Res 20(9): 1950–1960. https://doi.org/10.4209/aaqr.2019.11.0591
Li Q, Wu B, Liu J, Zhang H, Cai X, Song Y (2020b) Characteristics of the atmospheric boundary layer and its relation with PM2.5 during haze episodes in winter in the North China Plain. Atmos Environ 223: 117265. https://doi.org/10.1016/j.atmosenv.2020.117265
Liu B, Song N, Dai Q, Mei R, Sui B, Bi X, Feng Y (2016) Chemical composition and source apportionment of ambient PM2.5 during the non-heating period in Taian, China. Atmos Res 170:23–33. https://doi.org/10.1016/j.atmosres.2015.11.002
Liu B, Yang J, Yuan J, Wang J, Dai Q, Li T, Bi X, Feng Y, Xiao Z, Zhang Y, Xu H (2017) Source apportionment of atmospheric pollutants based on the online data by using PMF and ME2 models at a megacity, China. Atmos Res 185:22–31. https://doi.org/10.1016/j.atmosres.2016.10.023
Liu H, Tian H, Zhang K, Liu S, Cheng K, Yin S, Liu Y, Liu X, Wu Y, Liu W, Bai X, Wang Y, Shao P, Luo L, Lin S, Chen J, Liu X (2019) Seasonal variation, formation mechanisms and potential sources of PM2.5 in two typical cities in the Central Plains Urban Agglomeration, China. Sci Total Environ 657:657–670. https://doi.org/10.1016/j.scitotenv.2018.12.06
Luo Y, Zhou X, Zhang J, Xiao Y, Wang Z, Zhou Y, Wang W (2018) PM2.5 pollution in a petrochemical industry city of northern China: seasonal variation and source apportionment. Atmos Res 212:285–295. https://doi.org/10.1016/j.atmosres.2018.05.029
Mantas E, Remoundaki E, Halar I, Kassomenos P, Theodosi C, Hatzikioseyian A, Mihalopoulos N (2014) Mass closure and source apportionment of PM2.5 by Positive Matrix Factorization analysis in urban Mediterranean environment. Atmos Environ 94:154–163. https://doi.org/10.1016/j.atmosenv.2014.05.002
MEEP (2017) 2017 Air pollution prevention and management plan for the Beijing-Tianjin-Hebei Region and its surrounding areas
Pan H, Lu X, Lei K (2017) A comprehensive analysis of heavy metals in urban road dust of Xi’an, China: contamination, source apportionment and spatial distribution. Sci Total Environ 609:1361–1369. https://doi.org/10.1016/j.scitotenv.2017.08.004
Pang N, Gao J, Che F, Ma T, Liu S, Yang Y, Zhao P, Yuan J, Liu J, Xu Z, Chai F (2020a) Cause of PM2.5 pollution during the 2016–2017 heating season in Beijing, Tianjin, and Langfang, China. J Environ Sci 95:201–209. https://doi.org/10.1016/j.jes.2020.03.024
Pang Y, Huang W, Luo X, Chen Q, Zhao Z, Tang M, Hong Y, Chen J, Li H (2020b) In-vitro human lung cell injuries induced by urban PM2.5 during a severe air pollution episode: variations associated with particle components. Ecotoxicol Environ Saf 206:111406. https://doi.org/10.1016/j.ecoenv.2020.111406
Pathak RK, Wu WS, Wang T (2009) Summertime PM2.5 ionic species in four major cities of China: nitrate formation in an ammonia-deficient atmosphere. Atmos Chem Phys 9:1711–1722. https://doi.org/10.5194/acp-9-1711-2009
Peng J, Hu M, Shang D, Wu Z, Du Z, Tan T, Wang Y, Zhang F, Zhang R (2021) Explosive secondary aerosol formation during severe haze in the North China Plain. Environ Sci Technol 55(4):2189–2207. https://doi.org/10.1021/acs.est.0c07204
Polissar AV, Hopke PK, Harris JM, Bodhaine BA, Dutton EG (1998) Source regions for atmospheric aerosol measured in the western arctic. J Aerosol Sci 29:S513–S514. https://doi.org/10.1016/S0021-8502(98)00177-3
Qiao T, Zhao M, Xiu G, Yu J (2015) Seasonal variations of water-soluble composition (WSOC, Hulis and WSIIs) in PM1 and its implications on haze pollution in urban Shanghai, China. Atmos Environ 123:306–314. https://doi.org/10.1016/j.atmosenv.2015.03.010
Qiao B, Chen Y, Tian M, Wang H, Yang F, Shi G, Zhang L, Peng C, Luo Q, Ding S (2019) Characterization of water-soluble inorganic ions and their evolution processes during PM2.5 pollution episodes in a small city in southwest China. Sci Total Environ 650:2605–2613. https://doi.org/10.1016/j.scitotenv.2018.09.376
Sah D, Verma PK, Kandikonda MK, Lakhani A (2019) Pollution characteristics, human health risk through multiple exposure pathways, and source apportionment of heavy metals in PM10 at Indo-Gangetic site. Urban Clim 27:149–162. https://doi.org/10.1016/j.uclim.2018.11.010
Shen J, Zhao Q, Cheng Z, Huo J, Zhu W, Zhang Y, Duan Y, Wang X, Antony Chen L W, Fu Q (2020) Evolution of source contributions during heavy fine particulate matter (PM2.5) pollution episodes in eastern China through online measurements. Atmos Environ 232: 117569. https://doi.org/10.1016/j.atmosenv.2020.117569
Song M, Liu X, Tan Q, Feng M, Qu Y, An J, Zhang Y (2019) Characteristics and formation mechanism of persistent extreme haze pollution events in Chengdu, southwestern China. Environ Pollut 1–12. https://doi.org/10.1016/j.envpol.2019.04.081
Sun X, Wang K, Li B, Zong Z, Shi X, Ma L, Fu D, Thapa S, Qi H, Tian C (2020) Exploring the cause of PM2.5 pollution episodes in a cold metropolis in China. J Clean Prod 256: 120275. https://doi.org/10.1016/j.jclepro.2020.120275
Tan J, Zhang L, Zhou X, Duan J, Li Y, Hu J, He K (2017) Chemical characteristics and source apportionment of PM2.5 in Lanzhou. China Sci Total Environ 601–602:1743–1752. https://doi.org/10.1016/j.scitotenv.2017.06.050
Tao Y, Ye X, Ma Z, Xie Y, Wang R, Chen J, Yang X, Jiang S (2016) Insights into different nitrate formation mechanisms from seasonal variations of secondary inorganic aerosols in Shanghai. Atmos Environ 145:1–9. https://doi.org/10.1016/j.atmosenv.2016.09.012
Tian SL, Pan YP, Wang YS (2016) Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes. Atmos Chem Phys 16(1):1–19. https://doi.org/10.5194/acp-16-1-2016
Tian S, Pan Y, Liu Z, Wen T, Wang Y (2014) Size-resolved aerosol chemical analysis of extreme haze pollution events during early 2013 in urban Beijing, China. J Hazard Mater 279:452–460. https://doi.org/10.1016/j.jhazmat.2014.07.023
Vecchi R, Chiari M, Alessandro D, A, Fermo P. Lucarelli F, Mazzei F, Nava S, Piazzalunga A, Prati P, Silvani F, Valli G, (2008) A mass closure and PMF source apportionment study on the sub-micron sized aerosol fraction at urban sites in Italy. Atmos Environ 42(9):2240–2253. https://doi.org/10.1016/j.atmosenv.2007.11.039
Wang Y, Jia C, Tao J, Zhang L, Liang X, Ma J, Gao H, Huang T, Zhang K (2016) Chemical characterization and source apportionment of PM2.5 in a semi-arid and petrochemical-industrialized city, Northwest China. Sci Total Environ 573:1031–1040. https://doi.org/10.1016/j.scitotenv.2016.08.179
Wang H, Tian M, Chen Y, Shi G, Liu Y, Yang F, Zhang L, Deng L, Yu J, Peng C, Cao X (2018) Seasonal characteristics, formation mechanisms and source origins of PM2.5 in two megacities in Sichuan Basin, China. Atmos Chem Phys 18(2):865–881. https://doi.org/10.5194/acp-18-865-2018
Wang Q, Huang X, Tam F, Zhang X, Liu KM, Yeung C, Feng Y, Cheng Y, Wong YK, Ng WM, Wu C, Zhang Q, Zhang T, Lau NT, Yuan Z, Lau A, Yu JZ (2019a) Source apportionment of fine particulate matter in Macao, China with and without organic tracers: a comparative study using positive matrix factorization. Atmos Environ 198:183–193. https://doi.org/10.1016/j.atmosenv.2018.10.057
Wang S, Yin S, Zhang R, Yang L, Zhao Q, Zhang L, Yan Q, Jiang N, Tang X (2019b) Insight into the formation of secondary inorganic aerosol based on high-time-resolution data during haze episodes and snowfall periods in Zhengzhou, China. Sci Total Environ 660:47–56. https://doi.org/10.1016/j.scitotenv.2018.12.465
Wu G, Wu X, Du X, Fu X, Kong S, Chen J, Wang Z, Bai Z (2013) Chemical composition, mass closure and sources of atmospheric PM10 from industrial sites in Shenzhen, China. J Environ Sci 25(8):1626–1635. https://doi.org/10.1016/S1001-0742(12)60238-1
Xie Y, Liu Z, Wen T, Huang X, Liu J, Tang G, Yang Y, Li X, Shen R, Hu B, Wang Y (2019) Characteristics of chemical composition and seasonal variations of PM2.5 in Shijiazhuang, China: impact of primary emissions and secondary formation. Sci Total Environ 677:215–229. https://doi.org/10.1016/j.scitotenv.2019.04.300
Xu L, Duan F, He K, Ma Y, Zhu L, Zheng Y, Huang T, Kimoto T, Ma T, Li H, Ye S, Yang S, Sun Z, Xu B (2017) Characteristics of the secondary water-soluble ions in a typical autumn haze in Beijing. Environ Pollut 227:296–305. https://doi.org/10.1016/j.envpol.2017.04.076
Xue J, Griffith SM, Yu X, Lau AKH, Yu JZ (2014) Effect of nitrate and sulfate relative abundance in PM2.5 on liquid water content explored through half-hourly observations of inorganic soluble aerosols at a polluted receptor site. Atmos Environ 99:24–31. https://doi.org/10.1016/j.atmosenv.2014.09.049
Yang X, Cheng S, Li J, Lang J, Wang G (2017) Characterization of chemical composition in PM2.5 in Beijing before, during, and after a large-scale international event. Aerosol Air Qual Res 17(4): 896–907. https://doi.org/10.4209/aaqr.2016.07.0321
Yao L, Yang L, Yuan Q, Yan C, Dong C, Meng C, Sui X, Yang F, Lu Y, Wang W (2016) Sources apportionment of PM2.5 in a background site in the North China Plain. Sci Total Environ 541:590–598. https://doi.org/10.1016/j.scitotenv.2015.09.123
Ye S, Ma T, Duan F, Li H, He K, Xia J, Yang S, Zhu L, Ma Y, Huang T, Kimoto T (2019) Characteristics and formation mechanisms of winter haze in Changzhou, a highly polluted industrial city in the Yangtze River Delta, China. Environ Pollu 253:377–383. https://doi.org/10.1016/j.envpol.2019.07.011
Yin J and Harrison R M (2008) Pragmatic mass closure study for PM1.0, PM2.5 and PM10 at roadside, urban background and rural sites. Atmos Environ 42(5): 980–988. https://doi.org/10.1016/j.atmosenv.2007.10.005
Yu H, Zhao X, Wang J, Yin B, Geng C, Wang X, Gu C, Huang L, Yang W, Bai Z (2020) Chemical characteristics of road dust PM2.5 fraction in oasis cities at the margin of Tarim Basin. J Environ Sci 95:217–224. https://doi.org/10.1016/j.jes.2020.03.030
Zhang Y, Tang L, Yu H, Wang Z, Sun Y, Qin W, Chen W, Chen C, Ding A, Wu J, Ge S, Chen C, Zhou H (2015) Chemical composition, sources and evolution processes of aerosol at an urban site in Yangtze River Delta, China during wintertime. Atmos Environ 123:339–349. https://doi.org/10.1016/j.atmosenv.2015.08.017
Zhang R, Sun X, Shi A, Huang Y, Yan J, Nie T, Yan X, Li X (2018) Secondary inorganic aerosols formation during haze episodes at an urban site in Beijing, China. Atmos Environ 177:275–282. https://doi.org/10.1016/j.atmosenv.2017.12.031
Zhao N, Wang G, Li G, Lang J, Zhang H (2020) Air pollution episodes during the COVID-19 outbreak in the Beijing–Tianjin–Hebei region of China: an insight into the transport pathways and source distribution. Environ Pollut 267:115617. https://doi.org/10.1016/j.envpol.2020.115617
Zhong J, Zhang X, Dong Y, Wang Y, Liu C, Wang J, Zhang Y, Che H (2018) Feedback effects of boundary-layer meteorological factors on cumulative explosive growth of PM2.5 during winter heavy pollution episodes in Beijing from 2013 to 2016. Atmos Chem Phys 18(1):247–258. https://doi.org/10.5194/acp-18-247-2018
Zhou M, Jiang W, Gao W, Gao X, Ma M, Ma X (2021) Anthropogenic emission inventory of multiple air pollutants and their spatiotemporal variations in 2017 for the Shandong Province. China Environ Pollut 288:117666. https://doi.org/10.1016/j.envpol.2021.117666
Acknowledgements
The authors gratefully thank the staff from Zibo Eco-environmental Monitoring Center of Shandong Province.
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This study was funded by National Key R&D Program of China (2017YFC0212501), Fundamental Research Funds for the Central Universities (Nos. 2020YJSMT02), and Zibo Environmental Protection Bureau Program (ZDGL20160715).
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Samples were collected by Bo Xu. Sample analysis was performed by Jing Wang, Jian Wang, and Yinhong Ma. The first draft of the manuscript was written by Xueyan Zhao. The manuscript was edited and reviewed by Ruojie Zhao, Guangjie Zhao, Handong Liang, and Xianqing Li. Xianqing Li and Wen Yang acquired the funding. All authors read and approved the final manuscript.
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Zhao, X., Wang, J., Xu, B. et al. Causes of PM2.5 pollution in an air pollution transport channel city of northern China. Environ Sci Pollut Res 29, 23994–24009 (2022). https://doi.org/10.1007/s11356-021-17431-4
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DOI: https://doi.org/10.1007/s11356-021-17431-4