Abstract
Hourly measured PM2.5-bound species, gases, and meteorological data were analyzed by the PMF receptor model to quantify source contributions, and by the random forest to estimate decisive factors of variations of PM2.5, sulfur oxidation ratio (SOR), and nitrogen oxidation ratio (NOR) during different haze episodes. PM2.5 variation was influenced by CO (17%), SO2 (19%), NH3 (12%), O3 (10%), air pressure (P, 9.9%), and temperature (T, 10%) during the whole period. SOR was determined by SO2 (15%), temperature (T, 9.8%), relative humidity (RHU, 15%), and pondus hydrogenii (pH, 35%), and NOR was influenced by NOx (19%), O3 (14%), NH3 (13%), and RHU (15%). Three types of pollution episodes were captured. Process I was characterized by high CO (contributing 40% of PM2.5 concentration variation estimated by the random forest) due to coal combustion for heating during winter in northern China. According to the PMF, coal combustion (32%) and secondary sources (38%) were both the most important contributors in the first stage, and then, when the RHU increased to above 80%, the highest contribution was from secondary sources (40%). Process II was during the Spring Festival and was characterized by 8.8 μg m−3 firework contribution. High SO2 during this process, especially on the CNY’s Eve, was observed due to the firework displays, and SO2 gave a high contribution (24%) to PM2.5 variation. Process III showed high ions and high RHU in summer with sulfate and nitrate contributing 44% and 22%, respectively. Furthermore, meteorological parameters and NH3 play a key role on SOR and NOR.
Similar content being viewed by others
Data availability
All relevant data are within the manuscript and available from the corresponding author upon request.
References
Alastuey A, Querol X, Rodríguez S, Plana F, Lopez-Soler A, Ruiz C, Mantilla E (2004) Monitoring of atmospheric particulate matter around sources of secondary inorganic aerosol. Atmos Environ 38:4979–4992
Almetwally AA, Bin-Jumah M, Allam AA (2020) Ambient air pollution and its influence on human health and welfare: an overview. Environ Sci Pollut Res 27:24815–24830
Brimblecombe P, Spedding DJ (1972) Rate of solution of gaseous sulphur Dioxide at atmospheric concentrations. Nature 236:225
Chen Y, Xie S (2014) Characteristics and formation mechanism of a heavy air pollution episode caused by biomass burning in Chengdu, Southwest China. Sci Total Environ 473–474:507–517
Cheng YF, Zheng GJ, Wei C, Mu Q, Zheng B, Wang ZB, Gao M, Zhang Q, He KB, Carmichael G, Pöschl U, Su H (2016) Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China. Sci Adv 2:e1601530
Chow JC, Watson JG, Kuhns H, Etyemezian V, Lowenthal DH, Crow D, Kohl SD, Engelbrecht JP, Green MC (2004) Source profiles for industrial, mobile, and area sources in the Big Bend Regional Aerosol Visibility and Observational study. Chemosphere 54:185–208
Chen TQ, Guestrin C (2016) XGBoost: a scalable tree boosting system. In: Proceedings of the 22nd ACM SIGKDD International Conference on Knowledge Discovery and Data Mining, San Francisco, California, USA. 785-794. https://doi.org/10.1145/2939672.2939785
Dall'Osto M, Hellebust S, Healy RM, O'Connor IP, Kourtchev I, Sodeau JR, Ovadnevaite J, Ceburnis D, O'Dowd CD (2014) Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques. Sci Total Environ 493:197–208
Du QQ, Zhang CL, Mu YJ, Cheng Y, Zhang YY, Liu CT (2016) An important missing source of atmospheric carbonyl sulfide: domestic coal combustion. Geophys Res Lett 43:8720–8727
Eatough DJ, Grover BD, Woolwine WR, Eatough NL, Long R, Farber R (2008) Source apportionment of 1 h semi-continuous data during the 2005 Study of Organic Aerosols in Riverside (SOAR) using positive matrix factorization. Atmos Environ 42:2706–2719
Fuzzi S (1978) Study of iron(III) catalysed sulphur dioxide oxidation in aqueous solution over a wide range of pH. Atmos Environ 12:1439–1442
Fountoukis C, Nenes A (2007) ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+-Ca2+-Mg2+-NH4+-Na+-SO42−-NO3−-Cl−-H2O aerosols. Atmos Chem Phys 7:4639–4659
Guo H, Xu L, Bougiatioti A, Cerully KM, Capps SL, Hite JR Jr, Carlton AG, Lee SH, Bergin MH, Ng NL, Nenes A, Weber RJ (2015) Fine-particle water and pH in the southeastern United States. Atmos Chem Phys 15:5211–5228
Gao J, Peng X, Chen G, Xu J, Shi GL, Zhang YC, Feng YC (2016) Insights into the chemical characterization and sources of PM2.5 in Beijing at a 1-h time resolution. Sci. Total Environ 542:162–171
Guan L, Liang YL, Tian YZ, Yang ZR, Sun YM, Feng YC (2019) Quantitatively analyzing effects of meteorology and PM 2.5 sources on low visual distance. Sci. Total Environ 659:764–772
Han B, Zhang R, Yang W, Bai ZP, Ma ZQ, Zhang WJ (2016) Heavy haze episodes in Beijing during January 2013: inorganic ion chemistry and source analysis using highly time-resolved measurements from an urban site. Sci. Total Environ 544:319–329
Huang RJ, Zhang Y, Bozzetti C, Ho KF, Cao JJ, Han Y, Daellenbach KR, Slowik JG, Platt SM, Canonaco F, Zotter P, Wolf R, Pieber SM, Bruns EA, Crippa M, Ciarelli G, Piazzalunga A, Schwikowski M, Abbaszade G, Schnelle-Kreis J, Zimmermann R, An Z, Szidat S, Baltensperger U, Haddad I, Prévôt ASH (2014) High secondary aerosol contribution to particulate pollution during haze events in China. Nature 514:218–222
Jerrett M, Turner MC, Beckerman BS, Pope CA, van Donkelaar A, Martin RV, Serre M, Crouse D, Gapstur SM, Krewski D (2017) Comparing the health effects of ambient particulate matter estimated using ground-based versus remote sensing exposure estimates. Environ. Health Perspect 125:552–559
Kulshrestha UC, Saxena A, Kumar N, Kumari KM, Srivastava SS (1998) Chemical composition and association of size-differentiated aerosols at a suburban site in a semi-arid tract of India. J Atmos Chem 29:109–118
Kuwata M, Kai FM, Yang LDQ, Itoh M, Gunawan H, Harvey CF (2017) Temperature and burning history affect emissions of greenhouse gases and aerosol particles from tropical peatland fire. J Geophys Res-Atmos 122:1281–1292
Kota SH, Zhang HL, Chen G, Schade GW, Ying Q (2014) Evaluation of on-road vehicle CO and NOx national emission inventories using an urban-scale source-oriented air quality model. Atmos Environ 85:99–108
Karimian H, Li Q, Li CC, Chen G, Mo YQ, Wu CL, Fan JX (2019) Spatio-temporal variation of wind influence on distribution of fine particulate matter and its precursor gases. Atmos Pollut Res 10:53–64
Li YJ, Wang JH, Ren BN, Wang HL, Qiao LP, Zhu JP, Li L (2018) The characteristics of atmospheric phthalates in Shanghai: a haze case study and human exposure assessment. Atmos Environ 178:80–86
Luo J, Du P, Samat A, Xia J, Che M, Xue Z (2017) Spatiotemporal pattern of PM2.5 concentrations in Mainland China and analysis of its influencing factors using geographically weighted regression. Sci Rep 7:40607
Li JY, Xu TT, Liu XH, Chen H, Nizkorodov SA, Chen JM, Yang X, Mo ZY, Chen ZM, Liu HL, Mao JY, Liang GY (2017) Online single particle measurement of fireworks pollution during Chinese New Year in Nanning. J Environ Sci 53:184–195
Liu B, Li TK, Yang JM, Wu JH, Wang J, Gao JX, Bi XH, Feng YC, Zhang YF, Yang HH (2017) Source apportionment and a novel approach of estimating regional contributions to ambient PM2.5 in Haikou, China. Environ Pollut 223:334–345
Manigrasso M, Abballe F, Jack RF, Avino P (2010) Time-resolved measurement of the ionic fraction of atmospheric fine particulate matter. J Chromatogr Sci 48:549–552
Meng ZY, Lin WL, Jiang XM, Yan P, Wang Y, Zhang YM, Jia XF, Yu XL (2011) Characteristics of atmospheric ammonia over Beijing, China. Atmos Chem Phys 11:6139–6151
Notario A, Bravo I, Adame JA, Díaz-de-Mera Y, Aranda A, Rodríguez A, Rodríguez D (2013) Behaviour and variability of local and regional oxidant levels (OX = O3 + NO2) measured in a polluted area in central-southern of Iberian Peninsula. Environ Sci Pollut Res 20:188–200
Norris GA, Duvall R, Brown SG, Bai S (2014) EPA Positive Matrix Factorization (PMF) 5.0 Fundamentals and User Guide. Prepared for the, U.S. Environmental Protection Agency Office of Research and Development, Washington, DC (EPA/600/R-14/108; STI910511-5594-UG, April).
Ogulei D, Hopke PK, Zhou L, Pancras JP, Nair N, Ondov JM (2006) Source apportionment of Baltimore aerosol from combined size distribution and chemical composition data. Atmos Environ 40:396–410
Paatero P (1997) Least squares formulation of robust non-negative factor analysis. Chemom Intell Lab Syst 37:23–35
Paatero P, Tapper U (1994) Positive matrix factorization: a non-negative factor model with optimal utilization of error estimates of data values. Environmetrics 5:111–126
Pancras JP, Landis MS, Norris GA, Vedantham R, Dvonch JT (2013) Source apportionment of ambient fine particulate matter in Dearborn, Michigan, using hourly resolved PM chemical composition data. Sci Total Environ 448:2–13
Sarkar S, Khillare PS, Jyethi DS, Hasan A, Parween M (2010) Chemical speciation of respirable suspended particulate matter during a major firework festival in India. J Hazard Mater 184:321–330
Schelden VG, de Foy B, Herring C, Kaspari S, VanReken T, Jobson B (2017) Contributions of wood smoke and vehicle emissions to ambient concentrations of volatile organic compounds and particulate matter during the Yakima wintertime nitrate study. J Geophys Res Atmos 122:1871–1883
Svetnik V, Liaw A, Tong C, Culberson JC, Sheridan RP, Feuston BP (2003) Random Forest: A Classification and Regression Tool for Compound Classification and QSAR Modeling. J Chem Inf Comput Sci 43:1947–1958
Song S, Gao M, Xu W, Shao J, Shi G, Wang S, Wang Y, Sun Y, McElroy MB (2018) Fine-particle pH for Beijing winter haze as inferred from different thermodynamic equilibrium models. Atmos Chem Phys 18:7423–7438
Sakamoto K, Takada H, Sekiguchi K (2004) Influence of ozone, relative humidity, and flow rate on the deposition and oxidation of sulfur dioxide on yellow sand. Atmos Environ 38:6961–6967
Seinfeld JH, Pandis SN (1998) From Air Pollution to Climate Change. Wiley, New York
Shen ZH, Cao JJ, Arimoto R, Han YM, Zhu CS, Tian J, Liu SX (2010) Chemical Characteristics of Fine Particles (PM1) from Xi’an, China. Aerosol Sci Technol 44(6):461–472
Shen ZH, Cao JJ, Liu SX, Zhu CS, Wang X, Zhang T, Xu HM, Hu TF (2011) Chemical composition of PM10 and PM2.5 collected at ground level and 100 meters during a strong winter-time pollution episode in Xi’an, China. J Air Waste Manage Assoc 61(11):1150–1159
Tian YZ, Liu JY, Han SQ, Shi XR, Shi GL, Xu H, Yu HF, Zhang YF, Feng YC, Russell AG (2018a) Spatial, seasonal and diurnal patterns in physicochemical characteristics and sources of PM2.5 in both inland and coastal regions within a megacity in China. J Hazard Mater 342:139–149
Tiwari S, Srivastava AK, Bisht DS, Safai PD, Parmita P (2013) Assessment of carbonaceous aerosol over Delhi in the Indo-Gangetic Basin: characterization, sources and temporal variability. Nat Hazards 65:1745–1764
Tian YZ, Wang J, Peng X, Shi GL, Feng YC (2014) Estimation of the direct and indirect impacts of fireworks on the physicochemical characteristics of atmospheric PM10 and PM2.5. Atmos Chem Phys 14:9469–9479
Tian YZ, Xue QQ, Xiao ZM, Chen K, Feng YC (2018b) PMF-GAS Methods to estimate contributions of sources and oxygen for PM2.5, based on highly time-resolved PM2.5 species and gas data. Aerosol Air Qual Res 18:2956–2966
Trivedi DK, Ali K, Beig G (2014) Impact of meteorological parameters on the development of fine and coarse particles over Delhi. Sci Total Environ 478:175–183
Tian YZ, Zhang YF, Liang YL, Niu ZB, Xue QQ, Feng YC (2020) PM2.5 source apportionment during severe haze episodes in a Chinese megacity based on a 5-month period by using hourly species measurements: explore how to better conduct PMF during haze episodes. Atmos Environ 224:117364
U.S. Environmental Protection Agency (EPA), EPA Positive Matrix Factorization (PMF) 5.0 Fundamentals and User Guide, (2014) www.epa.gov.
Wang XQ, Wei W, Cheng SY, Zhang C, Duan WJ (2018) A monitoring-modeling approach to SO42− and NO3− secondary conversion ratio estimation during haze periods in Beijing, China. J Environ Sci 78:293–302
Wang S, Liao TT, Wang LL, Sun Y (2016) Process analysis of characteristics of the boundary layer during a heavy haze pollution episode in an inland megacity, China. J Environ Sci 40:138–144
Wang GH, Cheng CL, Huang Y, Tao J, Ren YQ, Wu F, Meng JJ, Li JJ, Cheng YT, Cao JJ, Liu SX, Zhang T, Zhang R, Chen YB (2014a) Evolution of aerosol chemistry in Xi’an, inland China, during the dust storm period of 2013 – Part 1: Sources, chemical forms and formation mechanisms of nitrate and sulfate. Atmos Chem Phys 14:11571–11585
Wang SB, Yin SS, Zhang RQ, Yang LM, Zhao QY, Zhang LS, Yan QS, Jiang N, Tang XY (2019a) 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
Wang ZF, Li J, Wang Z, Yang WY, Tang X, Ge BZ, Yan PZ, Zhu LL, Chen XS, Chen HS, Wand W, Li JJ, Liu B, Wang XY, Zhao YL, Lu N, Su DB (2014b) Modeling study of regional severe hazes over mid-eastern China in January 2013 and its implications on pollution prevention and control. Sci China Earth Sci 57:3–13
Wang SX, Wei W, Li D, Aunan K, Hao JM (2010) Air pollutants in rural homes in Guizhou, China – Concentrations, speciation, and size distribution. Atmos Environ 44:4575–4581
Wang Y, Zhuang GS, Xu C, An ZS (2007) The air pollution caused by the burning of fireworks during the lantern festival in Beijing. Atmos Environ 41:417–431
Wang XQ, Wei W, Cheng SY, Yao S, Zhang HY, Zhang C (2019b) Characteristics of PM2.5 and SNA components and meteorological factors impact on air pollution through 2013–2017 in Beijing, China. Atmos. Pollut. Res 10:1976–1984
Wu JM, Zhang YJ, Wang T, Qian YL (2020) Rapid improvement in air quality due to aerosol-pollution control during 2012–2018: an evidence observed in Kunshan in the Yangtze River Delta, China. Atmos Pollut Res 11:693–701
Wu P, Huang XJ, Zhang JK, Luo B, Luo JQ, Song HY, Zhang W, Rao ZH, Feng YP, Zhang JQ (2019) Characteristics and formation mechanisms of autumn haze pollution in Chengdu based on high time-resolved water-soluble ion analysis. Environ Sci Pollut Res 26:2649–2661
Xie YZ, Liu ZR, Wen TX, Huang XJ, Liu JY, Tang GQ, Yang Y, Li XG, Shen RR, Hu B, Wang YS (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
Xie SD, Yu T, Zhang YH, Zeng LM, Qi L, Tang XY (2005) Characteristics of PM10, SO2, NOx and O3 in ambient air during the dust storm period in Beijing. Sci Total Environ 345:153–164
Yao L, Garmash O, Bianchi F, Zheng J, Yan C, Kontkanen J, Junninen H, Mazon SB, Ehn M, Paasonen P, Sipilä M, Wang MY, Wang XK, Xiao S, Chen HF, Lu YQ, Zhang BW, Wang DF, Fu QY, Geng FH, Li L, Wang HL, Qiao LP, Yang X, Chen JM, Kerminen VM, Petäjä T, Worsnop DW, Kulmala M, Wang L (2018) Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity. Science 361:278–281
Yao Q, Liu ZR, Han SQ, Cai ZY, Liu JL, Hao TY, Liu JY, Huang XJ, Wang YS (2020) Seasonal variation and secondary formation of size-segregated aerosol water-soluble inorganic ions in a coast megacity of North China Plain. Environ Sci Pollut Res 27:26750–26762
Zhang Q, Jiang X, Tong D, Davis SJ, Zhao H, Geng G, Feng T, Zheng B, Lu Z, Streets DG, Ni R, Brauer M, van Donkelaar A, Martin RV, Huo H, Liu Z, Pan D, Kan H, Yan Y, Lin J, He KB, Guan DB (2017) Transboundary health impacts of transported global air pollution and international trade. Nature 543:705–709
Zheng M, Zhao X, Cheng Y, Yan C, Shi W, Zhang X, Weber RJ, Schauer JJ, Wang X, Edgerton ES (2014) Sources of primary and secondary organic aerosol and their diurnal variations. J Hazard Mater 264:536–544
Zou YF, Wang YH, Zhang YZ, Koo JH (2017) Arctic sea ice, Eurasia snow, and extreme winter haze in China. Sci Adv 3:e1602751
Zhang H, Shen Z, Wei X, Zhang M, Li Z (2012) Comparison of optical properties of nitrate and sulfate aerosol and the direct radiative forcing due to nitrate in China. Atmos Res 113:113–125
Funding
This study is supported by the National Natural Science Foundation of China (91544226 and 41977181) and Tianjin Science and Technology Program (18ZXSZSF00160).
Author information
Authors and Affiliations
Contributions
Junwei Yang, Zhimei Xiao, and Kui Chen performed the experiments.
Xin Du made the figures. Xin Du and Yingze Tian wrote the paper. All the authors contributed to the submitted version of the manuscript. Yingze Tian and Yinchang Feng acquired the funding.
Corresponding authors
Ethics declarations
Ethical approval
Not applicable.
Consent to participate
All authors participated in this work.
Consent to publish
All authors agree to publish.
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Responsible Editor: Gerhard Lammel
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Du, X., Yang, J., Xiao, Z. et al. Source apportionment of PM2.5 during different haze episodes by PMF and random forest method based on hourly measured atmospheric pollutant. Environ Sci Pollut Res 28, 66978–66989 (2021). https://doi.org/10.1007/s11356-021-14487-0
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-021-14487-0