In order to test the improvement of source apportionment of PM2.5 using the ME-2 model on unconstrained PMF analyses, a total of 153 daily PM2.5 samples were collected continuously from September 10, 2017 to August 29, 2018 at an industrial site in northern Shenzhen. The concentrations of 31 chemical compositions were determined, 17 of which were selected for model iteration. The annual mean concentration of PM2.5 at the industrial site was 32.3μg/m3, and nine sources of PM2.5 were identified by a prior PMF run, which were secondary sulfate, secondary nitrate, aged sea salt, soil dust, industrial emissions, coal combustion, biomass burning, ship emissions and vehicle emissions. However, the apportionment with PMF yielded mixed factors. Based on the PMF results and priori information obtained, four constrained factor profiles were input into the ME-2 model as a rotational control technique for model simulation. Compared to the PMF solution, tracers were more concentrated in source profiles of ME-2 results, and the ME-2 iteration provided a more significant fitting for time series of tracer concentrations and corresponding source contributions. Secondary nitrate, aged sea salt and industrial emissions were overestimated by 9% to 51% in the PMF results, while secondary sulfate, coal combustion and biomass burning were underestimated by 19% to 40%. The ME-2 result was found to be more environmentally and statistically significant than that of PMF and it could provide a more accurate scientific basis for pollution prevention and control at the same time.
唐孝炎,张远航,邵敏.大气环境化学[M]. 北京:高等教育出版社, 2006:268-548. Tang X Y, Zhang Y H, Shao M. Atmospheric environmental chemistry[M]. Beijing:Higher Education Press, 2006:268-548.
[2]
郑玫,张延君,闫才青,等.中国PM2.5来源解析方法综述[J]. 北京大学学报(自然科学版), 2014,50(6):1141-1154. Zheng M, Zhang Y J, Yan C Q, et al. Review of PM2.5 source apportionment methods in China[J]. Acta Scientiarum Naturalium Universitatis Pekinensis, 2014,50(6):1141-1154.
[3]
Chow J C, Watson J G, Lowenthal D H, et al. PM10 source apportionment in California's San Joaquin valley[J]. Atmospheric Environment, 1992,26(18):3335-3354.
[4]
EPA. Tools and Databases for Air Research[EB/OL]. https://www.epa.gov/air-research/models-tools-and-databases-air-research.
[5]
袁鸣蔚,吴亦潇,牛志华,等.基于科技论文产出的源解析受体模型CMB、PMF比较综述[A].//2014中囯环境科学学会学术年会论文集(第六章)[C]. 北京:中国环境科学出版社, 2014:5021-5026. Yuan M W, Wu Y X, Niu Z H, et al. A comparative review of CMB and PMF models based on the output of scientific papers[A].//2014annual conference of Chinese Society For Environmental Sciences(chapter 6)[C]. Beijing:China Environmental Science Press, 2014:5021-5026.
[6]
Lee J H, Hopke P K. Apportioning sources of PM2.5 in St. Louis, MO using speciation trends network data[J]. Atmospheric Environment, 2006,40:360-377.
[7]
Hasheminassab S, Daher N, Ostro B D, et al. Long-term source apportionment of ambient fine particulate matter (PM2.5) in the Los Angeles Basin:A focus on emissions reduction from vehicular sources[J]. Environmental Pollution, 2014,193:54-64.
[8]
Crippa M, Canonaco F, Lanz V A, et al. Organic aerosol components derived from 25AMS data sets across Europe using a consistent ME-2based source apportionment approach[J]. Atmospheric Chemistry and Physics,14,12(2014-06-23), 2014,14(12):6159-6176.
[9]
Visser S, Slowik J G, Furger M, et al. Advanced source apportionment of size-resolved trace elements at multiple sites in London during winter[J]. Atmospheric Chemistry and Physics, 2015,15(19):11291-11309.
[10]
Elser M, Huang R J, Wolf R, et al. New insights into PM2.5 chemical composition and sources in two major cities in China during extreme haze events using aerosol mass spectrometry[J]. Atmospheric Chemistry & Physics Discussions, 2015,15(21):30127-30174.
[11]
Sturtz T M, Adar S D, Gould T, et al. Constrained Source Apportionment of Coarse Particulate Matter and Selected Trace Elements in Three Cities from the Multi-Ethnic Study of Atherosclerosis[J]. Atmospheric Environment, 2014,84(1):65-77.
[12]
Zhu Q, Huang X F, Cao L M, et al. Improved source apportionment of organic aerosols in complex urban air pollution using the multilinear engine (ME-2)[J]. Atmospheric Measurement Techniques, 2018, 11(2):1049-1060.
[13]
Sun Y, Xu W Q, Zhang Q, et al. Source apportionment of organic aerosol from 2-year highly time-resolved measurements by an aerosol chemical speciation monitor in Beijing, China[J]. Atmospheric Chemistry and Physics, 2018,18(12):8469-8489.
[14]
Xu J, Peng X, Guo C S, et al. Sediment PAH source apportionment in the Liaohe River using the ME2 approach:A comparison to the PMF model[J]. Science of the Total Environment, 2016,553:164-171.
[15]
Zhang Q, Shen Z, Ning Z, et al. Characteristics and source apportionment of winter black carbon aerosols in two Chinese megacities of Xi'an and Hong Kong[J]. Environmental Science and Pollution Research, 2018,25(11):33783-33793.
[16]
Liu B, Yang J, Jie Y, et al. Source apportionment of atmospheric pollutants based on the online data by using PMF and ME2 models at a megacity, China[J]. Atmospheric Research, 2017,185:22-31.
[17]
杨佳美,戴启立,刘保双,等.关中地区背景点位环境空气PM2.5来源解析与多模型结果对比[J]. 环境科学研究, 2017,30(2):184-192. Yang J M, Dai Q L, Liu B S, et al. Source apportionment of ambient PM2.5 at background sites in Guanzhong area, China:comparison of results obtained by multiple models[J]. Research of Environmental Sciences, 2017,30(2):184-192.
[18]
深圳人居委.省生态环境厅发布2018年环境空气质量状况深圳PM2.5浓度26微克/立方米,达到历史最优[EB/OL]. http://www.sznews.com/news/content/2019-01/21/content_21364040.htm. Ecology Environment Bureau of Shenzhen Municipality, Shenzhen's PM2.5 concentration reached a record low of 26mic-rograms per cubic meter in 2018, according to the provincial department of ecology and environment[EB/OL]. http://www.sznews.com/news/content/2019-01/21/content_21364040.htm.
[19]
张文新.中国大城市人口居住郊区化现状、问题与对策[J]. 人口学刊, 2003,39(3):15-20. Zhang W X. The status quo, problems and countermeasures of Suburbanization of people's residence in China's big cities[J]. Population Journal, 2003,39(3):15-20.
[20]
周甜,闫才青,李小滢,等.华北平原城乡夏季PM2.5组成特征及来源研究[J]. 中国环境科学, 2017,37(9):3227-3236. Zhou T, Yan C Q, Li X Y, et al. Chemical characteristics and sources of PM2.5 in urban and rural sitesinthe North China Plain during summer[J]. China Environmental Science, 2017,37(9):3227-3236.
[21]
He L Y, Huang X F, Xue L, et al. Submicron aerosol analysis and organic source apportionment in an urban atmosphere in Pearl River Delta of China using high-resolution aerosol mass spectrometry[J]. Journal of Geophysical Research Atmospheres, 2011,116(D12):D12304.
[22]
Huang X F, He L Y, Hu M, et al. Characterization of submicron aerosols at a rural site in Pearl River Delta of China using an Aerodyne High-Resolution Aerosol Mass Spectrometer[J]. Atmos. Chem. Phys., 2011,11(5):1865-1877.
[23]
Paatero P. Least squares formulation of robust non-negative factor analysis[J]. Chemometrics & Intelligent Laboratory Systems, 1997, 37(1):23-35.
[24]
Paatero P, Tapper U. Positive matrix factorization:A non-negative factor model with optimal utilization of error estimates of data values[J]. Environmetrics, 1994,5(2):111-126.
[25]
Paatero P, Hopke P K. Rotational tools for factor analytic models[J]. Journal of Chemometrics, 2010,23(2):91-100.
[26]
Canonaco F, Crippa M, Slowik J G, et al. SoFi, an IGOR-based interface for the efficient use of the generalized multilinear engine (ME-2) for the source apportionment:ME-2application to aerosol mass spectrometer data[J]. Atmospheric Measurement Techniques, 2013,6(12):3649-3661.
[27]
Polissar A V, Hopke P K, Paatero P, et al. Atmospheric aerosol over Alaska:2. Elemental composition and sources[J]. Journal of Geophysical Research Atmospheres, 1998,103(D15):19045-19057.
[28]
Jimenez J L, Canagaratna M R, Donahue N M, et al. Evolution of organic aerosols in the atmosphere[J]. Science, 2009,326(5959):1525-1529.
[29]
Yuan Z, Lau A K H, Zhang H, et al. Identification and spatiotemporal variations of dominant PM10 sources over Hong Kong[J]. Atmospheric Environment, 2006,40(10):1803-1815.
[30]
Choi M, Lee D, Choi J, et al. (239+240)Pu concentration and isotope ratio ((240)Pu/(239)Pu) in aerosols during high dust (Yellow Sand) period, Korea[J]. Science of the Total Environment, 2006,370:262-270.
[31]
Wang Q Q, Huang X H H, Zhang T, et al. Organic tracer-based source analysis of PM2.5 organic and elemental carbon:A case study at Dongguan in the Pearl River Delta, China[J]. Atmospheric Environment, 2015,118:164-175.
[32]
Yudovich Y E, Ketris M P. Chlorine in coal:A review[J]. International Journal of Coal Geology, 2006,67(1):127-144.
[33]
Márcia A Y, Artaxo P, Miguel A H, et al. Chemical composition of aerosol particles from direct emissions of vegetation fires in the Amazon Basin:water-soluble species and trace elements[J]. Atmospheric Environment, 2000,34(10):1641-1653.
[34]
Chow J, Watson J. Review of PM2.5 and PM10 Apportionment for Fossil Fuel Combustion and Other Sources by the Chemical Mass Balance Receptor Model[J]. Energy & Fuels, 2002,16:222-260.
[35]
Bohemen H D V, Janssen Van De Laak W H. The Influence of Road Infrastructure and Traffic on Soil, Water, and Air Quality[J]. Environmental Management, 2003,31(1):50-68.
[36]
Lanz V A, Alfarra M R, Baltensperger U, et al. Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra[J]. Atmospheric Chemistry and Physics, 2007,7(6):1503-1522.
[37]
Yuan Z B, Yu J Z, Lau A K H, et al. Application of positive matrix factorization in estimating aerosol secondary organic carbon in Hong Kong and its relationship with secondary sulfate[J]. Atmos. Chem. Phys., 2006,6(1):25-34.
[38]
Tao J, Zhang L, Cao J, et al. Source apportionment of PM2.5 at urban and suburban areas of the Pearl River Delta region, south China-With emphasis on ship emissions[J]. Science of The Total Environment, 2017,574:1559-1570.
[39]
Huang X F, Zou B B, He L Y, et al. Exploration of PM2.5 sources on the regional scale in the Pearl River Delta based on ME-2modeling[J]. Atmos. Chem. Phys., 2018,18(16):11563-11580.
[40]
Yuan Z B, Yu J Z, Lau A K H, et al. Application of positive matrix factorization in estimating aerosol secondary organic carbon in Hong Kong and insights into the formation mechanisms[J]. Atmospheric Chemistry & Physics, 2006,5(4):1015-1026.
[41]
黄晓锋,云慧,宫照恒,等.深圳大气PM2.5来源解析与二次有机气溶胶估算[J]. 中国科学:地球科学, 2014,44(4):723-734. Huang X F, Yun H, Gong Z H, et al. Source apportionment and secondary organic aerosol estimation of PM2.5in an urban atmosphere in China[J]. Science China(Earth Sciences), 2014,44(4):723-734.
[42]
Millero F J, Feistel R, Wright D G, et al. The composition of Standard Seawater and the definition of the Reference-Composition Salinity Scale[J]. Deep-Sea Research Part I (Oceanography Research Papers), 2008,55(1):50-72.
[43]
Huang X F, Yu J Z, He L Y, et al. Water-soluble organic carbon and oxalate in aerosols at a coastal urban site in China:Size distribution characteristics, sources, and formation mechanisms[J]. Journal of Geophysical Research Atmospheres, 2006,111(D22):D22212.
[44]
Taylor S R, Mclennan S M. The Geochemical Evolution of the Continental Crust[J]. Reviews of Geophysics, 1995,33(2):241-265.
