广州地区大气棕色碳气溶胶光吸收特性
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摘要
2014年冬季在广州番禺站利用校正后的7波段黑碳仪数据,计算棕色碳(BrC)在不同波长的光吸收特性,并结合气溶胶及气体成分在线监测仪(MARGA)和在线OCEC分析仪同步观测数据,分析了BrC的来源.结果表明:BrC在370、470、520、590和660 nm处对光吸收的贡献随波长增大而变小,不同波段的贡献分别为25. 9%、19. 7%、14. 1%、11. 6%和7. 7%; BrC光吸收系数、水溶性钾离子(K~+)和有机碳(OC)浓度大致呈现日间低,夜间高的趋势,说明生物质燃烧产物对BrC的光吸收系数贡献很大,傍晚附近农村地区逐渐活跃的秸秆燃烧活动和夜间稳定的边界层也有利于污染物累积; BrC光吸收系数与OC的比值在午后出现低值,说明二次有机气溶胶和老化的气溶胶的吸光能力较弱.相关性分析表明,BrC光吸收系数与K+离子和OC浓度的相关性最高,BrC光吸收系数与硝酸根(NO_3~-)和铵根(NH_4~+)离子也具有较高的相关性.
In this work,we conducted measurements using a seven-wavelength aethalometer,an online OCEC analyzer,and a MARGA to investigate brown carbon( Br C) absorption properties and source origins during the winter of 2014 at Panyu station,Guangzhou. The results showed that the average absorption contributions of Br C decreased with an increase in wavelength,measured as 25. 9%,19. 7%,14. 1%,11. 6%,and 7. 7% at 370 nm,470 nm,520 nm,590 nm,and 660 nm,respectively. Diurnal variations in Br C absorption and the concentrations of potassium cations( K+) and organic carbon( OC) was high at night and low during the day,which was attributed to biomass burning. This indicated that Br C was emitted from straw burning in rural areas and accumulated in the steady planetary boundary layer at night. Diurnal variations in the ratio of Br C absorption to OC concentrations showed a distinct dip during the afternoon,indicating that aged aerosol and secondary organic aerosol( SOA) had a weaker Br C absorption capacity. There was a good overall correlation between Br C absorption and K+concentrations. Br C absorption was also moderately related to the concentrations of ammonium cations( NH_4~+) and nitrate anions( NO_3~-).
In this work,we conducted measurements using a seven-wavelength aethalometer,an online OCEC analyzer,and a MARGA to investigate brown carbon( Br C) absorption properties and source origins during the winter of 2014 at Panyu station,Guangzhou. The results showed that the average absorption contributions of Br C decreased with an increase in wavelength,measured as 25. 9%,19. 7%,14. 1%,11. 6%,and 7. 7% at 370 nm,470 nm,520 nm,590 nm,and 660 nm,respectively. Diurnal variations in Br C absorption and the concentrations of potassium cations( K+) and organic carbon( OC) was high at night and low during the day,which was attributed to biomass burning. This indicated that Br C was emitted from straw burning in rural areas and accumulated in the steady planetary boundary layer at night. Diurnal variations in the ratio of Br C absorption to OC concentrations showed a distinct dip during the afternoon,indicating that aged aerosol and secondary organic aerosol( SOA) had a weaker Br C absorption capacity. There was a good overall correlation between Br C absorption and K+concentrations. Br C absorption was also moderately related to the concentrations of ammonium cations( NH_4~+) and nitrate anions( NO_3~-).
引文
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[26] Segura S,Estellés V,Titos G,et al. Determination and analysis of in situ spectral aerosol optical properties by a multiinstrumental approach[J]. Atmospheric Measurement Techniques,2014,7(8):2373-2387.
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[29]王鑫彤,鞠法帅,韩德文,等.大气颗粒物中生物质燃烧示踪化合物的研究进展[J].环境化学,2015,34(10):1885-1894.Wang X T,Ju F S,Han D W,et al. Research progress on the organic tracers of biomass burning in atmospheric aerosols[J].Environmental Chemistry,2015,34(10):1885-1894.
[30] Satish R, Shamjad P, Thamban N, et al. Temporal characteristics of brown carbon over the central Indo-Gangetic Plain[J]. Environmental Science&Technology,2017,51(12):6765-6772.
[31] Pio C A,Legrand M,Alves C A,et al. Chemical composition of atmospheric aerosols during the 2003 summer intense forest fire period[J]. Atmospheric Environment,2008,42(32):7530-7543.
[32]吕文英,徐海娟,王新明.广州城区秋季大气PM2. 5中主要水溶性无机离子分析[J].环境科学与技术,2010,33(1):98-101.Lv W Y,Xu H J,Wang X M. Major inorganic water-soluble ions in fine particles collected in autumn in urban Guangzhou[J].Environmental Science&Technology,2010,33(1):98-101.
[33] Wang J P,Nie W,Cheng Y F,et al. Light absorption of brown carbon in eastern China based on 3-year multi-wavelength aerosol optical property observations and an improved absorptionngstrm exponent segregation method[J]. Atmospheric Chemistry and Physics,2018,18(12):9061-9074.
[34] Shen Z X,Zhang Q,Cao J J,et al. Optical properties and possible sources of brown carbon in PM2. 5over Xi'an,China[J].Atmospheric Environment,2017,150:322-330.
[35] Elliott E M,Kendall C,Boyer E W,et al. Dual nitrate isotopes in dry deposition:utility for partitioning NOxsource contributions to landscape nitrogen deposition[J]. Journal of Geophysical Research:Biogeosciences,2009,114(G4):G04020.
[2] Koch D,Bond T C,Streets D,et al. Global impacts of aerosols from particular source regions and sectors[J]. Journal of Geophysical Research:Atmospheres, 2007, 112(D2):D02205.
[3] Kirchstetter T W,Novakov T,Hobbs P V. Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon[J]. Journal of Geophysical Research:Atmospheres,2004,109(D21):D21208.
[4]闫才青,郑玫,张远航.大气棕色碳的研究进展与方向[J].环境科学,2014,35(11):4404-4414.Yan C Q, Zheng M, Zhang Y H. Research progress and direction of atmospheric brown carbon[J]. Environmental Science,2014,35(11):4404-4414.
[5] Cheng Y,He K B,Zheng M,et al. Mass absorption efficiency of elemental carbon and water-soluble organic carbon in Beijing,China[J]. Atmospheric Chemistry and Physics,2011,11(22):11497-11510.
[6] Bond T C,Bussemer M,Wehner B,et al. Light Absorption by primary particle emissions from a lignite burning plant[J].Environmental Science&Technology,1999,33(21):3887-3891.
[7] Desyaterik Y,Sun Y L,Shen X H,et al. Speciation of"brown"carbon in cloud water impacted by agricultural biomass burning in eastern China[J]. Journal of Geophysical Research:Atmospheres,2013,118(13):7389-7399.
[8] Laskin A,Laskin J,Nizkorodov S A. Chemistry of atmospheric brown carbon[J]. Chemical Reviews,2015,115(10):4335-4382.
[9] Lack D A,Langridge J M. On the attribution of black and brown carbon light absorption using thengstrm exponent[J].Atmospheric Chemistry and Physics,2013,13(20):10535-10543.
[10] Lack D A,Cappa C D. Impact of brown and clear carbon on light absorption enhancement, single scatter albedo and absorption wavelength dependence of black carbon[J]. Atmospheric Chemistry and Physics,2010,10(9):4207-4220.
[11] Hecobian A,Zhang X,Zheng M,et al. Water-soluble organic aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States[J].Atmospheric Chemistry and Physics,2010,10(13):5965-5977.
[12] Hoffer A,Gelencsér A,Guyon P,et al. Optical properties of Humic-like substances(HULIS)in biomass-burning aerosols[J]. Atmospheric Chemistry and Physics,2006,6(11):3563-3570.
[13]黄聪聪,马嫣,郑军.南京冬季气溶胶光学特性及黑碳光吸收增强效应[J].环境科学,2018,39(7):3057-3066.Huang C C,Ma Y,Zheng J. Aerosol optical properties and light absorption enhancement of EC during wintertime in Nanjing[J].Environmental Science,2018,39(7):3057-3066.
[14] Olson M R,Garcia M V,Robinson M A,et al. Investigation of black and brown carbon multiple-wavelength-dependent light absorption from biomass and fossil fuel combustion source emissions[J]. Journal of Geophysical Research:Atmospheres,2015,120(13):6682-6697.
[15] Washenfelder R A,Attwood A R,Brock C A,et al. Biomass burning dominates brown carbon absorption in the rural southeastern United States[J]. Geophysical Research Letters,2015,42(2):653-664.
[16] Yuan J F,Huang X F,Cao L M,et al. Light absorption of brown carbon aerosol in the PRD region of China[J].Atmospheric Chemistry and Physics,2016,16(3):1433-1443.
[17] Chan C K,Yao X H. Air pollution in mega cities in China[J].Atmospheric Environment,2008,42(1):1-42.
[18] Huang R J,Zhang Y L,Bozzetti C,et al. High secondary aerosol contribution to particulate pollution during haze events in China[J]. Nature,2014,514(7521):218-222.
[19] Wu C,Wu D,Yu J Z. Quantifying black carbon light absorption enhancement with a novel statistical approach[J]. Atmospheric Chemistry and Physics,2018,18(1):289-309.
[20] Qin Y M,Tan H B,Li Y J,et al. Chemical characteristics of brown carbon in atmospheric particles at a suburban site near Guangzhou,China[J]. Atmospheric Chemistry and Physics,2018,18(22):16409-16418.
[21] Weingartner E,Saathoff H,Schnaiter M,et al. Absorption of light by soot particles:determination of the absorption coefficient by means of aethalometers[J]. Journal of Aerosol Science,2003,34(10):1445-1463.
[22] Coen M C,Weingartner E,Apituley A,et al. Minimizing light absorption measurement artifacts of the Aethalometer:evaluation of five correction algorithms[J]. Atmospheric Measurement Techniques,2010,3(2):457-474.
[23] Drinovec L,Moˇc nik G,Zotter P,et al. The “dual-spot”Aethalometer:an improved measurement of aerosol black carbon with real-time loading compensation[J]. Atmospheric Measurement Techniques,2015,8(5):1965-1979.
[24] Wu D,Wu C,Liao B,et al. Black carbon over the South China Sea and in various continental locations in South China[J].Atmospheric Chemistry and Physics,2013,13(24):12257-12270.
[25] Wu D,Mao J T,Deng X J,et al. Black carbon aerosols and their radiative properties in the Pearl River Delta region[J].Science in China Series D:Earth Sciences,2009,52(8):1152-1163.
[26] Segura S,Estellés V,Titos G,et al. Determination and analysis of in situ spectral aerosol optical properties by a multiinstrumental approach[J]. Atmospheric Measurement Techniques,2014,7(8):2373-2387.
[27] Bodhaine B A. Aerosol absorption measurements at Barrow,Mauna Loa and the south pole[J]. Journal of Geophysical Research:Atmospheres,1995,100(D5):8967-8975.
[28] Yang M,Howell S G,Zhuang J,et al. Attribution of aerosol light absorption to black carbon,brown carbon,and dust in China-interpretations of atmospheric measurements during EAST-AIRE[J]. Atmospheric Chemistry and Physics Discussions,2009,8(3):10913-10954.
[29]王鑫彤,鞠法帅,韩德文,等.大气颗粒物中生物质燃烧示踪化合物的研究进展[J].环境化学,2015,34(10):1885-1894.Wang X T,Ju F S,Han D W,et al. Research progress on the organic tracers of biomass burning in atmospheric aerosols[J].Environmental Chemistry,2015,34(10):1885-1894.
[30] Satish R, Shamjad P, Thamban N, et al. Temporal characteristics of brown carbon over the central Indo-Gangetic Plain[J]. Environmental Science&Technology,2017,51(12):6765-6772.
[31] Pio C A,Legrand M,Alves C A,et al. Chemical composition of atmospheric aerosols during the 2003 summer intense forest fire period[J]. Atmospheric Environment,2008,42(32):7530-7543.
[32]吕文英,徐海娟,王新明.广州城区秋季大气PM2. 5中主要水溶性无机离子分析[J].环境科学与技术,2010,33(1):98-101.Lv W Y,Xu H J,Wang X M. Major inorganic water-soluble ions in fine particles collected in autumn in urban Guangzhou[J].Environmental Science&Technology,2010,33(1):98-101.
[33] Wang J P,Nie W,Cheng Y F,et al. Light absorption of brown carbon in eastern China based on 3-year multi-wavelength aerosol optical property observations and an improved absorptionngstrm exponent segregation method[J]. Atmospheric Chemistry and Physics,2018,18(12):9061-9074.
[34] Shen Z X,Zhang Q,Cao J J,et al. Optical properties and possible sources of brown carbon in PM2. 5over Xi'an,China[J].Atmospheric Environment,2017,150:322-330.
[35] Elliott E M,Kendall C,Boyer E W,et al. Dual nitrate isotopes in dry deposition:utility for partitioning NOxsource contributions to landscape nitrogen deposition[J]. Journal of Geophysical Research:Biogeosciences,2009,114(G4):G04020.