Determination of crustal element iron light absorption contribution and effects on black carbon light absorption enhancement estimation: a case study in Wuhan
TAN Jian1,2,3, XIA Rui1,2,3, WU Dui1,2,3, KONG Shao-fei4,5, CHEN Nan5,6, CHENG Chun-lei1,2,3, DENG Tao7, TAO Li-ping1,2,3, ZHANG Xue1,2,3, WU Bo-xi1,2,3, WU Liang-bin1,2,3, WANG Qing1,2,3, WU Cheng1,2,3
1. Institute of Mass Spectrometry and Atmospheric Environment, Jinan University, Guangzhou 510632, China; 2. Guangdong-Hongkong-Macau Joint Laboratory of Collaborative Innovation for Environmental Quality, Guangzhou 510632, China; 3. Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air Pollution, Guangzhou 510632, China; 4. School of Environmental Studies, China University of Geosciences(Wuhan), Wuhan 430074, China; 5. Research Centre for Complex Air Pollution of Hubei Province, Wuhan 430074, China; 6. Eco-Environmental Monitoring Centre of Hubei Province, Wuhan 430074, China; 7. Institute of Tropical and Marine Meteorology, China Meteorological Administration, Guangzhou 510640, China
Abstract：The traditional method uses empirical absorption Ångström exponent to estimate the light absorption of crustal elements or brown carbon, and this method can only handle the two components scenario (blackcarbon/brown carbon or blackcarbon/crustal elements), leading to substantial uncertainties. This study introduces a new method that uses the Fe as the crustal element tracer. Using measurement data in Wuhan (February, March, August, and September 2021) by applying the minimum R-squared method (MRS), the crustal elements light absorption contribution can be obtained. After subtracting the crustal elements light absorption, absorption enhancement factor (Eabs) can be obtained. The results showed that the average crustal elements absorption contribution at 370nm during the observation period was 12.3%, with a monthly average ranging from 5.7% to 15.5%. Meanwhile, AAE exhibited a positive dependence on the concentration of Fe. These collective clues indicate that the crustal elements absorption contribution cannot be ignored. Crustal elements light absorption demonstrated a considerable seasonality, which was low in winter and high in spring. There are deviations in the calculated Eabs before and after the separation of crustal elements light absorption, which is influenced by the correlation between blackcarbon and iron. During the observation period, after deducting the light absorption of crustal elements, the average Eabs was 1.43±0.53, and Eabs was high in spring and summer, and low in autumn and winter. HighEabs in spring was associated with a higher degree of BC aging. The analysis found that Eabs demonstrated a positive dependence on the content of inorganic salts and organic matters, which proves the influence of these coating materials on the enhancement of light absorption.
谭健, 夏瑞, 吴兑, 孔少飞, 陈楠, 成春雷, 邓涛, 陶丽萍, 张雪, 吴柏禧, 吴良斌, 王庆, 吴晟. 地壳元素铁的吸光贡献对黑碳吸光增强估算的影响——以武汉为例[J]. 中国环境科学, 2022, 42(7): 3033-3045.
TAN Jian, XIA Rui, WU Dui, KONG Shao-fei, CHEN Nan, CHENG Chun-lei, DENG Tao, TAO Li-ping, ZHANG Xue, WU Bo-xi, WU Liang-bin, WANG Qing, WU Cheng. Determination of crustal element iron light absorption contribution and effects on black carbon light absorption enhancement estimation: a case study in Wuhan. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(7): 3033-3045.
Wu D, Mao J T, Deng X J, et al. Black carbon aerosols and their radiative properties in the Pearl River Delta region[J]. Sci. China Ser. D., 2009,52(8):1152-1163.
[2]
Bond T C, Doherty S J, Fahey D W, et al. Bounding the role of black carbon in the climate system:A scientific assessment[J]. J. Geophys. Res., 2013,118(11):5380-5552.
[3]
Ding A J, Huang X, Nie W, et al. Enhanced haze pollution by black carbon in megacities in China[J]. Geophys. Res. Lett., 2016,43(6):2873-2879.
[4]
Yuan C, Zheng J, Ma Y, et al. Significant restructuring and light absorption enhancement of black carbon particles by ammonium nitrate coating[J]. Environ. Pollut., 2020,262:114172.
[5]
Schnaiter M, Linke C, Mohler O, et al. Absorption amplification of black carbon internally mixed with secondary organic aerosol[J]. J. Geophys. Res., 2005,110(D19):D19204.
[6]
Zhang R Y, Khalizov A F, Pagels J, et al. Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing[J]. Proc. Natl. Acad. Sci. USA, 2008,105(30):10291-10296.
[7]
Pei X, Hallquist M, Eriksson A C, et al. Morphological transformation of soot:investigation of microphysical processes during the condensation of sulfuric acid and limonene ozonolysis product vapors[J]. Atmos. Chem. Phys., 2018,18(13):9845-9860.
[8]
Liu S, Aiken A C, Gorkowski K, et al. Enhanced light absorption by mixed source black and brown carbon particles in UK winter[J]. Nat. Commun., 2015,6(1):8435.
[9]
Sun J Y, Wu C, Wu D, et al. Amplification of black carbon light absorption induced by atmospheric aging:temporal variation at seasonal and diel scales in urban Guangzhou[J]. Atmos. Chem. Phys., 2020,20(4):2445-2470.
[10]
Cappa C D, Onasch T B, Massoli P, et al. Radiative absorption enhancements due to the mixing state of atmospheric black carbon[J]. Science, 2012,337(6098):1078-1081.
[11]
Ueda S, Nakayama T, Taketani F, et al. Light absorption and morphological properties of soot-containing aerosols observed at an East Asian outflow site, Noto Peninsula, Japan[J]. Atmos. Chem. Phys., 2016,16(4):2525-2541.
[12]
Mbengue S, Zikova N, Schwarz J, et al. Mass absorption cross-section and absorption enhancement from long term black and elemental carbon measurements:A rural background station in Central Europe[J]. Sci. Total Environ., 2021,794:148365.
[13]
Fierce L, Bond T C, Bauer S E, et al. Black carbon absorption at the global scale is affected by particle-scale diversity in composition[J]. Nat. Commun., 2016,7:12361.
[14]
Matsui H, Hamilton D S, Mahowald N M. Black carbon radiative effects highly sensitive to emitted particle size when resolving mixing-state diversity[J]. Nat. Commun., 2018,9(1):3446.
[15]
Cappa C D, Zhang X, Russell L M, et al. Light absorption by ambient black and brown carbon and its dependence on black carbon coating state for two California, USA cities in winter and summer[J]. J. Geophys. Res., 2019,124(3):1550-1577.
[16]
Wu Y, Cheng T, Zheng L. Light absorption of black carbon aerosols strongly influenced by particle morphology distribution[J]. Environ. Res. Lett., 2020,15(9):094051.
[17]
Cui X, Wang X, Yang L, et al. Radiative absorption enhancement from coatings on black carbon aerosols[J]. Sci. Total Environ., 2016,551:51-56.
[18]
Zhang Y, Zhang Q, Cheng Y, et al. Amplification of light absorption of black carbon associated with air pollution[J]. Atmos. Chem. Phys., 2018,18(13):9879-9896.
[19]
Bai Z, Cui X, Wang X, et al. Light absorption of black carbon is doubled at Mt. Tai and typical urban area in North China[J]. Sci. Total Environ., 2018,635:1144-1151.
[20]
Cui F, Chen M, Ma Y, et al. An intensive study on aerosol optical properties and affecting factors in Nanjing, China[J]. Journal of Environmental Sciences, 2016,40:35-43.
[21]
Chen D, Zhao Y, Lyu R, et al. Seasonal and spatial variations of optical properties of light absorbing carbon and its influencing factors in a typical polluted city in Yangtze River Delta, China[J]. Atmos. Environ., 2019,199:45-54.
[22]
Ma Y, Huang C, Jabbour H, et al. Mixing state and light absorption enhancement of black carbon aerosols in summertime Nanjing, China[J]. Atmos. Environ., 2020,222:117141.
[23]
孙嘉胤,吴晟,吴兑,等.广州城区黑碳气溶胶吸光增强特性研究[J].中国环境科学, 2020,40(10):4177-4189. Sun J Y, Wu C, Wu D, et al. The light absorbtion enhancement characteristics of black carbon aerosols in urban Guangzhou[J]. China Environmental Science, 2020,40(10):4177-4189.
[24]
Fu Y, Peng X, Guo Z, et al. Filter-based absorption enhancement measurement for internally mixed black carbon particles over southern China[J]. Sci. Total Environ., 2021,762:144194.
[25]
Mian C, Diehl T, Dubovik O, et al. Light absorption by pollution, dust, and biomass burning aerosols:a global model study and evaluation with AERONET measurements[J]. Ann. Geophys., 2009,27(9):3439-3464.
[26]
Wu X, Liu J, Wu Y, et al. Aerosol optical absorption coefficients at a rural site in Northwest China:The great contribution of dust particles[J]. Atmos. Environ., 2018,189:145-152.
[27]
Sun J, Zhang M, Liu T. Spatial and temporal characteristics of dust storms in China and its surrounding regions, 1960-1999:Relations to source area and climate[J]. J. Geophys. Res., 2001,106(D10):10325-10333.
[28]
吴兑,吴晟,李菲,等.粗粒子气溶胶远距离输送造成华南严重空气污染的分析[J].中国环境科学, 2011,31(4):540-545. Wu D, Wu C, Li F, et al. Air pollution episode in southern China due to the long range transport of coarse particle aerosol[J]. China Environmental Science, 2011,31(4):540-545.
[29]
Casotti Rienda I, Alves C A. Road dust resuspension:A review[J]. Atmos. Res., 2021,261:105740.
[30]
Xie C, He Y, Lei L, et al. Contrasting mixing state of black carboncontaining particles in summer and winter in Beijing[J]. Environ. Pollut., 2020,263:114455.
[31]
Wu C, Wu D, Yu J Z. Estimation and uncertainty analysis of secondary organic carbon using one-year of hourly organic and elemental carbon data[J]. J. Geophys. Res., 2019,124(5):2774-2795.
[32]
程丁,吴晟,吴兑,等.深圳市城区和郊区黑碳气溶胶对比研究[J].中国环境科学, 2018,38(5):1653-1662. Cheng D, Wu C, Wu D, et al. Comparative study on the characteristics of black carbon aerosol in urban and suburban areas of Shenzhen[J]. China Environmental Science, 2018,38(5):1653-1662.
[33]
Weingartner E, Saathoff H, Schnaiter M, et al. Absorption of light by soot particles:determination of the absorption coefficient by means of aethalometers[J]. J. Aerosol Sci., 2003,34(10):1445-1463.
[34]
Wu C, Wu D, Yu J Z. Quantifying black carbon light absorption enhancement with a novel statistical approach[J]. Atmos. Chem. Phys., 2018,18(1):289-309.
[35]
Wang Q, Han Y, Ye J, et al. High Contribution of secondary brown carbon to aerosol light absorption in the southeastern margin of Tibetan Plateau[J]. Geophys. Res. Lett., 2019,46(9):4962-4970.
[36]
Turpin B J, Huntzicker J J. Secondary formation of organic aerosol in the Los-Angeles Basin-a descriptive analysis of organic and elemental carbon concentrations[J]. Atmos. Environ., 1991,25(2):207-215.
[37]
Millet D B, Donahue N M, Pandis S N, et al. Atmospheric volatile organic compound measurements during the Pittsburgh Air Quality Study:Results, interpretation, and quantification of primary and secondary contributions[J]. J. Geophys. Res., 2005,110(D7):D07S.
[38]
Wu C, Yu J Z. Determination of primary combustion source organic carbon-to-elemental carbon (OC/EC) ratio using ambient OC and EC measurements:secondary OC-EC correlation minimization method[J]. Atmos. Chem. Phys., 2016,16(8):5453-5465.
[39]
Alfaro S C, Lafon S, Rajot J L, et al. Iron oxides and light absorption by pure desert dust:An experimental study[J]. J. Geophys. Res., 2004,109(D8):D08208.
[40]
Hu W W, Hu M, Deng Z Q, et al. The characteristics and origins of carbonaceous aerosol at a rural site of PRD in summer of 2006[J]. Atmos. Chem. Phys., 2012,12(4):1811-1822.
[41]
Wu C, Yu J Z. Evaluation of linear regression techniques for atmospheric applications:the importance of appropriate weighting[J]. Atmos. Meas. Tech., 2018,11(2):1233-1250.
[42]
Zhang Y L, Cao F. Fine particulate matter (PM2.5) in China at a city level[J]. Sci. Rep., 2015,5(1):1-12.
[43]
Huang T, Chen J, Zhao W, et al. Seasonal variations and correlation analysis of water-soluble inorganic ions in PM2.5 in Wuhan, 2013[J]. Atmosphere, 2016,7(4):49.
[44]
Zheng H, Kong S, Zheng M, et al. A 5.5-year observations of black carbon aerosol at a megacity in Central China:Levels, sources, and variation trends[J]. Atmos. Environ., 2020,232:117581.
[45]
Xu Q, Wang S, Jiang J, et al. Nitrate dominates the chemical composition of PM2.5 during haze event in Beijing, China[J]. Sci Total Environ, 2019,689:1293-1303.
[46]
Zhang Y, Vu T V, Sun J, et al. Significant changes in chemistry of fine particles in wintertime Beijing from 2007 to 2017:Impact of Clean Air Actions[J]. Environ. Sci. Technol., 2020,54(3):1344-1352.
[47]
Liu S C. Possible effects on tropospheric O3 and OH due to No emissions[J]. Geophys. Res. Lett., 1977,4(8):325-328.
[48]
Canonaco F, Slowik J G, Baltensperger U, et al. Seasonal differences in oxygenated organic aerosol composition:implications for emissions sources and factor analysis[J]. Atmos. Chem. Phys., 2015,15(12):6993-7002.
[49]
Ji D, Zhang J, He J, et al. Characteristics of atmospheric organic and elemental carbon aerosols in urban Beijing, China[J]. Atmos. Environ., 2016,125:293-306.
[50]
Wu C, Huang X H H, Ng W M, et al. Inter-comparison of NIOSH and IMPROVE protocols for OC and EC determination:implications for inter-protocol data conversion[J]. Atmos. Meas. Tech., 2016,9(9):4547-4560.
[51]
Yao L, Huo J, Wang D, et al. Online measurement of carbonaceous aerosols in suburban Shanghai during winter over a three-year period:Temporal variations, meteorological effects, and sources[J]. Atmos. Environ., 2020,226:117408.
[52]
Bressi M, Sciare J, Ghersi V, et al. A one-year comprehensive chemical characterisation of fine aerosol (PM2.5) at urban, suburban and rural background sites in the region of Paris (France)[J]. Atmos. Chem. Phys., 2013,13(15):7825-7844.
[53]
Blanchard C L, Shaw S L, Edgerton E S, et al. Ambient PM2.5 organic and elemental carbon in New York City:changing source contributions during a decade of large emission reductions[J]. J. Air Waste Manage Assoc., 2021,71(8):995-1012.
[54]
Ji D, Gao M, Maenhaut W, et al. The carbonaceous aerosol levels still remain a challenge in the Beijing-Tianjin-Hebei region of China:Insights from continuous high temporal resolution measurements in multiple cities[J]. Environ. Int., 2019,126:171-183.
[55]
Bond T C, Bergstrom R W. Light absorption by carbonaceous particles:An investigative review[J]. Aerosol Sci. Technol., 2006,40(1):27-67.
[56]
Xu X, Zhao W, Zhang Q, et al. Optical properties of atmospheric fine particles near Beijing during the HOPE-J3A campaign[J]. Atmos. Chem. Phys., 2016,16(10):6421-6439.
[57]
Xie C, Xu W, Wang J, et al. Light absorption enhancement of black carbon in urban Beijing in summer[J]. Atmos. Environ., 2019,213:499-504.
[58]
Sun J, Xie C, Xu W, et al. Light absorption of black carbon and brown carbon in winter in North China Plain:comparisons between urban and rural sites[J]. Sci. Total Environ., 2021,770:144821.
[59]
Chen B, Bai Z, Cui X, et al. Light absorption enhancement of black carbon from urban haze in Northern China winter[J]. Environ. Pollut., 2017,221:418-426.
[60]
Wang Q Y, Huang R J, Cao J J, et al. Mixing state of black carbon aerosol in a heavily polluted urban area of China:Implications for light absorption enhancement[J]. Aerosol Sci. Technol., 2014,48(7):689-697.
[61]
Xu X, Zhao W, Qian X, et al. Influence of photochemical aging on light absorption of atmospheric black carbon and aerosol single scattering albedo[J]. Atmos. Chem. Phys., 2018,18:16829-16844.
[62]
Cao F, Zhang X, Hao C, et al. Light absorption enhancement of particulate matters and their source apportionment over the Asian continental outflow site and South Yellow Sea[J]. Environ. Sci. Pollut. R., 2021,28:8022-8035.
[63]
Wang T, Zhao G, Tan T, et al. Effects of biomass burning and photochemical oxidation on the black carbon mixing state and light absorption in summer season[J]. Atmos. Environ., 2021,248:118230.
[64]
黄凡,陈楠,周家斌,等.2016~2017年武汉市城区大气PM2.5污染特征及来源解析[J].中国环境监测, 2019,35(1):17-25. Huang F, Chen N, Zhou J B,et al. Charateristics and source apportionment of PM2.5 in urban areas of Wuhan during 2016~2017[J]. Environmental Monitoring in China, 2019,35(1):17-25.
[65]
Wang G, Zhang R, Gomez M E, et al. Persistent sulfate formation from London Fog to Chinese haze[J]. Proc. Natl. Acad. Sci. USA, 2016, 113(48):13630-13635.
[66]
Li G, Lu D, Yang X, et al. Resurgence of sandstorms complicates China's air pollution situation[J]. Environ. Sci. Technol., 2021, 55(17):11467-11469.
[67]
Fialho P, Hansen A D A, Honrath R E. Absorption coefficients by aerosols in remote areas:a new approach to decouple dust and black carbon absorption coefficients using seven-wavelength Aethalometer data[J]. J. Aerosol Sci., 2005,36(2):267-282.
[68]
Yuan J F, Huang X F, Cao L M, et al. Light absorption of brown carbon aerosol in the PRD region of China[J]. Atmos. Chem. Phys., 2016,16(3):1433-1443.
[69]
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]. Atmos. Chem. Phys., 2009,9(6):2035-2050.
[70]
Mahowald N, Albani S, Kok J F, et al. The size distribution of desert dust aerosols and its impact on the Earth system[J]. Aeolian Research, 2014,15:53-71.
[71]
Mori I, Nishikawa M, Tanimura T, et al. Change in size distribution and chemical composition of kosa (Asian dust) aerosol during long-range transport[J]. Atmos. Environ., 2003,37(30):4253-63.
[72]
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]. Atmos. Chem. Phys., 2010,10(9):4207-4220.
[73]
Fierce L, Onasch T B, Cappa C D, et al. Radiative absorption enhancements by black carbon controlled by particle-to-particle heterogeneity in composition[J]. Proc. Natl. Acad. Sci. USA, 2020, 117(10):5196-5203.
[74]
Zhai J, Yang X, Li L, et al. Absorption Enhancement of Black Carbon Aerosols Constrained by Mixing-State Heterogeneity[J]. Environ. Sci. Technol., 2022,56(3):1586-1593.
