西安冬季大气棕碳光学特征及辐射强迫

屈垚, 刘卉昆, 周岳, 张勇, 时迎强, 师菊莲, 王楠, 朱崇抒

中国环境科学 ›› 2022, Vol. 42 ›› Issue (10) : 4486-4493.

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中国环境科学 ›› 2022, Vol. 42 ›› Issue (10) : 4486-4493.
大气污染与控制

西安冬季大气棕碳光学特征及辐射强迫

  • 屈垚1,2, 刘卉昆1, 周岳1, 张勇1, 时迎强3, 师菊莲3, 王楠3, 朱崇抒1,2
作者信息 +

Optical properties and radiative forcing contribution of brown carbon in Xi'an during winter

  • QU Yao1,2, LIU Hui-kun1, ZHOU Yue1, ZHANG Yong1, SHI Ying-qiang3, SHI Ju-lian3, WANG Nan3, ZHU Chong-shu1,2
Author information +
文章历史 +

摘要

为探讨西安冬季不同大气污染状况(污染天和清洁天)大气细粒子(PM2.5)及其一次棕碳(BrCpri)和二次棕碳(BrCsec)的光学特征及辐射效应,开展了高分辨率多波段光学参数观测,获得PM2.5多波段光学吸收系数(babs),通过进一步数据分析得到BrCpri和BrCsec的光谱依赖指数(AAE)及其相对黑碳(BC)的辐射强迫.结果显示,污染天时段370nm光学吸收(babs(370))和880nm光学吸收(babs(880))均值分别为(733±311) Mm-1和(185±80) Mm-1,分别高出清洁天约5.9倍和6.2倍.清洁天PM2.5的AAE1.08~2.09,变化幅度大于污染天(1.28~1.79).清洁天棕碳光学吸收(babs(BrC))在370nm波长对总吸收占比高于污染天,均超过30%.一次棕碳光学吸收(babs(BrCpri))在清洁天和污染天均对babs(BrC)呈现高贡献,占比范围分别为76%~86%和82%~91%,说明一次排放仍然是造成西安冬季污染的重要原因.清洁天BrC、BrCpri和BrCsec的AAE均值分别为4.42、4.31和4.78,均高于污染天,说明清洁天粒子等效直径相对较小,老化程度较高导致BrC的高光谱依赖性.babs(BrCsec)日间变化表明污染天凌晨高湿条件下的液相反应可能是BrCsec形成的主要机制,比清洁天更为强烈,而污染天日间BrCsec受光漂白的影响较大.最后估算了BrCpri和BrCsec的辐射强迫效应,在紫外波段(300~400nm),污染天BrCpri和BrCsec相对BC的辐射强迫分别为62%和16%,而清洁天分别为59%和23%,表明BrCpri和BrCsec在西安冬季的辐射强迫效应不容忽视.

Abstract

To investigate the light absorption coefficient (babs) and radiative forcing of primary and secondary brown carbon (BrCpri and BrCsec) during winter haze and clean days in Xi'an, Aethalometer (AE33) was used to obtain the babs of PM2.5 from 15th December 2015 to 31st January 2016, the absorption Ångström exponent(AAE) and radiation forcing relative to black carbon (BC) of BrCpri and BrCsecwere further analyzed. The results showed that the mean values of babs(370) and babs(880) were (733±311)Mm-1 and (185±80)Mm-1in haze days, those were 5.9 and 6.2 times higher than that in clean days, respectively. The AAEs of PM2.5 varied from1.08 to 2.09 in clean days, which showed higher amplitude than those in haze days (1.28~1.79). The contributions of babs(BrC) to total babsat 370 nm in clean days were higher than those in haze days (>30%). High contributions of babs(BrCpri) to babs(BrC) in clean days (76%~86%) and haze days (82%~91%) indicated that the primary emissions were the important causes of severe air pollution during wintertime in Xi'an. The AAEs values of BrC(4.42), BrCpri(4.31) and BrCsec(4.78) in clean days were higher than those in haze days, which may be attributed to the smaller equivalent diameter and higher aging of PM2.5 in clean days. The results indicated the dominance of the aqueous reactions mechanism for BrCsec formation before the sunrise during polluted days. After sunrise, the bleaching of BrCsec chromophores through oxidative processes was of more importance in polluted days than that in clean days. The relative radiative forcing of BrCpri and BrCsec to BC(300~400nm) were 59% and 23% in clean days, while those were 62% and 16% in haze days, respectively. The results underlined the radiative forcing of BrCpri and BrCsec in winter.

关键词

辐射强迫 / 光学吸收 / 西安 / 棕碳

Key words

brown carbon / light absorption / radiation forcing / Xi'an

引用本文

导出引用
屈垚, 刘卉昆, 周岳, 张勇, 时迎强, 师菊莲, 王楠, 朱崇抒. 西安冬季大气棕碳光学特征及辐射强迫[J]. 中国环境科学. 2022, 42(10): 4486-4493
QU Yao, LIU Hui-kun, ZHOU Yue, ZHANG Yong, SHI Ying-qiang, SHI Ju-lian, WANG Nan, ZHU Chong-shu. Optical properties and radiative forcing contribution of brown carbon in Xi'an during winter[J]. China Environmental Science. 2022, 42(10): 4486-4493
中图分类号: X513   

参考文献

[1] Gelencsér A.Carbonaceous aerosol[Z].Springer, 2004,350.
[2] Jimenez J L, Canagaratnam R, Donahue Nm, et al.Evolution of organic aerosols in the atmosphere[J].Science, 2009,326.
[3] moosmüller H, Chakrabarty R K, Arnott W P.Aerosol light absorption and its measurement:A review[J].Journal of Quantitative Spectroscopy and Radiative Transfer, 2009,110(11):844-878.
[4] Jacobsonm C, Hansson H C, Noone K J, et al.Organic atmospheric aerosols:review and state of the science[J].Reviews of Geophysics, 2000,38(2):267-294.
[5] Andreaem O, A Gelencsér.Black carbon or brown carbon? The nature of light~absorbing carbonaceous aerosols[J].Atmospheric Chemistry and Physics, 2006,6(10):3131-3148.
[6] 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].Journal of Geophysical Research, 2013,118:5380-5552.
[7] moosmüller H, Chakrabarty R K, Ehlers Km, et al.Absorption angström coefficient, brown carbon, and aerosols:basic concepts, bulkmatter, and spherical particles[J].Atmospheric Chemistry and Physics, 2011,11:1217-1225.
[8] Lu Z, Streets D G, Winijkul E, et al.Light absorption properties and radiative effects of primary organic aerosol emissions[J].Environmental Science and Technology, 2015,49(8):4868-4877.
[9] 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, D21208.
[10] Hoffer A, Gelencsér A, Guyon P, et al.Optical properties of humic~like substances (HULIS) in biomass~burning aerosols[J].Atmospheric Chemistry and Physics, 2006,6:3563-3570.
[11] Laskin A, Laskin J, Nizkorodov S A.Chemistry of atmospheric brown carbon[J].Chemical Reviews, 2015,115(10):4335.
[12] Wang Q, Ye J, Wang Y, et al.Wintertime optical properties of primary and secondary brown carbon at a regional site in the North China Plain[J].Environmental Science and Technology, 2019,53:12389− 12397.
[13] Zhu C S, Qu Y, Zhou Y, et al.High light absorption and radiative forcing contributions of primary brown carbon and black carbon to urban aerosol[J].Gondwana Research, 2021,90(10):159-164.
[14] Dumka U C, Kaskaoutis D G, Tiwari S, et al.Assessment of biomass burning and fossil fuel contribution to black carbon concentrations in Delhi during winter[J].Atmospheric Environment, 2018,194(DEC.):93-109.
[15] Huang R J, Yang L, Cao J J, et al.Brown carbon aerosol in urban Xi'an, Northwest China:the composition and light absorption properties[J].Environmental Science and Technology, 2018,52:6825-6833.
[16] Utry N, Ajtai T, Pintérm, et al.Mass specific optical absorption coefficients and imaginary part of the complex refractive indices of mineral dust components measured by amulti~wavelength photoacoustic spectrometer[J].Atmospheric measurement Techniques, 2015,8(1):401-410.
[17] Sandradewi J, Prevot A S H, Szidat S, et al.Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter[J].Environmental Science and Technology, 2008,42(9):3316-3323.
[18] Wang G, Chen C, Li J, et al.Molecular composition and size distribution of sugars, sugar-alcohols and carboxylic acids in airborne particles during a severe urban haze event caused by wheat straw burning[J].Atmospheric Environment, 2011,45:2473-2479.
[19] Zhang J K, Sun Y, Liu Z R, et al.Characterization of submicron aerosols during a month of serious pollution in Beijing, 2013[J].Atmospheric Chemistry and Physics, 2014,14:2887-2903.
[20] Lou S, Yang Y, Wang H, et al.Black carbon amplifies haze over the North China Plain by weakening the east Asian winter monsoon[J].Geophysical Research Letters, 2019,46:452-460.
[21] Wang L, Jin W J, Sun J Z, et al.Seasonal features of brown carbon in northern China:Implications for BrC emission control[J].Atmospheric Research, 2021,257:105610.
[22] Zhang Q, Shen Z X, Zhang T, et al.Spatial distribution and sources of winter black carbon and brown carbon in six Chinese megacities[J].Science of the Total Environment, 2021,762:143075.
[23] Shen Z, Zhang Q, Cao J, et al.Optical properties and possible sources of brown carbon in PM2.5 over Xi'an, China[J].Atmospheric Environment, 2017,150:322330.
[24] 曹宁,黄学敏,祝颖,等.西安冬季重污染过程PM2.5理化特征及来源解析[J].中国环境科学, 2019,39(1):32-39.Cao N, Hunag X M, Zhu Y, et al.Pollution characteristics and source apportionment of fine particles during a heavy pollution in winter in Xi'an City[J].China Environmental Science, 2019,39(1):32-39.
[25] 王宇翔.西安市黑碳气溶胶污染特征及其吸收特性研究[D].西安:西安建筑科技大学, 2016.Wang Y X.The study for characteristics of black carbon aerosol pollution and their absorption properties in Xi'an[D].Xi'an:Xi'an University of Architecture and Technology, 2016.
[26] Drinovec L,močnik 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.
[27] 蔡园青,徐学哲,周家成,等.黑碳仪测量气溶胶吸收系数的校正算法和影响因素研究进展[J].中国环境科学, 2021,41(9):4026-4035.Cai Y Q, Xu X Z, Zhou J C, et al.Research progress of correction algorithm and influence factors for aerosol absorption coefficient from aethalometer measurement[J].Chinese Environmental Science, 2021, 41(9):4026-4035.
[28] Shamjad P M, Tripathi S N, Pathak R, et al.Contribution of brown carbon to direct radiative forcing over the Indo~Gangetic Plain[J].Environmental Science and Technology, 2015,49(17):10474-10481.
[29] Lack D A, Langridge Jm.On the attribution of black and brown carbon light absorption using the angström exponent[J].Atmospheric Chemistry and Physics, 2013,13(20):10535-10543.
[30] 崔杰,黄晓锋,袁金凤等.基于在线观测的大气PM2.5中棕色碳吸光贡献估算[J].中国环境科学, 2017,37(2):401-406.Cui J, Huang X F, Yuan J F, et al.Estimation of light absorption by brown carbon in PM2.5 based on on-line measurement[J].Chinese Environmental Science, 2017,37(2):401-406.
[31] 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, 2009,9(6):2035−2050.
[32] 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].Geophysical Research Letters, 2019,46:4962− 4970.
[33] 谭健,夏瑞,吴兑,等.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 J, Xia R, Wu D, et al.Determination of crustal element iron light absorption contribution and effects on black carbon light absorption enhancement estimation:a case study in Wuhan[J].Chinese Environmental Science, 2022,42(7):3033-3045.
[34] Kirillova E N, Andersson A, Tiwari S, et al.Water-soluble organic carbon aerosols during a full New Delhi winter:Isotope based source apportionment and optical properties[J].Journal of Geophysical Research:Atmospheres, 2014,119:3476-3485.
[35] Levinson R, Akbari H, Berdahl P.Measuring solar reflectance−part I:defining ametric that accurately predicts solar heat gain[J].Solar Energy, 2010,84:1717-1744.
[36] Cao J J, Shen Z X, Chow J C, et al.Winter and summer PM2.5 chemical compositions in fourteen Chinese cities[J].Journal of the Air & Waste management Association, 2012,62(10):1214-1226.
[37] Chao L, Eddy C C, Yan Y, et al.The absorption angström exponent of black carbon:From numerical aspects[J].Atmospheric Chemistry and Physics, 2018,18(9):6259-6273.
[38] Wu Y, Li J, Jiang C, et al.Spectral absorption properties of organic carbon aerosol during a polluted winter in Beijing, China[J].Science of The Total Environment, 2021,755(Pt 2):142600.
[39] Luo J, Zhang Y, Zhang Q.The angström exponent and single-scattering albedo of black carbon:effects of different coating materials[J].Atmosphere, 2020,11(10):1103.
[40] Zhang W Y, Wang W G, Li J, et al.Light absorption properties and potential sources of brown carbon in Fenwei Plain during winter 2018~2019[J].Journal of Environmental Science, 2021,102:53-63.
[41] Li X R, Zhao Q, Yang Y, et al.Composition and sources of brown carbon aerosols in megacity Beijing during the winter of 2016[J].Atmospheric Research, 2021,262:105773.
[42] Cheng Y, Cao X B, Liu J M, et al.Primary nature of brown carbon absorption in a frigid atmosphere with strong haze chemistry[J].Environment Research, 2022,204:112324.
[43] Kaskaoutis D G, Grivas G, Stavroulas I, et al.Apportionment of black and brown carbon spectral absorption sources in the urban environment of Athens, Greece, during winter[J].Science of the Total Environment, 2021,801:149739.
[44] Zhang Y, Wang Q Y, Tian J et al.Impact of COVID-19 lockdown on the optical properties and radiative effects of urban brown carbon aerosol[J].Geoscience Frontiers, 2021,101320.
[45] Hems R F, Schnitzler E G, Liu-Kang C, et al.Aging of atmospheric brown carbon aerosol[J].ACS Earth and Space Chemistry, 2021,5(4):722-748.
[46] Liakakou E, Kaskaoutis D G, Grivas G, et al.Long-term brown carbon spectral characteristics in a Mediterranean city (Athens)[J].Science of the Total Environment, 2020,708:135019.
[47] Li J J, Zhang Q, Wang G H, et al.Optical properties and molecular compositions of water-soluble and water-insoluble brown carbon (BrC) aerosols in northwest China[J].Atmospheric Chemistry and Physics, 2020,20(8):4889-4904.
[48] Peng C, Yang F M, Tian M, et al.Brown carbon aerosol in two megacities in the Sichuan Basin of southwestern China:Light absorption properties and implications[J].Science of the Total Environment, 2020,719:137483.
[49] Soleimanian E, Mousavi A, Taghvaee S, et al.Impact of secondary and primary particulate matter (PM) sources on the enhanced light absorption by brown carbon (BrC) particles in central Los Angeles[J].Science of the Total Environment, 2019,705:135902.

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中华人民共和国科技部资助(2017YFC0212200)

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