基于在线观测的重庆冬季棕碳吸光特性、来源及辐射效应研究:二次转化影响

Abstract
Figure/Table
References
Related Citation (15)

Download: PDF (1677 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract To investigate the light absorption characteristics and environmental effects of brown carbon (BrC) during pollution and clean periods, the light absorption coefficients of BrC were obtained by Aethalometer (AE33) from 20^th January 2023 to 21^st February 2023 in Chongqing. The results showed that the AAE values of PM_2.5 were 1.58 and 1.55 during pollution and clean periods, implying the presence of BrC in urban PM_2.5. During the campaign, BC and BrC contributed 58%~90% and 10%~42% to PM_2.5 absorption at 370~660 nm, indicating σ_abs was mainly affected by BC, but the contribution of BrC can not be ignored. The light absorption coefficient of BrC at 370 nm [σ_BrC(370)] was (35.30±8.21) Mm^-1 during pollution periods, 2.47 times higher than that during clean periods [(14.28±7.10) Mm^-1], and its contribution to σ_abs (10%~42%) was higher than those during clean periods (8%~41%). It is worth noting that the AAE_BrC values during pollution periods ranged from 3.2 to 4.7, generally lower than those during clean periods (3.6~4.9), which might be related to the difference of BrC components during the different periods. The light absorption coefficients of primary brown carbon (BrC_pri) and secondary brown carbon (BrC_sec) were obtained based on the minimum R squired method (MRS). The contributions of BrC_pri to σ_BrC were 74%~80% and 57%~74% during pollution and clean periods, higher than that of BrC_sec (20%~26% and 26%~43%). However, The AAE values of BrC_pri during pollution and clean periods were 3.42 and 3.08, significantly lower than the corresponding AAE(BrC_sec) (4.22 and 5.15), which was related to the strong wavelength dependence of BrC_sec light absorption. In addition, the daily variation of σ_BrC_sec(370) suggested that BrC_sec production might be mainly affected by the liquid-phase reaction under high humidity conditions at night. The radiative absorption contribution of BrC relative to BC was more significant in short wavelengths and decreased obviously with increasing wavelengths. The radiative absorption contributions of BrC_pri and BrC_sec at 370~950 nm were 24.8% and 10.2% during pollution periods, higher than that during clean periods (18.4% and 9.8%), respectively. The results of the potential source contribution function (PSCF) showed that the local emissions were the main sources of BrC during pollution periods in Chongqing, while regional transport from Hunan province and Guizhou province had major impacts of BrC during clean periods.

Key words： secondary brown carbon pollution periods light absorption characteristic radiation absorption Chongqing

Received: 15 November 2023

PACS:

X513

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	DENG Jing-cheng
	PENG Chao
	LU Pei-li
	LI Zhen-liang
	CHEN Yang
	ZHAI Chong-zhi
	YANG Fu-mo
	TIAN Mi

Cite this article:

DENG Jing-cheng,PENG Chao,LU Pei-li等. Characteristics of light absorption, sources, and radiative effects of brown carbon aerosol in Chongqing during winter based on on-line measurement: Implications of secondary formation[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(7): 3553-3562.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I7/3553

[1] Pöschl U. Aerosol particle analysis: Challenges and progress [J]. Analytical and Bioanalytical Chemistry, 2003,375(1):30-32.
[2] Spracklen D V, Carslaw K S, Pöschl U, et al. Global cloud condensation nuclei influenced by carbonaceous combustion aerosol [J]. Atmospheric Chemistry and Physics, 2011,11(17):9067-9087.
[3] Bond T C, Bergstrom R W. Light absorption by carbonaceous particles: An investigative review [J]. Aerosol Science and Technology, 2006, 40(1):27-67.
[4] 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).
[5] Andreae M O, Gelencsér A. Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols [J]. Atmospheric Chemistry and Physics, 2006,6(10):3131-3148.
[6] Saleh R, Hennigan C J, Mcmeeking G R, et al. Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions [J]. Atmospheric Chemistry and Physics, 2013,13(15):7683-7693.
[7] 王玉珏,胡敏,李晓,等.大气颗粒物中棕色碳的化学组成、来源和生成机制[J]. 化学进展, 2020,32(5):627-641. Wang Y Y, Hu M, Li X, et al. Chemical composition, sources and formation mechanisms of particulate brown carbon in the atmosphere [J]. Progress in Chemistry, 2020,32(5):627-641.
[8] Yuan W, Huang R, Yang L, et al. Characterization of the light- absorbing properties, chromophore composition and sources of brown carbon aerosol in Xi'an, northwestern China [J]. Atmospheric Chemistry and Physics, 2020,20(8):5129-5144.
[9] 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.
[10] 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, 2014,11(35):4404-4414. Yan C Q, Zheng M, Zhang Y H. Research progress and direction of atmospheric brown carbon [J]. Environmental Science, 2014,11(35): 4404-4414.
[11] Laskin A, Laskin J, Nizkorodov S A. Chemistry of atmospheric brown carbon [J]. Chemical Reviews, 2015,115(10):4335-4382.
[12] Clarke A, Mcnaughton C, Kapustin V, et al. Biomass burning and pollution aerosol over North America: Organic components and their influence on spectral optical properties and humidification response [J]. Journal of Geophysical Research: Atmospheres, 2007,112(D12): D12S18.
[13] Bones D L, Henricksen D K, Mang S A, et al. Appearance of strong absorbers and fluorophores in limonene-O₃ secondary organic aerosol due to NH₄⁺-mediated chemical aging over long time scales [J]. Journal of Geophysical Research: Atmospheres, 2010,115(D5):D05203.
[14] Du Z, He K, Cheng Y, et al. A yearlong study of water-soluble organic carbon in Beijing II: Light absorption properties [J]. Atmospheric Environment, 2014,89:235-241.
[15] Zhang X, Lin Y, Surratt J D, et al. Light-absorbing soluble organic aerosol in Los Angeles and Atlanta: A contrast in secondary organic aerosol [J]. Geophysical Research Letters, 2011,38(21):L21810.
[16] 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-Atmospheres, 2013,118(11):5380-5552.
[17] Wang Q, Zhou Y, Ma N, et al. Review of brown carbon aerosols in China: Pollution level, optical properties, and emissions [J]. Journal of Geophysical Research: Atmospheres, 2022,127(16):e2021JD035473.
[18] Yan J, Wang X, Gong P, et al. Review of brown carbon aerosols: Recent progress and perspectives [J]. Science of the Total Environment, 2018,634:1475-1485.
[19] Lack D A, Bahreini R, Langridge J M, et al. Brown carbon absorption linked to organic mass tracers in biomass burning particles [J]. Atmospheric Chemistry and Physics, 2013,13(5):2415-2422.
[20] Chen Y, Xie S, Luo B, et al. Particulate pollution in urban Chongqing of southwest China: Historical trends of variation, chemical characteristics and source apportionment [J]. Science of the Total Environment, 2017,584-585:523-534.
[21] Hu H L, Tian M, Zhang L M, et al. Sources and gas-particle partitioning of atmospheric parent, oxygenated, and nitrated polycyclic aromatic hydrocarbons in a humid city in southwest China [J]. Atmospheric Environment, 2019,206(3):1-10.
[22] Wang H B, Zhang L M, Huo T T, et al. Application of parallel factor analysis model to decompose excitation-emission matrix fluorescence spectra for characterizing sources of water-soluble brown carbon in PM_2.5 [J]. Atmospheric Environment, 2020,223:117192.
[23] Peng C, Yang F, 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.
[24] Peng C, Tian M, Wang X, et al. Light absorption of brown carbon in PM_2.5 in the Three Gorges Reservoir region, southwestern China: Implications of biomass burning and secondary formation [J]. Atmospheric Environment, 2020,229:117409.
[25] Chen Y, Zhang S, Peng C, et al. Impact of the COVID-19 pandemic and control measures on air quality and aerosol light absorption in Southwestern China [J]. Science of the Total Environment, 2020,749: 141419.
[26] 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]. China Environmental Science, 2021, 41(9):4026-4035.
[27] 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.
[28] 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.
[29] Xie C, Xu W, Wang J, et al. Vertical characterization of aerosol optical properties and brown carbon in winter in urban Beijing, China [J]. Atmospheric Chemistry and Physics, 2019,19(1):165-179.
[30] Zhang W, Wang W, Li J, et al. Light absorption properties and potential sources of brown carbon in Fenwei Plain during winter 2018~2019[J]. Journal of Environmental Sciences, 2021,102:53-63.
[31] Wang X, Heald C L, Liu J, et al. Exploring the observational constraints on the simulation of brown carbon [J]. Atmospheric Chemistry and Physics, 2018,18(2):635-653.
[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(9):4962-4970.
[33] 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]. Atmospheric Chemistry and Physics, 2016,16(8):5453-5465.
[34] 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.
[35] 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 & Technology, 2019,53(21):12389-12397.
[36] Wang Y Q, Zhang X Y, Draxler R R. TrajStat: GIS-based software that uses various trajectory statistical analysis methods to identify potential sources from long-term air pollution measurement data [J]. Environmental Modelling & Software, 2009,24(8):938-939.
[37] 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(6):3476-3485.
[38] Zhao Z, Cao J, Chow J C, et al. Multi-wavelength light absorption of black and brown carbon at a high-altitude site on the Southeastern margin of the Tibetan Plateau, China [J]. Atmospheric Environment, 2019,212:54-64.
[39] Huang R, Yang L, Cao J, et al. Brown carbon aerosol in urban Xi'an, northwest china: The composition and light absorption properties [J]. Environmental Science & Technology, 2018,52(12):6825-6833.
[40] Levinson R, Akbari H, Berdahl P. Measuring solar reflectance-Part I: Defining a metric that accurately predicts solar heat gain [J]. Solar Energy, 2010,84(9):1717-1744.
[41] Li Z, Tan H, Zheng J, et al. Light absorption properties and potential sources of particulate brown carbon in the Pearl River Delta region of China [J]. Atmospheric Chemistry and Physics, 2019,19(18):11669-11685.
[42] Wang J, Nie W, Cheng Y, et al. Light absorption of brown carbon in eastern China based on 3-year multi-wavelength aerosol optical property observations and an improved absorption Ångström exponent segregation method [J]. Atmospheric Chemistry and Physics, 2018, 18(12):9061-9074.
[43] 彭超,陈阳,杨复沫,等.重庆市棕碳气溶胶吸光特性及其影响因素研究[J]. 大气与环境光学学报, 2022,17(1):135-147. Peng C, Chen Y, Yang F M, et al. Light absorption properties and implications of particulate brown carbon in Chongqing [J]. Journal of Atmospheric and Environmental Optics, 2022,17(1):135-147.
[44] 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.
[45] 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.
[46] Qiu Y, Wu X, Zhang Y, et al. Aerosol light absorption in a coastal city in Southeast China: Temporal variations and implications for brown carbon [J]. Journal of Environmental Sciences, 2019,80:257-266.
[47] Zhu C, 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, 2021,90:159-164.
[48] Chen Y, Wenger J C, Yang F, et al. Source characterization of urban particles from meat smoking activities in Chongqing, China using single particle aerosol mass spectrometry [J]. Environmental Pollution, 2017,228:92-101.
[49] 屈垚,刘卉昆,周岳,等.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 Y, Liu H K, Zhou Y, et al. Optical properties and radiative forcing contribution of brown carbon in Xi’an during winter [J]. China Environmental Science, 2022,42(10):4486-4493.
[50] Canonaco F, Slowik J G, Baltensperger U, et al. Seasonal differences in oxygenated organic aerosol composition: Implications for emissions sources and factor analysis [J]. Atmospheric Chemistry and Physics, 2015,15(12):6993-7002.
[51] Wang Q, Huang R, Zhao Z, et al. Effects of photochemical oxidation on the mixing state and light absorption of black carbon in the urban atmosphere of China [J]. Environmental Research Letters, 2017, 12(4):044012.
[52] 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.
[53] 彭超,李振亮,向英,等.重庆典型城区冬季碳质气溶胶的污染特征及来源解析[J]. 环境科学, 2024,45(1):48-60. Peng C, Li Z L, Xiang Y, et al. Characteristics and source apportionment of carbonaceous aerosols in the typical urban areas in chongqing during winter [J]. Environmental Science, 2024,45(1):48-60.
[54] Bao Z E, Zhang X Y, Li Q, et al. Measurement report: Intensive biomass burning emissions and rapid nitrate formation drive severe haze formation in the Sichuan Basin, China-insights from aerosol mass spectrometry [J]. Atmospheric Chemistry and Physics, 2023, 23:1147-1167.
[55] 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]. Atmospheric Environment, 2019,199:45-54.
[56] Li C, Yan F, Kang S, et al. Light absorption characteristics of carbonaceous aerosols in two remote stations of the southern fringe of the Tibetan Plateau, China [J]. Atmospheric Environment, 2016,143:79-85.
[57] Liu J, Scheuer E, Dibb J, et al. Brown carbon aerosol in the North American continental troposphere: sources, abundance, and radiative forcing [J]. Atmospheric Chemistry and Physics, 2015,15(14):7841-7858.