The light absorbing and molecule characteristic of PM2.5 brown carbon observed in urban Shanghai

被引:4
作者
Bai, Zhe [1 ,2 ]
Wen, Wen [1 ]
Zhang, Wei [1 ]
Li, Ling [1 ]
Wang, Lina [1 ,3 ]
Chen, Jianmin [1 ,3 ]
机构
[1] Fudan Univ, Dept Environm Sci & Engn, Shanghai Key Lab Atmospher Particle Pollut & Preve, Shanghai 200433, Peoples R China
[2] Inner Mongolia Univ, Sch Ecol & Environm, Hohhot, Peoples R China
[3] Inst Ecochongming IEC, Shanghai, Peoples R China
基金
中国国家自然科学基金;
关键词
Brown carbon; Long-chain; Aliphatic organosulfates; Diesel fuel; SECONDARY ORGANIC AEROSOL; ISOPRENE-DERIVED ORGANOSULFATES; AIR-POLLUTION SOURCES; PEARL RIVER DELTA; PARTICULATE ORGANOSULFATES; CHEMICAL-CHARACTERIZATION; NITRATED PHENOLS; BLACK CARBON; ABSORPTION; PHOTOOXIDATION;
D O I
10.1016/j.envpol.2022.120874
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Both brown carbon (BrC) and the non-absorbing components coated on black carbon (BC) aerosols can enhance the light absorption of BC aerosols. BrC is a complicated mixture of organic compounds and not well charac-terized, which hinders exploring the links between BrC and optical properties. We conducted an in-depth field study on optical properties of ambient aerosols at a monitoring site in Shanghai, China via real-time monitoring and offline analysis. Results showed that BrC caused light absorption coefficients were 3.3 +/- 3.3 Mm-1, 2.2 +/- 5.0 Mm-1, 1.2 +/- 1.2 Mm-1 at lambda = 370, 470 and 520 nm, respectively, accounting for 11%, 10%, 6% of the total aerosol absorption for the corresponding wavelengths. A larger proportion of long-chain aliphatic organosulfates (OSs, CnH2n+2O4S, (CH2)nO5S, (CH2)nO6S) with double bond equivalent (DBE) values of 0 or 1 accounted for 5-20% of the light absorption (lambda = 365 nm) for soluble brown carbon (BrC), which were dominating for the days with less N-containing aromatic compounds appearing. Furthermore, the structure of CnH2n+2O4S, (CH2)nO5S, (CH2)nO6S were explored using target MS/MS of HPLC-Q-ToF-MS: (CH2)nO5S series, the most abundant family of OSs, were constructed by functionalizing a saturated hydrocarbon with one sulfate and one carbonyl group. CnH2n+2O4S series were oxidized with only one sulfate group in the aliphatic chain R. (CH2)nO6S series were proposed as aliphatic OSs with one ester group. We speculated aliphatic OSs were formed via acid catalyzed perhydrolysis of hydroperoxides derived from long-chain alkanes releasing from diesel fueled vehicles, followed by the reaction with sulfate anion radicals. Therefore, relevant technologies should be further explored to reduce the impacts from vehicle emissions.
引用
收藏
页数:10
相关论文
共 72 条
[31]   Airborne measurements of organosulfates over the continental US [J].
Liao, Jin ;
Froyd, Karl D. ;
Murphy, Daniel M. ;
Keutsch, Frank N. ;
Yu, Ge ;
Wennberg, Paul O. ;
St. Clair, Jason M. ;
Crounse, John D. ;
Wisthaler, Armin ;
Mikoviny, Tomas ;
Jimenez, Jose L. ;
Campuzano-Jost, Pedro ;
Day, Douglas A. ;
Hu, Weiwei ;
Ryerson, Thomas B. ;
Pollack, Ilana B. ;
Peischl, Jeff ;
Anderson, Bruce E. ;
Ziemba, Luke D. ;
Blake, Donald R. ;
Meinardi, Simone ;
Diskin, Glenn .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2015, 120 (07) :2990-3005
[32]   Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols [J].
Liggio, John ;
Li, Shao-Meng .
GEOPHYSICAL RESEARCH LETTERS, 2006, 33 (13)
[33]   Molecular characterization of brown carbon (BrC) chromophores in secondary organic aerosol generated from photo-oxidation of toluene [J].
Lin, Peng ;
Liu, Jiumeng ;
Shilling, John E. ;
Kathmann, Shawn M. ;
Laskin, Julia ;
Laskin, Alexander .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (36) :23312-23325
[34]   Organosulfates in Humic-like Substance Fraction Isolated from Aerosols at Seven Locations in East Asia: A Study by Ultra-High-Resolution Mass Spectrometry [J].
Lin, Peng ;
Yu, Jian Zhen ;
Engling, Guenter ;
Kalberer, Markus .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2012, 46 (24) :13118-13127
[35]   Ultraviolet and visible complex refractive indices of secondary organic material produced by photooxidation of the aromatic compounds toluene and m-xylene [J].
Liu, P. F. ;
Abdelmalki, N. ;
Hung, H. -M. ;
Wang, Y. ;
Brune, W. H. ;
Martin, S. T. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2015, 15 (03) :1435-1446
[36]   Seasonal and diurnal variations of particulate organosulfates in urban Shanghai, China [J].
Ma, Ye ;
Xu, Xinkai ;
Song, Weihua ;
Geng, Fuhai ;
Wang, Lin .
ATMOSPHERIC ENVIRONMENT, 2014, 85 :152-160
[37]   Exploring sources of biogenic secondary organic aerosol compounds using chemical analysis and the FLEXPART model [J].
Martinsson, Johan ;
Monteil, Guillaume ;
Sporre, Moa K. ;
Hansen, Anne Maria Kaldal ;
Kristensson, Adam ;
Stenstrom, Kristina Eriksson ;
Swietlicki, Erik ;
Glasius, Marianne .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2017, 17 (18) :11025-11040
[38]   Aerosol Light Extinction Measurements by Cavity Attenuated Phase Shift (CAPS) Spectroscopy: Laboratory Validation and Field Deployment of a Compact Aerosol Particle Extinction Monitor [J].
Massoli, Paola ;
Kebabian, Paul L. ;
Onasch, Timothy B. ;
Hills, Frank B. ;
Freedman, Andrew .
AEROSOL SCIENCE AND TECHNOLOGY, 2010, 44 (06) :428-435
[39]   Contribution of Nitrated Phenols to Wood Burning Brown Carbon Light Absorption in Detling, United Kingdom during Winter Time [J].
Mohr, Claudia ;
Lopez-Hilfiker, Felipe D. ;
Zotter, Peter ;
Prevot, Andre S. H. ;
Xu, Lu ;
Ng, Nga L. ;
Herndon, Scott C. ;
Williams, Leah R. ;
Franklin, Jonathan P. ;
Zahniser, Mark S. ;
Worsnop, Douglas R. ;
Knighton, W. Berk ;
Aiken, Allison C. ;
Gorkowski, Kyle J. ;
Dubey, Manvendra K. ;
Allan, James D. ;
Thornton, Joel A. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (12) :6316-6324
[40]   Design and performance of a three-wavelength LED-based total scatter and backscatter integrating nephelometer [J].
Mueller, T. ;
Laborde, M. ;
Kassell, G. ;
Wiedensohler, A. .
ATMOSPHERIC MEASUREMENT TECHNIQUES, 2011, 4 (06) :1291-1303