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
[11]   Optical-chemical-microphysical relationships and closure studies for mixed carbonaceous aerosols observed at Jeju Island; 3-laser photoacoustic spectrometer, particle sizing, and filter analysis [J].
Flowers, B. A. ;
Dubey, M. K. ;
Mazzoleni, C. ;
Stone, E. A. ;
Schauer, J. J. ;
Kim, S. -W. ;
Yoon, S. C. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (21) :10387-10398
[12]   Contribution of isoprene-derived organosulfates to free tropospheric aerosol mass [J].
Froyd, K. D. ;
Murphy, S. M. ;
Murphy, D. M. ;
de Gouw, J. A. ;
Eddingsaas, N. C. ;
Wennberg, P. O. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2010, 107 (50) :21360-21365
[13]   Composition and sources of carbonaceous aerosols in Northern Europe during winter [J].
Glasius, M. ;
Hansen, A. M. K. ;
Claeys, M. ;
Henzing, J. S. ;
Jedynska, A. D. ;
Kasper-Giebl, A. ;
Kistler, M. ;
Kristensen, K. ;
Martinsson, J. ;
Maenhaut, W. ;
Nojgaard, J. K. ;
Spindler, G. ;
Stenstrom, K. E. ;
Swietlicki, E. ;
Szidat, S. ;
Simpson, D. ;
Yttri, K. E. .
ATMOSPHERIC ENVIRONMENT, 2018, 173 :127-141
[14]   Measurement of the light absorbing properties of diesel exhaust particles using a three-wavelength photoacoustic spectrometer [J].
Guo, Xuesong ;
Nakayama, Tomoki ;
Yamada, Hiroyuki ;
Inomata, Satoshi ;
Tonokura, Kenichi ;
Matsumi, Yutaka .
ATMOSPHERIC ENVIRONMENT, 2014, 94 :428-437
[15]   Nitrated phenols in the atmosphere: a review [J].
Harrison, MAJ ;
Barra, S ;
Borghesi, D ;
Vione, D ;
Arsene, C ;
Olariu, RL .
ATMOSPHERIC ENVIRONMENT, 2005, 39 (02) :231-248
[16]   Organosulfates from Pinene and Isoprene over the Pearl River Delta, South China: Seasonal Variation and Implication in Formation Mechanisms [J].
He, Quan-Fu ;
Ding, Xiang ;
Wang, Xin-Ming ;
Yu, Jian-Zhen ;
Fu, Xiao-Xin ;
Liu, Teng-Yu ;
Zhang, Zhou ;
Xue, Jian ;
Chen, Duo-Hong ;
Zhong, Liu-Ju ;
Donahue, Neil M. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (16) :9236-9245
[17]   Water-Soluble Organic Aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States [J].
Hecobian, A. ;
Zhang, X. ;
Zheng, M. ;
Frank, N. ;
Edgerton, E. S. ;
Weber, R. J. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (13) :5965-5977
[18]   Brown Carbon Aerosol in Urban Xi'an, Northwest China: The Composition and Light Absorption Properties [J].
Huang, Ru-Jin ;
Yang, Lu ;
Cao, Junji ;
Chen, Yang ;
Chen, Qi ;
Li, Yongjie ;
Duan, Jing ;
Zhu, Chongshu ;
Dai, Wenting ;
Wang, Kai ;
Lin, Chunshui ;
Ni, Haiyan ;
Corbin, Joel C. ;
Wu, Yunfei ;
Zhang, Renjian ;
Tie, Xuexi ;
Hoffmann, Thorsten ;
O'Dowd, Colin ;
Dusek, Uli .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2018, 52 (12) :6825-6833
[19]   The formation of organic sulfate esters in the limonene ozonolysis secondary organic aerosol (SOA) under acidic conditions [J].
Iinuma, Yoshiteru ;
Mueller, Conny ;
Boege, Olaf ;
Gnauk, Thomas ;
Herrmann, Hartmut .
ATMOSPHERIC ENVIRONMENT, 2007, 41 (27) :5571-5583
[20]   Methyl-Nitrocatechols: Atmospheric Tracer Compounds for Biomass Burning Secondary Organic Aerosols [J].
Iinuma, Yoshiteru ;
Boege, Olaf ;
Graefe, Ricarda ;
Herrmann, Hartmut .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2010, 44 (22) :8453-8459