Transboundary Secondary Organic Aerosol in Western Japan Indicated by the δ13C of Water-Soluble Organic Carbon and the m/z 44 Signal in Organic Aerosol Mass Spectra

被引:17
作者
Irei, Satoshi [1 ]
Takami, Akinori [1 ]
Hayashi, Masahiko [2 ]
Sadanaga, Yasuhiro [3 ]
Hara, Keiichiro [2 ]
Kaneyasu, Naoki [4 ]
Sato, Kei [1 ]
Arakaki, Takemitsu [5 ]
Hatakeyama, Shiro [6 ]
Bandow, Hiroshi [3 ]
Hikida, Toshihide [7 ]
Shimono, Akio [7 ]
机构
[1] Natl Inst Environm Studies, Tsukuba, Ibaraki 3058506, Japan
[2] Fukuoka Univ, Dept Earth Syst Sci, Fac Sci, Jonan Ku, Fukuoka 8140180, Japan
[3] Osaka Prefecture Univ, Grad Sch Engn, Dept Appl Chem, Naka Ku, Sakai, Osaka 5998531, Japan
[4] Natl Inst Adv Ind Sci & Technol, Tsukuba, Ibaraki 3058569, Japan
[5] Univ Ryukyus, Dept Chem Biol & Marine Sci, Nishihara, Okinawa 9030213, Japan
[6] Tokyo Univ Agr & Technol, Dept Agr, Fuchu, Tokyo 1838509, Japan
[7] Shoreline Sci Res Inc, Hachioji, Tokyo 1920045, Japan
关键词
STABLE CARBON; ISOTOPIC COMPOSITION; MARINE AEROSOLS; HYDROCARBONS; PARTICLES; ACIDS; C-13; FRACTIONATION; SPECTROMETER; VAPORIZATION;
D O I
10.1021/es405362y
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The stable carbon isotope ratio ((delta C-13) of low-volatile water-soluble organic carbon (LV-WSOC) was measured in filter samples of total suspended particulate matter, collected every 24 h in the winter of 2010 at an urban site and two rural sites in western Japan. Concentrations of the major chemical species in fine aerosol (<1.0 mu m) were also measured in real time by aerosol mass spectrometers. The oxidation state of organic aerosol was evaluated using f(44); i.e., the proportion of the signal at m/z 44 (CO2+ ions from the carboxyl group) to the sum of all m/z signals in the organic mass spectra. A strong correlation between LV-WSOC and m/z 44 concentrations was observed, which suggested that LV-WSOC was likely to be associated with carboxylic acids in fine aerosol. Plots of delta C-13 of LV-WSOC versus f(44) showed random variation at the urban site and systematic trends at the rural sites. The systematic trends qualitatively agreed with a simple binary mixture model of secondary organic aerosol with background LV-WSOC with an f(44) of similar to 0.08 and delta C-13 of -17 parts per thousand or higher. Comparison with reference values suggested that the source of background LV-WSOC was likely to be primary emissions associated with C-4 plants.
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页码:6273 / 6281
页数:9
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