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1.
論文(リポジトリ) |
Deng, Yange ; Fujinari, Hiroaki ; Yai, Hikari ; Shimada, Kojiro ; Miyazaki, Yuzo ; Tachibana, Eri ; Deshmukh, K. Dhananjay ; Kawamura, Kimitaka ; Nakayama, Tomoki ; Tatsuta, Shiori ; Cai, Mingfu ; Xu, Hanbing ; Li, Fei ; Tan, Haobo ; Ohata, Sho ; Kondo, Yutaka ; Takami, Akinori ; Hatakeyama, Shiro ; Mochida, Michihiro
概要:
Filter-based offline analysis of atmospheric aerosol hygroscopicity coupled to composition analysis provides information
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complementary to that obtained from online analysis. However, its application itself and comparison to online analysis have remained limited to date. In this study, daily submicrometer aerosol particles (PM0.95, 50 % cutoff diameter 0.95 µm) were collected onto quartz fiber filters on Okinawa Island, a receptor of East Asian outflow, in the autumn of 2015. The chemical composition of water-soluble matter (WSM) in PM0.95, PM0.95 itself, and their respective hygroscopicities were characterized through the offline use of an aerosol mass spectrometer and a hygroscopicity tandem differential mobility analyzer. Thereafter, results were compared with those obtained from online analyses. Sulfate dominated the WSM mass (59 %), followed by water-soluble organic matter (WSOM, 20 %) and ammonium (13 %). WSOM accounted for most (91 %) of the mass of extracted organic matter (EOM) and the atomic O-to-C ratios (O : C) of WSOM and EOM were high (mean ± standard deviation were 0.84 ± 0.08 and 0.78 ± 0.08, respectively), both of which indicate highly aged characteristics of the observed aerosol. The hygroscopic growth curves showed clear hysteresis for most samples. At 85 % relative humidity (RH), the calculated hygroscopicity parameter κ values of the WSM (κWSM), WSOM, EOM, andPM0.95 (κPM0.95 ) were 0.50 ± 0.03, 0.22 ± 0.12, 0.20 ± 0.11, and 0.47 ± 0.03, respectively. An analysis using the thermodynamic Extended Aerosol Inorganics Model (E-AIM) shows, on average, that inorganic salts and WSOM contributed 88 % and 12 %, respectively, of the κWSM (or κPM0.95 ). High similarities were found between offline and online analysis for chemical compositions that are related to particle hygroscopicity (the mass fractions and O : C of organics and the degree of neutralization) and also for aerosol hygroscopicity. As possible factors governing the variation in κWSM, the influences of WSOM abundance and the neutralization of inorganic salts were assessed. At high RH (70 %–90 %), the hygroscopicity of WSM and PM0.95 was affected considerably by the presence of organic components; at low RH (20 %–50 %), the degree of neutralization could be important.This study not only characterized aerosol hygroscopicity at the receptor site of East Asian outflow but also shows that offline hygroscopicity analysis is an appropriate method, at least for aerosols of the studied type. The results encourage further applications to other environments and to more in-depth hygroscopicity analysis, in particular for organic fractions.
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2.
論文(リポジトリ) |
Tatsuta, Shiori ; Shimada, Kojiro ; Chan, K. Chak ; Kim, Pyo Yong ; Lin, Neng-Huei ; Takami, Akinori ; Hatakeyama, Shiro
概要:
We observed the size distributions of mass concentration, ionic composition, and trace metal concentration in aerosols c
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ollected at an urban site in Kumamoto Prefecture (KM) and a rural site at Cape Hedo in Okinawa Prefecture (HD) between 2012 and 2015. To evaluate the contribution of transboundary nitrate and locally emitted nitrate in the aerosols at Kumamoto, we distinguished between days of transboundary air pollution from East Asia and days of local air pollution on the basis of a threshold for Pb concentration and the ratio Pb (in 0.5 < projected area diameter (Dp) < 1.0 µm)/Cu (in 2.5 < Dp < 10 µm). Fine nitrate (particulate NH_4NO_3) did not arrive at HD from the Asian continent even under long-range transport conditions. Fine nitrate emitted in Kumamoto and its vicinity also was not transported to HD, even in an air mass that passed over KM and reached HD within one day. Almost all fine nitrate was converted to coarse nitrate during transport by dissociation of fine nitrate and adsorption of HNO_3 on larger aerosol particles. Transboundary nitrate existed largely in the particle size range of 0.5 < Dp < 10 µm, and the contribution of transboundary nitrate in the particle size range of 0.1 < Dp < 0.5 µm was about 20% even under long-range transport conditions. The contribution of transboundary nitrate in particles with Dp < 2.5 µm at KM was approximately 50%, 50%, and 80% in spring, autumn, and winter, respectively.
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3.
論文(リポジトリ) |
Itahashi, Syuichi ; Hatakeyama, Shiro ; Shimada, Kojiro ; Tatsuta, Shiori ; Taniguchi, Yuta ; Chan, K. Chak ; Kim, Pyo Yong ; Lin, Neng-Huei ; Takami, Akinori
概要:
An intensive observation campaign at Cape Hedo, Okinawa, Japan was conducted from late October to early November 2015 to investigate the behavior of long-range transported atmospheric pollutants. During this period, sulfate
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(SO_4^<2->) was the dominant aerosol component. The sources of SO_4^<2-> were estimated by using the air quality model with the tagged tracer method. The main source of high SO_4^<2-> concentration varied day-to-day. When the westerly wind was dominant (October 27), the main source was anthropogenic SO_2 emissions in China. When the northerly wind prevailed (November 1), the impact of volcanoes in western Japan was significant and the conversion ratio from SO_2 to SO_4^<2-> was lowest, at less than 70%, because of the faster transport. During the latter part of the campaign, the northerly to easterly winds were prominent, and the impacts of Korea, Japan, and ships on SO_4^<2-> observed at Cape Hedo were also clear. When the contributions from Korea, Japan, and ships were the highest (November 4), the conversion ratio was also the highest, at greater than 95% because of long-range transport. The modeled sources of volcanoes and ship emissions corresponded well with the observed coarse-mode SO_4^<2-> and V/Mn ratio, respectively. The mutual evaluation of sources from model and observations enable SO_4^<2-> sources to be estimated with higher confidence.
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