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Water-Soluble Ionic Species and Trace Metals in Sapporo Aerosols

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Water-Soluble Ionic Species and Trace Metals in Sapporo Aerosols EGU Journal Logos (RGB) Open Access Open Access Open Access Advances in Annales Nonlinear Processes Geosciences Geophysicae in Geophysics Open Access Open Access Natural Hazards Natural Hazards and Earth System and Earth System Sciences Sciences Discussions Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Open Access Open Access Atmos. Chem. Phys. Discuss., 13, 6589–6629,Atmospheric 2013 Atmospheric www.atmos-chem-phys-discuss.net/13/6589/2013/Chemistry Chemistry doi:10.5194/acpd-13-6589-2013 ACPD and Physics and Physics © Author(s) 2013. CC Attribution 3.0 License. 13, 6589–6629, 2013 Discussions Open Access Open Access Atmospheric Atmospheric This discussion paper is/hasMeasurement been under review for the journal AtmosphericMeasurement Chemistry Water-soluble ionic and Physics (ACP). Please referTechniques to the corresponding final paper in ACP ifTechniques available. species and trace Discussions metals in Sapporo Open Access Year-round observations of water-solubleOpen Access aerosols Biogeosciences Biogeosciences ionic species and trace metals in SapporoDiscussions C. M. Pavuluri et al. Open Access aerosols: implication for significant Open Access Climate Climate Title Page of the Past of the Past contributions from terrestrial biologicalDiscussions Abstract Introduction Open Access sources in Northeast Asia Open Access Conclusions References Earth System Earth System 1 1 1,2 1,3 Tables Figures C. M. Pavuluri , K. KawamuraDynamics, N. Mihalopoulos , and P. Fu Dynamics Discussions 1 Institute of Low Temperature Science, Hokkaido University, N19, W08, Kita-ku, Sapporo J I Open Access 060-0819, Japan Geoscientific Geoscientific Open Access 2Environmental Chemical ProcessesInstrumentation Laboratory, Department of Chemistry,Instrumentation University of J I Crete, P.O. Box 2208, 71003 Voutes,Methods Heraklion, and Greece Methods and 3State Key Laboratory of AtmosphericData Systems Boundary Layer Physics and AtmosphericData Systems Chemistry, Back Close Discussions Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, ChinaOpen Access Open Access Full Screen / Esc Geoscientific Received: 5 February 2013 –Geoscientific Accepted: 5 March 2013 – Published: 13 March 2013 Model Development Model Development Printer-friendly Version Correspondence to: C. M. Pavuluri ([email protected]) Discussions Interactive Discussion Open Access Published by Copernicus Publications on behalfOpen Access of the European Geosciences Union. Hydrology and Hydrology and Earth System 6589 Earth System Sciences Sciences Discussions Open Access Open Access Ocean Science Ocean Science Discussions Open Access Open Access Solid Earth Solid Earth Discussions Open Access Open Access The Cryosphere The Cryosphere Discussions Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | Abstract ACPD High aerosol loadings are prevalent in the atmosphere of East Asia, where the aerosols impact the Earth’s climate system and human health; however, their sources and sea- 13, 6589–6629, 2013 sonal variations are not clearly understood. To better understand the sources of water- 5 soluble ionic species and trace metals in Northeast Asia, we studied atmospheric Water-soluble ionic 2− aerosol samples collected in Sapporo, northern Japan for one-year period. SO4 (aver- species and trace age 3.47±1.03µgm−3) was found as the most abundant ionic species, which accounted metals in Sapporo for on average 43 ± 15 % of the measured total ionic mass followed by Cl− (13 ± 12 %) aerosols ≈ NO− ≈ Na+ > NH+ > Ca2+ > Mg2+ > K+ > MSA−. Among the metals determined, Ca 3 4 C. M. Pavuluri et al. 10 was found as the most abundant (45±5.2 %) followed by Fe (27±4.5 %), Al (21±3.1 %), Zn (3.2 ± 1.7), Ti, Mn, Ni, Pb, Cu, V, As, Cr and Cd. Based on factor analysis, linear relations of selected species with biomarkers, and backward air mass trajectories, we found that long-range atmospheric transport of soil dust (∼ 33 %) from arid regions of Title Page Mongolia and/or Northeast China is a major source for Sapporo aerosols as well as ter- Abstract Introduction 15 restrial biogenic emissions (≥ 24 %) including microbial activities and biomass burning mostly from distant source region(s) (e.g. Siberia). We also found that the contributions Conclusions References of soil dust to the aerosols maximized in early spring whereas those of vegetational Tables Figures emissions maximized in spring/summer. Contributions of microbial activities to aerosols peaked in autumn whereas forest fires/biomass burning peaked in autumn/winter. On J I 20 the contrary, fossil fuel combustion/industrial activities and oceanic emissions to Sap- poro aerosols are suggested to be rather minor. This study also suggests that fungal J I spores contribute to some trace metals (i.e. Ni, Cu, As) while pollen contributes to Zn in aerosols. Back Close Full Screen / Esc 1 Introduction Printer-friendly Version 25 Atmospheric aerosols have an impact on the Earth’s climate system directly by absorb- Interactive Discussion ing and reflecting solar radiation and indirectly by acting as cloud condensation (CCN) 6590 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | and ice nuclei (IN) and thus altering their hygroscopic properties on local, regional and global scales (Ramanathan et al., 2001; Poschl¨ et al., 2010). They also have an ACPD adverse effect on the human health (Nel, 2005). Such impacts of aerosols are largely 13, 6589–6629, 2013 depend on aerosol loading and chemical composition (Baustian et al., 2012; Deandreis´ 5 et al., 2012; Dentener et al., 1996; Nel, 2005; Schaumann et al., 2004; Sciare et al., 2005; Zhang et al., 2012) that are spatially and seasonally highly variable in the lower Water-soluble ionic atmosphere. Aerosol concentrations vary in the range of 1–100 µgm−3 and their dom- species and trace inant chemical components are characterized by sulfate, nitrate, ammonium, sea salt, metals in Sapporo minerals, organics and elemental carbon, each of which typically contribute about 10– aerosols 10 30 % of the overall mass load (Poschl,¨ 2005). 2− C. M. Pavuluri et al. Aerosol SO4 could affect the radiation budget directly by reflecting solar radiation and indirectly by altering the physical properties of aerosols and the CCN activity (Deandreis´ et al., 2012). Inorganic salts are more water-soluble and their solubility Title Page is much higher than organics, enhancing CCN activity of the particles (Zhang et al., 15 2012). On the other hand, mineral dust adds complexity, because it can play a signif- Abstract Introduction icant role in radiative forcing (Dentener et al., 1996) as well as in the uptake of acidic gases (Goodman et al., 2000). Trace elements are typically present in elevated con- Conclusions References centrations, especially in urban aerosols, and can play an important role in the risk of Tables Figures human health due to their high bioreactivity (Moreno et al., 2011; Schaumann et al., 20 2004). J I High aerosol loadings are commonly observed in East Asia due to anthropogenic ac- tivities (Carmichael et al., 2009). Radiative forcing and climatic effects over East Asia J I have been shown to be large (Nakajima et al., 2007) with significant seasonal varia- Back Close tions due to the enhanced concentrations of dust in spring (Li-Xia and Zhi-Wei, 2011) 2− 25 and/or SO4 in summer (Su et al., 2012). East Asian aerosols, including dusts from arid Full Screen / Esc regions in Mongolia and North China, could be further transported across the Pacific Ocean (Alfaro et al., 2003; Kawamura et al., 2004; Uno et al., 2011) with an impact Printer-friendly Version on the regional to global climate. However, the aerosol composition, sources and sea- sonal variations, which are crucial in reducing the uncertainty in modeling of the aerosol Interactive Discussion 6591 Discussion Paper | Discussion Paper | Discussion Paper | Discussion Paper | impacts, are still far from being fully understood, despite the extensive studies over the past decade (e.g. Huebert et al., 2003; Nakajima et al., 2007). For example, Huang ACPD et al. (2006) reported an underestimation of the annual averaged model-simulated 13, 6589–6629, 2013 aerosol optical depth (AOD) by ∼ 45%. They interpreted that the obtained negative 2− 5 intercept is due to the inclusion of only the anthropogenic aerosols (SO4 , black car- bon and organic carbon), suggesting that the contributions from natural sources might Water-soluble ionic also be significant in this region. species and trace It is generally believed that anthropogenic activities (largely coal combustion) and metals in Sapporo 2− volcanic emissions are two major sources of particulate non-sea-salt (nss)-SO4 (An- aerosols 10 dres and Kasgnoc, 1998; Moore et al., 2006; Smith et al., 2011). Biological produc- 2− C. M. Pavuluri et al. tion of dimethylsulfide (DMS) is also considered as a significant source of nss-SO4 2− at least in marine regions (Moore et al., 2006; Oduro et al., 2012). Unlike nss-SO4 , − methanesulfonate (MSA ) can only be produced by the oxidation of DMS that origi- Title Page − 2− nates from the microbial activity in the ocean. Abundant levels of MSA and nss-SO4 15 were reported in the ocean/coastal atmosphere (Bates et al., 1992; Gaston et al., 2010; Abstract Introduction Gondwe et al., 2004; Legrand and Pasteur, 1998; Yang et al., 2009; Kouvarakis et al., Conclusions References 2002; Mihalopoulos et al., 1997). Recently, Miyazaki et al. (2012) reported significant − concentrations
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