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    The impact of biomass burning and aqueous-phase processing on air quality: A multi-year source apportionment study in the Po Valley, Italy
    (Katlenburg-Lindau : EGU, 2020) Paglione, Marco; Gilardoni, Stefania; Rinaldi, Matteo; Decesari, Stefano; Zanca, Nicola; Sandrini, Silvia; Giulianelli, Lara; Bacco, Dimitri; Ferrari, Silvia; Poluzzi, Vanes; Scotto, Fabiana; Trentini, Arianna; Poulain, Laurent; Herrmann, Hartmut; Wiedensohler, Alfred; Canonaco, Francesco; Prévôt, André S.H.; Massoli, Paola; Carbone, Claudio; Facchini, Maria Cristina; Fuzzi, Sandro
    The Po Valley (Italy) is a well-known air quality hotspot characterized by particulate matter (PM) levels well above the limit set by the European Air Quality Directive and by the World Health Organization, especially during the colder season. In the framework of Emilia-Romagna regional project "Supersito", the southern Po Valley submicron aerosol chemical composition was characterized by means of high-resolution aerosol mass spectroscopy (HR-AMS) with the specific aim of organic aerosol (OA) characterization and source apportionment. Eight intensive observation periods (IOPs) were carried out over 4 years (from 2011 to 2014) at two different sites (Bologna, BO, urban background, and San Pietro Capofiume, SPC, rural background), to characterize the spatial variability and seasonality of the OA sources, with a special focus on the cold season. On the multi-year basis of the study, the AMS observations show that OA accounts for averages of 45 ± 8 % (ranging from 33 % to 58 %) and 46 ± 7 % (ranging from 36 % to 50 %) of the total non-refractory submicron particle mass (PM1-NR) at the urban and rural sites, respectively. Primary organic aerosol (POA) comprises biomass burning (23±13 % of OA) and fossil fuel (12±7 %) contributions with a marked seasonality in concentration. As expected, the biomass burning contribution to POA is more significant at the rural site (urban / rural concentration ratio of 0.67), but it is also an important source of POA at the urban site during the cold season, with contributions ranging from 14 % to 38 % of the total OA mass. Secondary organic aerosol (SOA) contributes to OA mass to a much larger extent than POA at both sites throughout the year (69 ± 16 % and 83 ± 16 % at the urban and rural sites, respectively), with important implications for public health. Within the secondary fraction of OA, the measurements highlight the importance of biomass burning aging products during the cold season, even at the urban background site. This biomass burning SOA fraction represents 14 %-44 % of the total OA mass in the cold season, indicating that in this region a major contribution of combustion sources to PM mass is mediated by environmental conditions and atmospheric reactivity. © 2020 Author(s).
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    The acidity of atmospheric particles and clouds
    (Katlenburg-Lindau : EGU, 2020) Pye, Havala O.T.; Nenes, Athanasios; Alexander, Becky; Ault, Andrew P.; Barth, Mary C.; Clegg, Simon L.; Collett Jr, Jeffrey L.; Fahey, Kathleen M.; Hennigan, Christopher J.; Herrmann, Hartmut; Kanakidou, Maria; Kelly, James T.; Ku, I-Ting; McNeill, V. Faye; Riemer, Nicole; Schaefer, Thomas; Shi, Guoliang; Tilgner, Andreas; Walker, John T.; Wang, Tao; Weber, Rodney; Xing, Jia; Zaveri, Rahul A.; Zuend, Andreas
    Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO3, NH3, HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale. © 2020 Author(s).