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A source apportionment scheme based on gas and aerosol phase reactive tracers has been implemented in the chemical-transport model FARM, to efficiently estimate contributions of different sources to ambient concentrations. The on-line scheme deals with all the main processes that the chemical species undergo in the model, to enhance consistency with the calculation of bulk concentrations. The fate of precursors through gas-phase chemical reactions is followed by an efficient solver that determines their incremental reactivity, while the contributions to the secondary particulate species from their gaseous precursors is determined by assuming the thermodynamic equilibrium between the two phases. The paper details the new employed methodologies and illustrates the application of the apportionment scheme (based on 6 source sectors) to PM10 and O3, simulated on three domains of different dimensions in Italy, all sharing the same horizontal resolution and a common region (Lombardy). Spatial patterns of results show, on average, a relevant contribution of heating on PM10 concentration in January, with local hotspots dominated by road traffic. Contributions appear consistent in the three simulated domains, apart from the boundary conditions, influenced by the dimension of the domain. Hourly series of contributions to O3 concentrations in July at three selected sites show the dominance of boundary conditions, underlining the large scale of O3 formation. Finally, for PM10 components, the resulting sectorial contributions are compared with the impacts computed via the brute force method, showing that results are similar for elemental carbon and sulfate, while they are different for nitrate and ammonium, due to a different allocation of contributions and impacts between the methods. Each approach responds in principle to a different purpose, and their combined use provides possibly a wide set of information useful for addressing the different air quality management needs. [ABSTRACT FROM AUTHOR]

This work is an overview of the oxidative potential (OP) values up to date measured in Italy, with the aim to provide a picture of the spatial and seasonal variability of OP in the various geographical areas across Italy. The summarized works used the common acellular assays-based dithiothreitol (OPDTT), ascorbic acid (OPAA), glutathione (OPGSH), and 2′,7′-dichlorodfluorescein (OPDCFH) assays. The paper describes the association of OP responses with PM chemical composition, the sensitivity of various acellular OP assays to PM components and emission sources, and PM size distribution of the measured OP values. Our synthesis indicates that crustal and transition metals (e.g., Fe, Ni, Cu, Cr, Mn, Zn, and V), secondary ions and carbonaceous components (elemental carbon, EC, organic carbon, OC and water soluble carbon, WSOC) show significant correlations with OP across different urban and rural areas and size ranges. These chemical species are mainly associated with various PM sources, including residual/fuel oil combustion, traffic emissions, and secondary organic aerosol formation. Although the OP assays are sensitive to the same redox-active species, they differ in the association with PM chemical components. The DDT assay is mainly sensitive to the organic compounds that are mostly accumulated in the fine PM fraction, i.e., tracers of burning sources, and redox active organics associated with other markers of photochemical aging. In contrast, OPAA and OPGSH were mostly responsive to metals, mainly those related to non-exhaust traffic emissions (Cu, Zn, Cr, Fe, Ni, Mn, Sn, Cd, Pb), that are mainly accumulated in the coarse PM. Among the investigated sites, our synthesis shows larger OP values in Trentino region and the Po Valley, that may be explained by the high density of anthropogenic sources, and the orographic and meteorological characteristics, that favor the pollutants accumulation and aerosol photo-oxidative aging. [ABSTRACT FROM AUTHOR]