Attribution of aerosol particle number size distributions to main sources using an 11-year urban dataset

Abstract

Source apportionment was performed using size-segregated atmospheric particle number concentrations (PNCs) in 27 size channels over a diameter range of 6–1000 nm augmented by air pollutants with a time resolution of 1 h in Budapest for 11 full years. The input dataset was treated for the effect of the local meteorology using dispersion correction. Both the uncorrected dataset and corrected dataset were evaluated using positive matrix factorization for separate seasons. Six source types including nucleation, two road vehicle emission sources separated into a semi-volatile fraction and a solid-core fraction, a diffuse urban source, a secondary inorganic aerosol (SIA) source, and an ozone-associated secondary aerosol source were identified, characterized and quantified. The dispersion correction did not considerably change the profiles, diel variations or patterns of the sources, while it substantially modified the relative shares of the nucleation source in all seasons. The mean relative contributions of the traffic emissions (60 %) indicate that on-road motor vehicles were the leading source of particle numbers. The nucleation was responsible for 24 % of the PNC annually as a lower estimate. It exhibited a compound character consisting of photochemically induced nucleation and traffic-related nucleation. Its contributions were the highest in spring and the lowest in winter. The shares of the urban diffuse and SIA source types were the largest in autumn and winter and in spring and summer, respectively, but they were typically ⪅ 10 %. The O3-associated secondary aerosol made up the smallest (⪅ 3 %) contributions. The conditional bivariate probability function analysis showed considerable spatial variations in the source origin. The combination of the size-segregated particle number concentrations, wide overall range of the size channels, considerably long dataset, dispersion correction and modelling over separate seasons led jointly to a unique adaptation of the source apportionment and yielded novel and valuable insights into the urban aerosol sources and processes both for Budapest and in general.