Decomposing PM2.5 concentrations in urban environments into meaningful factors: 1. Separating the contribution of local anthropogenic activities from background and long-range transport.

Fine particulate matter (PM2.5) is a complex mixture of aerosol particles with varying properties and sources, both local and distant. In areas lacking detailed monitoring of PM2.5 speciation, the common source-apportionment analyses are not applicable. This study demonstrates an alternative framework for estimating sources and processes that affect observed PM2.5 concentrations when information on the particle composition is unavailable. Eight years (2012-2019) of half-hourly PM2.5 observations from 10 air quality monitoring (AQM) stations, clustered according to their airmass transport sector were analyzed, using Non-negative Matrix Factorization (NMF). Factors were determined based on their variation in time, space, and between airmass sectors. Employing a supervised machine-learning model provided insights into the relationships between the extracted factors, meteorological parameters and co-measured airborne pollutants. Factor interpretations were evaluated through comparisons with measurements of PM2.5 species from a nearby Surface PARTiculate mAtter Network (SPARTAN) station. The NMF successfully separated background factors from an urban anthropogenic-activity factor, with the latter accounting for approximately 60 % of the observed PM2.5 levels in Tel Aviv (∼10±6µg/m3). Positive monotonic relationships were observed between the PM2.5 urban anthropogenic-activity factor and measurements of nitrogen oxides (NOx) and absolute humidity (AH), representing the impact of traffic emissions and hygroscopic growth, respectively. The summer background factor was found to represent long-range transport (LRT) from Europe, showing a good agreement (R2 = 0.81) with ammonium sulphate concentrations. Our results demonstrate that a spatial NMF analysis can reliably estimate contributions of different sources with distinct compositions and properties to the total observed PM2.5. Using such an analysis, future environmental health studies could assess health risks associated with exposure to distinct PM2.5 fractions. This information may assist decision makers to set environmental targets for abating PM2.5 with specific compositions and properties.

Decomposing PM2.5 concentrations in urban environments into meaningful factors 2. Extracting the contribution of traffic-related exhaust emissions.

Vehicle-emitted fine particulate matter (PM2.5) has been associated with significant health outcomes and environmental risks. This study estimates the contribution of traffic-related exhaust emissions (TREE) to observed PM2.5 using a novel factorization framework. Specifically, co-measured nitrogen oxides (NOx) concentrations served as a marker of vehicle-tailpipe emissions and were integrated into the optimization of a Non-negative Matrix Factorization (NMF) analysis to guide the factor extraction. The novel TREE-NMF approach was applied to long-term (2012-2019) PM2.5 observations from air quality monitoring (AQM) stations in two urban areas. The extracted TREE factor was evaluated against co-measured black carbon (BC) and PM2.5 species to which the TREE-NMF optimization was blind. The contribution of the TREE factor to the observed PM2.5 concentrations at an AQM station from the first location showed close agreement (R2=0.79) with monitored BC data. In the second location, a comparison of the extracted TREE factor with measurements at a nearby Surface PARTiculate mAtter Network (SPARTAN) station revealed moderate correlations with PM2.5 species commonly associated with fuel combustion, and a good linear regression fit with measured equivalent BC concentrations. The estimated concentrations of the TREE factor at the second location accounted for 7-11 % of the observed PM2.5 in the AQM stations. Moreover, analysis of specific days known to be characterized by little traffic emissions suggested that approximately 60-78 % of the traffic-related PM2.5 concentrations could be attributed to particulate traffic-exhaust emissions. The methodology applied in this study holds great potential in areas with limited monitoring of PM2.5 speciation, in particular BC, and its results could be valuable for both future environmental health research, regional radiative forcing estimates, and promulgation of tailored regulations for traffic-related air pollution abatement.