For reducing health impacts from air pollution, it is important to know the sources contributing to human exposure. This study systematically reviewed and analysed available source apportionment studies on particulate matter (of diameter of 10 and 2.5 microns, PM10 and PM2.5) performed in cities to estimate typical shares of the sources of pollution by country and by region. A database with city source apportionment records, estimated with the use of receptor models, was also developed and available at the website of the World Health Organization. Systematic Scopus and Google searches were performed to retrieve city studies of source apportionment for particulate matter. Six source categories were defined. Country and regional averages of source apportionment were estimated based on city population weighting. A total of 419 source apportionment records from studies conducted in cities of 51 countries were used to calculate regional averages of sources of ambient particulate matter. Based on the available information, globally 25% of urban ambient air pollution from PM2.5 is contributed by traffic, 15% by industrial activities, 20% by domestic fuel burning, 22% from unspecified sources of human origin, and 18% from natural dust and salt. The available source apportionment records exhibit, however, important heterogeneities in assessed source categories and incompleteness in certain countries/regions. Traffic is one important contributor to ambient PM in cities. To reduce air pollution in cities and the substantial disease burden it causes, solutions to sustainably reduce ambient PM from traffic, industrial activities and biomass burning should urgently be sought. However, further efforts are required to improve data availability and evaluation, and possibly to combine with other types of information in view of increasing usefulness for policy making.JRC.H.2-Air and Climat

Chemically resolved atmospheric aerosol data sets from the largest intercomparison of the Aerodyne aerosol chemical speciation monitors (ACSMs) performed to date were collected at the French atmospheric supersite SIRTA. In total 13 quadrupole ACSMs (Q-ACSM) from the European ACTRIS ACSM network, one time-of-flight ACSM (ToF-ACSM), and one high-resolution ToF aerosol mass spectrometer (AMS) were operated in parallel for about 3 weeks in November and December~2013. Part 1 of this study reports on the accuracy and precision of the instruments for all the measured species. In this work we report on the intercomparison of organic components and the results from factor analysis source apportionment by positive matrix factorisation (PMF) utilising the multilinear engine 2 (ME-2). Except for the organic contribution of mass-to-charge ratio m/z 44 to the total organics (f₄₄), which varied by factors between 0.6 and 1.3 compared to the mean, the peaks in the organic mass spectra were similar among instruments. The m/z 44 differences in the spectra resulted in a variable f₄₄ in the source profiles extracted by ME-2, but had only a minor influence on the extracted mass contributions of the sources. The presented source apportionment yielded four factors for all 15 instruments: hydrocarbon-like organic aerosol (HOA), cooking-related organic aerosol (COA), biomass burning-related organic aerosol (BBOA) and secondary oxygenated organic aerosol (OOA). ME-2 boundary conditions (profile constraints) were optimised individually by means of correlation to external data in order to achieve equivalent / comparable solutions for all ACSM instruments and the results are discussed together with the investigation of the influence of alternative anchors (reference profiles). A comparison of the ME-2 source apportionment output of all 15 instruments resulted in relative standard deviations (SD) from the mean between 13.7 and 22.7 % of the source's average mass contribution depending on the factors (HOA: 14.3 ± 2.2 %, COA: 15.0 ± 3.4 %, OOA: 41.5 ± 5.7 %, BBOA: 29.3 ± 5.0 %). Factors which tend to be subject to minor factor mixing (in this case COA) have higher relative uncertainties than factors which are recognised more readily like the OOA. Averaged over all factors and instruments the relative first SD from the mean of a source extracted with ME-2 was 17.2 %.

As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall – early-winter period (November–December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM₁) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM₁ total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r² > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM₁, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.

This work reviews the existing methodologies for source apportionment and sensitivity analysis to identify key differences and stress their implicit limitations. The emphasis is laid on the differences between source impacts (sensitivity analysis) and contributions (source apportionment) obtained by using four different methodologies: brute-force top-down, brute-force bottom-up, tagged species and decoupled direct method (DDM). A simple theoretical example to compare these approaches is used highlighting differences and potential implications for policy. When the relationships between concentration and emissions are linear, impacts and contributions are equivalent concepts. In this case, source apportionment and sensitivity analysis may be used indifferently for both air quality planning purposes and quantifying source contributions. However, this study demonstrates that when the relationship between emissions and concentrations is nonlinear, sensitivity approaches are not suitable to retrieve source contributions and source apportionment methods are not appropriate to evaluate the impact of abatement strategies. A quantification of the potential nonlinearities should therefore be the first step prior to source apportionment or planning applications, to prevent any limitations in their use. When nonlinearity is mild, these limitations may, however, be acceptable in the context of the other uncertainties inherent to complex models. Moreover, when using sensitivity analysis for planning, it is important to note that, under nonlinear circumstances, the calculated impacts will only provide information for the exact conditions (e.g. emission reduction share) that are simulated.

A database of atmospheric particulate matter emission source profiles in Europe (SPECIEUROPE) was developed by the Joint Research Center in the framework of the Forum for air quality modeling in Europe (FAIRMODE, Working Group 3). It contains the chemical composition of particulate matter (PM) emission sources reported in the scientific literature and reports drafted by competent authorities. The first release of SPECIEUROPE consists of 151 measured profiles (original), 13 composite (merging different subcategories of similar sources), 6 calculated (from stoichiometric composition) and 39 profiles derived from source apportionment studies. Each profile is related to one or more source categories or subcategories. The sources with the highest PM relative mass toxic pollutants such as PAHs are fuel oil burning, ship emissions, coke burning and wood burning. Heavy metals are most abundant in metal processing activities while halogens are mostly present in fertilizer production, coal burning and metallurgic sector. Anhydrosugars are only measured in biomass and wood burning source categories. The alkaline earth metals are mostly present in road dust, cement production, soil dust and sometime coal burning. Source categories as traffic and industrial, which contain heterogeneous subcategories, show the greatest internal variability. The relationships between source profiles were also explored using a cluster analysis approach based upon the Standardized Identity Distance (SID) indicator. The majority of profiles are distributed in 8 clusters, which for heterogeneous sources do not correspond to the commonly used broad source category. For example the industrial source spread among three clusters with different characteristics.JRC.H.2-Air and Climat