1. Rolling vs. seasonal PMF : real-world multi-site and synthetic dataset comparisonMarta Via, Gang Chen, Francesco Canonaco, Kaspar Rudolf Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, 2022, izvirni znanstveni članek Opis: Abstract. Particulate matter (PM) has become a major concern in terms of human health
and climate impact. In particular, the source apportionment (SA) of organic
aerosols (OA) present in submicron particles (PM1) has gained relevance
as an atmospheric research field due to the diversity and complexity of its
primary sources and secondary formation processes. Moreover, relatively
simple but robust instruments such as the Aerosol Chemical Speciation
Monitor (ACSM) are now widely available for the near-real-time online
determination of the composition of the non-refractory PM1. One of the
most used tools for SA purposes is the source-receptor positive matrix
factorisation (PMF) model. Even though the recently developed rolling PMF technique has
already been used for OA SA on ACSM datasets, no study has assessed its
added value compared to the more common seasonal PMF method using a practical
approach yet. In this paper, both techniques were applied to a synthetic
dataset and to nine European ACSM datasets in order to spot the main output
discrepancies between methods. The main advantage of the synthetic dataset
approach was that the methods' outputs could be compared to the expected
“true” values, i.e. the original synthetic dataset values. This approach
revealed similar apportionment results amongst methods, although the
rolling PMF profile's adaptability feature proved to be advantageous, as it
generated output profiles that moved nearer to the truth points. Nevertheless,
these results highlighted the impact of the profile anchor on the solution,
as the use of a different anchor with respect to the truth led to
significantly different results in both methods. In the multi-site study,
while differences were generally not significant when considering year-long
periods, their importance grew towards shorter time spans, as in intra-month
or intra-day cycles. As far as correlation with external measurements is
concerned, rolling PMF performed better than seasonal PMF globally for the ambient
datasets investigated here, especially in periods between seasons. The results of this
multi-site comparison coincide with the synthetic dataset in terms of
rolling–seasonal similarity and rolling PMF reporting moderate improvements. Altogether, the
results of this study provide solid evidence of the robustness of both
methods and of the overall efficiency of the recently proposed rolling PMF
approach. Ključne besede: particulate matter, synthetic dataset comparison, source apportionment, organic aerosols Objavljeno v RUNG: 10.05.2024; Ogledov: 978; Prenosov: 7 Celotno besedilo (2,03 MB) Gradivo ima več datotek! Več... |
2. Towards a better understanding of fine PM sources : online and offline datasets combination in a single PMFMarta Via, Jesús Yus-Díez, Francesco Canonaco, Jean-Eudes Petit, Philip Hopke, Cristina Reche, Marco Pandolfi, Matic Ivančič, Martin Rigler, Andre S. H. Prevot, 2023, izvirni znanstveni članek Ključne besede: multi-time resolution, source apportionment, submicronic particulate matter, positive matrix factorisation, PMF, multilinear engine, SoFi, ME2, organic sources, metals Objavljeno v RUNG: 24.10.2023; Ogledov: 1701; Prenosov: 8 Celotno besedilo (3,23 MB) Gradivo ima več datotek! Več... |
3. European Aerosol Phenomenology - 8: Harmonised Source Apportionment of Organic Aerosol using 22 Year-long ACSM/AMS DatasetsGang Chen, Francesco Canonaco, Anna Tobler, Griša Močnik, MaríaCruz Minguillón, André Prévôt, Marta Via, 2022, izvirni znanstveni članek Opis: Organic aerosol (OA) is a key component to total submicron particulate matter (PM1), and comprehensive knowledge of OA sources across Europe is crucial to mitigate PM1 levels. Europe has a well-established air quality research infrastructure from which yearlong datasets using 21 aerosol chemical speciation monitors (ACSMs) and 1 aerosol mass spectrometer (AMS) were gathered during 2013-2019. It includes 9 non-urban and 13 urban sites. This study developed a state-of-the-art source apportionment protocol to analyse long-term OA mass spectrum data by applying the most advanced source apportionment strategies (i.e., rolling PMF, ME-2, and bootstrap). This harmonised protocol was followed strictly for all 22 datasets, making the source apportionment results more comparable. In addition, it enables the quantifications of the most common OA components such as hydrocarbon-like OA (HOA), biomass burning OA (BBOA), cooking-like OA (COA), more oxidised-oxygenated OA (MO-OOA), and less oxidised-oxygenated OA (LO-OOA). Other components such as coal combustion OA (CCOA), solid fuel OA (SFOA: mainly mixture of coal and peat combustion), cigarette smoke OA (CSOA), sea salt (mostly inorganic but part of the OA mass spectrum), coffee OA, and ship industry OA could also be separated at a few specific sites. Oxygenated OA (OOA) components make up most of the submicron OA mass (average = 71.1%, range from 43.7 to 100%). Solid fuel combustion-related OA components (i.e., BBOA, CCOA, and SFOA) are still considerable with in total 16.0% yearly contribution to the OA, yet mainly during winter months (21.4%). Overall, this comprehensive protocol works effectively across all sites governed by different sources and generates robust and consistent source apportionment results. Our work presents a comprehensive overview of OA sources in Europe with a unique combination of high time resolution (30-240 minutes) and long-term data coverage (9-36 months), providing essential information to improve/validate air quality, health impact, and climate models. Ključne besede: air pollution, source apportionment, organic aeroosl, black carbon Objavljeno v RUNG: 03.06.2022; Ogledov: 3412; Prenosov: 20 Celotno besedilo (4,69 MB) Gradivo ima več datotek! Več... |
4. Equal abundance of summertime natural and wintertime anthropogenic Arctic organic aerosolsVaios Moschos, Katja Dzepina, Deepika Bhattu, Houssni Lamkaddam, Roberto Casotto, Kaspar R. Daellenbach, Francesco Canonaco, Pragati Rai, Wenche Aas, Silvia Becagli, Giulia Calzolai, Konstantinos Eleftheriadis, Claire E. Moffett, Jürgen Schnelle-Kreis, Mirko Severi, Sangeeta Sharma, Henrik Skov, Mika Vestenius, Wendy Zhang, Hannele Hakola, Heidi Hellén, Lin Huang, Jean-Luc Jaffrezo, Andreas Massling, Jakob K. Nøjgaard, Tuuka Petäjä, Olga Popovicheva, Rebecca J. Sheesley, Rita Traversi, Karl Espen Yttri, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Imad El Haddad, 2022, izvirni znanstveni članek Opis: Aerosols play an important yet uncertain role in modulating the radiation balance of the sensitive Arctic atmosphere. Organic aerosol is one of the most abundant, yet least understood, fractions of the Arctic aerosol mass. Here we use data from eight observatories that represent the entire Arctic to reveal the annual cycles in anthropogenic and biogenic sources of organic aerosol. We show that during winter, the organic aerosol in the Arctic is dominated by anthropogenic emissions, mainly from Eurasia, which consist of both direct combustion emissions and long-range transported, aged pollution. In summer, the decreasing anthropogenic pollution is replaced by natural emissions. These include marine secondary, biogenic secondary and primary biological emissions, which have the potential to be important to Arctic climate by modifying the cloud condensation nuclei properties and acting as ice-nucleating particles. Their source strength or atmospheric processing is sensitive to nutrient availability, solar radiation, temperature and snow cover. Our results provide a comprehensive understanding of the current pan-Arctic organic aerosol, which can be used to support modelling efforts that aim to quantify the climate impacts of emissions in this sensitive region. Ključne besede: Arctic, Organic aerosols, Emission sources, Climate change Objavljeno v RUNG: 01.03.2022; Ogledov: 2477; Prenosov: 0 Gradivo ima več datotek! Več... |
5. Characterization of non-refractory (NR) PM[sub]1 and source apportionment of organic aerosol in Kraków, PolandAnna Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, 2021, izvirni znanstveni članek Opis: Kraków is routinely affected by very high air pollution levels, especially during the winter months. Although a lot of effort has been made to characterize ambient aerosol, there is a lack of online and long-term measurements of non-refractory aerosol. Our measurements at the AGH University of Science and Technology provide the online long-term chemical composition of ambient submicron particulate matter (PM1) between January 2018 and April 2019. Here we report the chemical characterization of non-refractory submicron aerosol and source apportionment of the organic fraction by positive matrix factorization (PMF). In contrast to other long-term source apportionment studies, we let a small PMF window roll over the dataset instead of performing PMF over the full dataset or on separate seasons. In this way, the seasonal variation in the source profiles can be captured. The uncertainties in the PMF solutions are addressed by the bootstrap resampling strategy and the random a-value approach for constrained factors.
We observe clear seasonal patterns in the concentration and composition of PM1, with high concentrations during the winter months and lower concentrations during the summer months. Organics are the dominant species throughout the campaign. Five organic aerosol (OA) factors are resolved, of which three are of a primary nature (hydrocarbon-like OA (HOA), biomass burning OA (BBOA) and coal combustion OA (CCOA)) and two are of a secondary nature (more oxidized oxygenated OA (MO-OOA) and less oxidized oxygenated OA (LO-OOA)). While HOA contributes on average 8.6 % ± 2.3 % throughout the campaign, the solid-fuel-combustion-related BBOA and CCOA show a clear seasonal trend with average contributions of 10.4 % ± 2.7 % and 14.1 %, ±2.1 %, respectively. Not only BBOA but also CCOA is associated with residential heating because of the pronounced yearly cycle where the highest contributions are observed during wintertime. Throughout the campaign, the OOA can be separated into MO-OOA and LO-OOA with average contributions of 38.4 % ± 8.4 % and 28.5 % ± 11.2 %, respectively. Ključne besede: air pollution, PM1, organic aerosol, black carbon, source apportionment, PMF Objavljeno v RUNG: 08.10.2021; Ogledov: 2818; Prenosov: 0 Gradivo ima več datotek! Več... |
6. Sarajevo Canton Winter Field Campaign 2018 : particulate air pollution in a global hotspotKatja Džepina, Vaios Moschos, Anna Tobler, Francesco Canonaco, Deepika Bhattu, Roberto Casotto, Athanasia Vlachou, Jasna Huremović, Sabina Žero, Griša Močnik, 2020, objavljeni povzetek znanstvenega prispevka na konferenci Opis: Nowadays, urban centres in countries of the Western Balkan region (including Bosnia and Herzegovina (B&H)) are experiencing some of the poorest European and global air quality due to the extensive use of solid fuels (e.g., wood, coal) and old vehicle fleet. Western Balkan countries lack state-of-the-art atmospheric sciences research despite high levels of ambient pollution, which makes the efforts to understand the mechanisms of their air pollution imperative. The city of Sarajevo, the capital of B&H, is situated in a basin surrounded by mountains. Particularly during the winter months, topography and meteorology cause significant pollution episodes.
The Sarajevo Canton Winter Field Campaign 2018 (SAFICA) took place from Dec 04, 2017 to Mar 15, 2018 with on-line aerosol measurements and collection of daily, continuous filter PM10 samples for off-line laboratory analyses. SAFICA aimed to give the first detailed characterization of the Western Balkans aerosol composition including organic aerosol (OA) to elucidate aerosol emission sources and atmospheric processing and to estimate the adverse health effects. PM10 samples (ntotal=180) were collected at four sites in the Sarajevo Canton: a) Bjelave and b) Pofalići (urban background); c) Otoka (urban); d) Ivan Sedlo (remote). The urban sites were distributed along the city basin to study the pollutants’ urban evolution and the remote site was chosen to compare urban to background air masses.
SAFICA PM10 samples underwent different off-line laboratory chemical analyses: 1) Bulk chemical composition of the total filter-collected water-soluble inorganic and OA by a high-resolution Aerodyne Aerosol Mass Spectrometer (AMS). The measured AMS OA spectra were further analysed by Positive Matrix Factorization (PMF) using the graphical user interface SoFi (Source Finder) to separate OA into subtypes characteristic for OA sources and atmospheric processes. 2) Organic and elemental carbon (OC/EC), water-soluble organic carbon, polycyclic aromatic hydrocarbons, levoglucosan, and 14C content of total carbon to evaluate OA chemical composition. 3) Major inorganic anions and cations to evaluate aerosol inorganic species. 4) Metal content in aerosol determined by two analytical techniques (AAS and ICP-MS). SAFICA on-line measurements of black carbon (Aethalometer) and the particle number concentration (Condensation Particle Counter and Optical Particle Sizer) enabled the insights into the daily evolution of primary pollutants and an assessment of aerosol size and number distribution.
The combined SAFICA results for on- and off-line measurements will be presented. Our results show that the carbon-containing species make ~2/3 of PM10 mass and the majority are oxygenated, water-soluble OA species with an average OM/OC = 1.9 (Fig.1). Urban air pollution crises in the Western Balkan will be put in the context of local, regional and global air quality. Finally, we will present the scientific questions opened by SAFICA, including the advantages and limitations of SAFICA data set, and give the recommendations for future studies. Ključne besede: Sarajevo, urban air pollution, PM10, PM2.5 Objavljeno v RUNG: 26.05.2021; Ogledov: 3819; Prenosov: 25 Povezava na celotno besedilo Gradivo ima več datotek! Več... |
7. Chemical characterization of PM2.5 and source apportionment of organic aerosol in New Delhi, IndiaAnna Tobler, Deepika Bhattu, Francesco Canonaco, Vipul Lalchandani, Ashutosh Shukla, Navaneeth Thamban, Suneeti Mishra, Atul Srivastava, Deewan Bisht, Suresh Tiwari, Surender Singh, Griša Močnik, Urs Baltensperger, Sachchida Tripathi, J. G. Slowik, André S. H. Prévôt, 2020, izvirni znanstveni članek Opis: Delhi is one of the most polluted cities worldwide and a comprehensive understanding and deeper insight into the air pollution and its sources is of high importance. We report 5 months of highly time-resolved measurements of non-refractory PM2.5 and black carbon (BC). Additionally, source apportionment based on positive matrix factorization (PMF) of the organic aerosol (OA) fraction is presented. The highest pollution levels are observed during winter in December/January. During that time, also uniquely high chloride concentrations are measured, which are sometimes even the most dominant NR-species in the morning hours. With increasing temperature, the total PM2.5 concentration decreases steadily, whereas the chloride concentrations decrease sharply. The concentrations measured in May are roughly 6 times lower than in December/January. PMF analysis resolves two primary factors, namely hydrocarbon-like (traffic-related) OA (HOA) and solid fuel combustion OA (SFC-OA), and one or two secondary factors depending on the season. The uncertainties of the PMF analysis are assessed by combining the random a-value approach and the bootstrap resampling technique of the PMF input. The uncertainties for the resolved factors range from ±18% to ±19% for HOA, ±7% to ±19% for SFC-OA and ±6 % to ±11% for the OOAs. The average correlation of HOA with eBCtr is R2 = 0.40, while SFC-OA has a correlation of R2 = 0.78 with eBCsf. Anthracene (m/z 178) and pyrene (m/z 202) (PAHs) are mostly explained by SFC-OA and follow its diurnal trend (R2 = 0.98 and R2 = 0.97). The secondary oxygenated aerosols are dominant during daytime. The average contribution during the afternoon hours (1 pm–5 pm) is 59% to the total OA mass, with contributions up to 96% in May. In contrast, the primary sources are more important during nighttime: the mean nightly contribution (22 pm–3 am) to the total OA mass is 48%, with contributions up to 88% during some episodes in April. Ključne besede: New Delhi, PM2.5, Source apportionment, PMF Objavljeno v RUNG: 20.07.2020; Ogledov: 3498; Prenosov: 0 Gradivo ima več datotek! Več... |