Online coupling of pure O2 thermo-optical methods – 14C AMS for source apportionment of carbonaceous aerosols

Agrios, Konstantinos A.; Salazar, Gary; Zhang, Yanlin; Uglietti, Chiara; Battaglia, Michael; Luginbühl, Marc; Ciobanu, V.; Vonwiller, Matthias; Szidat, Sönke

doi:10.1016/j.nimb.2015.06.008

Cited by 27 publications

(45 citation statements)

References 12 publications

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“…Based on the instrumentation setup described in Agrios et al (2015) and on the method described in Zotter et al (2014b), radiocarbon analysis of TC and EC was conducted on a set of 33 filters. The 14 C content of blank filters was measured for TC only, as there was no EC found on these filters.…”

Section: C Analysismentioning

confidence: 99%

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

et al. 2018

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Abstract. Carbonaceous aerosols are related to adverse human health effects. Therefore, identification of their sources and analysis of their chemical composition is important. The offline AMS (aerosol mass spectrometer) technique offers quantitative separation of organic aerosol (OA) factors which can be related to major OA sources, either primary or secondary. While primary OA can be more clearly separated into sources, secondary (SOA) source apportionment is more challenging because different sources -anthropogenic or natural, fossil or non-fossil -can yield similar highly oxygenated mass spectra. Radiocarbon measurements provide unequivocal separation between fossil and non-fossil sources of carbon. Here we coupled these two offline methods and analysed the OA and organic carbon (OC) of different size fractions (particulate matter below 10 and 2.5 µm -PM 10 and PM 2.5 , respectively) from the Alpine valley of Magadino (Switzerland) during the years 2013 and 2014 (219 samples). The combination of the techniques gave further insight into the characteristics of secondary OC (SOC) which was rather based on the type of SOC precursor and not on the volatility or the oxidation state of OC, as typically considered. Out of the primary sources separated in this study, biomass burning OC was the dominant one in winter, with average concentrations of 5.36 ± 2.64 µg m −3 for PM 10 and 3.83 ± 1.81 µg m −3 for PM 2.5 , indicating that wood combustion particles were predominantly generated in the fine mode. The additional information from the size-segregated measurements revealed a primary sulfur-containing factor, mainly fossil, detected in the coarse size fraction and related to non-exhaust traffic emissions with a yearly average PM 10 (PM 2.5 ) concentration of 0.20 ± 0.24 µg m −3 (0.05 ± 0.04 µg m −3 ). A primary biological OC (PBOC) was also detected in the coarse mode peaking in spring and summer with a yearly average PM 10 (PM 2.5 ) concentration of 0.79 ± 0.31 µg m −3 (0.24 ± 0.20 µg m −3 ). The secondary OC was separated into two oxygenated, non-fossil OC factors which were identified based on their seasonal variability (i.e. summer and winter oxygenated organic carbon, OOC) and a third anthropogenic OOC factor which correlated with fossil OC mainly peaking in winter and spring, contributing on average 13 % ± 7 % (10 % ± 9 %) to the total OC in PM 10 (PM 2.5 ). The winter OOC was also connected to anthropogenic sources, contributing on average 13 % ± 13 % (6 % ± 6 %) to the total OC in PM 10 (PM 2.5 ). The summer OOC (SOOC), stemming from oxidation of biogenic emissions, was more pronounced in the fine mode, contributing on average 43 % ± 12 % (75 % ± 44 %) to the total OC in PM 10 (PM 2.5 ). In total the non-fossil OC significantly dominated the fossil OC throughout all seasons, by contributing on average 75 % ± 24 % to the total OC. The results also suggested that during the cold period the prevailing source was residential biomass burning while during the warm period primaryPublished by Copernicus Publications o...

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Section: C Analysismentioning

confidence: 99%

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

et al. 2018

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“…2). Recently the Sunset instrument was directly coupled to the zeolite trap of the GIS , which allows online 14 C measurements of the carbonaceous fractions separated in the Sunset system (Agrios et al, 2015). When combusted, the gaseous carbonaceous species pass through a MnO 2 bed heated to 850 • C for completing the oxidation to CO 2 , which is further transported by helium to the zeolite trap.…”

Section: Recent Optimisation In Oc/ec Separation and Ams Analysismentioning

confidence: 99%

“…Further the preparation and measurement time is significantly reduced because there is no need for offline combustion, resulting in a total measurement time of approximately 35 min per sample only. In addition, it not only allows for an automated protocol of standard injection for AMS calibration, but also offers the possibility for easy and regular (daily) survey of the 14 C background in the entire process line (Sunset-GIS-AMS) by analysis of variably sized standards and blanks if required (Agrios et al, 2015). Finally, the Sunset system enables continuous monitoring of the combustion process, reducing a potential bias due to charring, and the standardised and automated combustion protocol (Swiss 4S) ensures high reproducibility increasing the overall precision.…”

Section: Recent Optimisation In Oc/ec Separation and Ams Analysismentioning

confidence: 99%

“…For defining the contamination contribution of the overall instrument set-up (constant contamination) and the memory effect between subsequent samples of very different 14 C content and carbon mass (cross contamination), a series with varying amounts of solid grains of fossil NaOAc and the modern reference material oxalic acid II was combusted with the Sunset and measured for its 14 C content. The constant contaminant mass was estimated as 0.4 ± 0.2 µg carbon with a F 14 C of 0.8 ± 0.4 and for the cross contamination 0.5 ± 0.4 % of the carbon of the previous sample was found to mix with the next injection (Agrios et al, 2015).…”

Section: Radiocarbon Dating Uncertaintiesmentioning

confidence: 99%

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Radiocarbon dating of glacier ice: overview, optimisation, validation and potential

et al. 2016

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Abstract. High-altitude glaciers and ice caps from midlatitudes and tropical regions contain valuable signals of past climatic and environmental conditions as well as human activities, but for a meaningful interpretation this information needs to be placed in a precise chronological context. For dating the upper part of ice cores from such sites, several relatively precise methods exist, but they fail in the older and deeper parts, where plastic deformation of the ice results in strong annual layer thinning and a non-linear age-depth relationship. If sufficient organic matter such as plant, wood or insect fragments were found, radiocarbon ( 14 C) analysis would have thus been the only option for a direct and absolute dating of deeper ice core sections. However such fragments are rarely found and, even then, they would not be very likely to occur at the desired depth and resolution. About 10 years ago, a new, complementary dating tool was therefore introduced by our group. It is based on extracting the µg-amounts of the water-insoluble organic carbon (WIOC) fraction of carbonaceous aerosols embedded in the ice matrix for subsequent 14 C dating. Since then this new approach has been improved considerably by reducing the measurement time and improving the overall precision. Samples with ∼ 10 µg WIOC mass can now be dated with reasonable uncertainty of around 10-20 % (variable depending on sample age). This requires about 300 to 800 g of ice for WIOC concentrations typically found in midlatitude and low-latitude glacier ice. Dating polar ice with satisfactory age precision is still not possible since WIOC concentrations are around

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“…Many studies have revealed that organic matter (OM) is the largest fraction of ambient fine particles, typically comprising 20-90 % of the submicron particulate mass . Factor analysis of aerosol mass spectra from the Aerodyne aerosol mass spectrometer enables the deconvolution of OM into different factors based on their mass spectral fingerprints (Lanz et al, 2007;Aiken et al, 2009;Ulbrich et al, 2009). Such results provided valuable insights into the source and transformation processes of organic aerosols (OA) in the atmosphere (Lanz et al, 2010;Ng et al, 2011;Hildebrandt et al, 2011;Canonaco et al, 2013;Bougiatioti et al, 2014;Huang et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

Ulevičius

Byčenkienė²,

Bozzetti

et al. 2016

Atmos. Chem. Phys.

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In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM 1 ) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m −3 and black carbon (BC) up to 17 µg m −3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon ( 14 C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OC nf ) was the dominant fraction of PM 1 , with the primary (POC nf ) and secondary (SOC nf ) fractions contributing 26-44 % and 13-23 % to the total carbon (TC), respectively. 5-8 % of the TC had a primary fossil origin (POC f ), whereas the contribution of fossil secondary organic carbon (SOC f ) was 4-13 %. Nonfossil EC (EC nf ) and fossil EC (EC f ) ranged from 13-24 and 7-13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning. Published by CopernicusPublications on behalf of the European Geosciences Union. 5514 V. Ulevicius et al.: Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols

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Online coupling of pure O2 thermo-optical methods – 14C AMS for source apportionment of carbonaceous aerosols

Cited by 27 publications

References 12 publications

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

Advanced source apportionment of carbonaceous aerosols by coupling offline AMS and radiocarbon size-segregated measurements over a nearly 2-year period

Radiocarbon dating of glacier ice: overview, optimisation, validation and potential

Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

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