Radiocarbon Analysis of Carbonaceous Aerosols: Recent Developments

Szidat, Sönke

doi:10.2533/chimia.2009.157

Cited by 26 publications

(28 citation statements)

References 24 publications

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“…The following laboratories participated in this intercomparison (here compiled in alphabetical order and anonymized in the following): Bern/PSI/ETH (Szidat 2009); INFN-LABEC (Calzolai et al 2011); Irvine (Santos et al 2007); LLNL (Bench et al 2007); Lund (Genberg et al 2011); NIES (Uchida et al 2010); Stockholm (Zencak et al 2007), Utrecht; and Woods Hole . Five filter samples were distributed among the participants: 2 ambient samples; 1 corresponding blank; and 2 reference materials on filter media.…”

Section: Methodsmentioning

confidence: 99%

“…In recent years, individual 14 C measurements of OC, EC, and some other subfractions or specific compounds have gathered importance (Szidat et al 2004;Zencak et al 2007;Uchida et al 2010;Zhang et al 2012;Bernardoni et al 2013). Separate 14 C measurement of OC and EC is advantageous compared to analysis of TC alone, since the different sources of OC and EC result in diverse 14 C levels (Szidat 2009). Whereas OC may be emitted by non-combustion processes or formed in the atmosphere from gaseous precursors with a typical dominance of non-fossil sources, EC solely originates from combustion processes of fossil fuels or wood and is therefore frequently dominated by 14 C-free material.…”

Section: Introductionmentioning

confidence: 99%

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Intercomparison of 14C Analysis of Carbonaceous Aerosols: Exercise 2009

et al. 2013

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ABSTRACT. Radiocarbon analysis of the carbonaceous aerosol allows an apportionment of fossil and non-fossil sources of airborne particulate matter (PM). A chemical separation of total carbon (TC) into its subfractions organic carbon (OC) and elemental carbon (EC) refines this powerful technique, as OC and EC originate from different sources and undergo different processes in the atmosphere. Although 14 C analysis of TC, EC, and OC has recently gained increasing attention, interlaboratory quality assurance measures have largely been missing, especially for the isolation of EC and OC. In this work, we present results from an intercomparison of 9 laboratories for 14 C analysis of carbonaceous aerosol samples on quartz fiber filters. Two ambient PM samples and 1 reference material (RM 8785) were provided with representative filter blanks. All laboratories performed 14 C determinations of TC and a subset of isolated EC and OC for isotopic measurement. In general, 14 C measurements of TC and OC agreed acceptably well between the laboratories, i.e. for TC within 0.015-0.025 F 14 C for the ambient filters and within 0.041 F 14 C for RM 8785. Due to inhomogeneous filter loading, RM 8785 demonstrated only limited applicability as a reference material for 14 C analysis of carbonaceous aerosols. 14 C analysis of EC revealed a large deviation between the laboratories of 28-79% as a consequence of different separation techniques. This result indicates a need for further discussion on optimal methods of EC isolation for 14 C analysis and a second stage of this intercomparison.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Intercomparison of 14C Analysis of Carbonaceous Aerosols: Exercise 2009

et al. 2013

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“…[107] Accelerator MS is commonly used in environmental studies to distinguish between fossil and non-fossil carbon based on quantitative measurements of 14 C radiocarbon. [111] Because of a radioactive decay on an ,5700-year time scale, fossil carbon is devoid of 14 C. Therefore, the isotopic ratio of emissions from fossil fuel combustion or modern carbon sources that can be relevant to both natural (e.g. biogenic SOAs) and man-made (e.g.…”

Section: Field and Test Facilities Studies Anthropogenic Aerosolsmentioning

confidence: 99%

Mass spectrometric approaches for chemical characterisation of atmospheric aerosols: critical review of the most recent advances

Laskin¹,

Laskin²,

Nizkorodov³

2012

Environ. Chem.

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Environmental context. Atmospheric aerosols have profound effects on the environment through several physicochemical processes, such as absorption and scattering of sunlight, heterogeneous gas-particle reactions and adverse effects on the respiratory and cardiovascular systems. Understanding aerosol atmospheric chemistry and its environmental impact requires comprehensive characterisation of the physical and chemical properties of particles. Results from mass spectrometry provide important new insights into the origin of atmospheric aerosols, the evolution of their physicochemical properties, their reactivity and their effect on the environment.Abstract. This manuscript presents an overview of the most recent instrument developments for the field and laboratory applications of mass spectrometry (MS) to investigate the chemistry and physics of atmospheric aerosols. A range of MS instruments, employing different sample introduction methods, ionisation and mass detection techniques are used both for 'online' and 'offline' characterisation of aerosols. Online MS techniques enable detection of individual particles with simultaneous measurement of particle size distributions and aerodynamic characteristics and are ideally suited for field studies that require high temporal resolution. Offline MS techniques provide a means for detailed molecular-level analysis of aerosol samples, which is essential to gain fundamental knowledge regarding aerosol chemistry, mechanisms of particle formation and atmospheric aging. Combined, complementary MS techniques provide comprehensive information on the chemical composition, size, morphology and phase of aerosols -data of key importance for evaluating hygroscopic and optical properties of particles, their health effects, understanding their origins and atmospheric evolution. Over the last few years, developments and applications of MS techniques in aerosol research have expanded remarkably as evident by skyrocketing publication statistics. The goal of this review is to present the most recent developments in the field of aerosol mass spectrometry for the time period of late 2010 to early 2012, which have not been conveyed in previous reviews.

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“…The radioactive isotope of carbon ( 14 C) is used to distinguish fossil (coal, gasoline, diesel) and contemporary (wood, agricultural waste, pollen, vegetation) contributions to ambient OA (Szidat, 2009). Schichtel et al (2008) present the isotopic composition for 12 rural sites collocated with the IM-PROVE network.…”

Section: Oa Isotopic Compositionmentioning

confidence: 99%

The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol

et al. 2011

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Abstract.Semi-volatile and reactive primary organic aerosols are modeled on a global scale using the GISS GCM II' "unified" climate model. We employ the volatility basis set framework to simulate emissions, chemical reactions and phase partitioning of primary and secondary organic aerosol (POA and SOA). The model also incorporates the emissions and reactions of intermediate volatility organic compounds (IVOCs) as a source of organic aerosol (OA), one that has been missing in most prior work. Model predictions are evaluated against a broad set of observational constraints including mass concentrations, degree of oxygenation, volatility and isotopic composition. A traditional model that treats POA as non-volatile and non-reactive is also compared to the same set of observations to highlight the progress made in this effort. The revised model predicts a global dominance of SOA and brings the POA/SOA split into better agreement with ambient measurements. This change is due to traditionally defined POA evaporating and the evaporated vapors oxidizing to form non-traditional SOA. IVOCs (traditionally not included in chemical transport models) oxidize to form condensable products that account for a third of total OA, suggesting that global models have been missing a large source of OA. Predictions of the revised model for the SOA fraction at 17 different locations compared much better to observations than predictions from the traditional model. Modelpredicted volatility is compared with thermodenuder data collected at three different different field campaigns: FAME-2008, MILAGRO-2006 and SOAR-2005. The revised model predicts the OA volatility much more closely than the traditional model. When compared against monthly averaged OA Correspondence to: P. J. Adams (peter.adams@cmu.edu) mass concentrations measured by the IMPROVE network, predictions of the revised model lie within a factor of two in summer and mostly within a factor of five during winter. A sensitivity analysis indicates that the winter comparison can be improved either by increasing POA emissions or lowering the volatility of those emissions. Model predictions of the isotopic composition of OA are compared against those computed via a radiocarbon isotope analysis of field samples. The contemporary fraction, on average, is slightly under-predicted (20 %) during the summer months but is a factor of two lower during the winter months. We hypothesize that the large wintertime under-prediction of surface OA mass concentrations and the contemporary fraction is due to an under-representation of biofuel (particularly, residential wood burning) emissions in the emissions inventory. Overall, the model evaluation highlights the importance of treating POA as semi-volatile and reactive in order to predict accurately the sources, composition and properties of ambient OA.

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Radiocarbon Analysis of Carbonaceous Aerosols: Recent Developments

Cited by 26 publications

References 24 publications

Intercomparison of 14C Analysis of Carbonaceous Aerosols: Exercise 2009

Intercomparison of 14C Analysis of Carbonaceous Aerosols: Exercise 2009

Mass spectrometric approaches for chemical characterisation of atmospheric aerosols: critical review of the most recent advances

The influence of semi-volatile and reactive primary emissions on the abundance and properties of global organic aerosol

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