Online molecular characterisation of organic aerosols in an atmospheric chamber using extractive electrospray ionisation mass spectrometry

Gallimore, Peter J.; Giorio, Chiara; Mahon, Brendan M.; Kalberer, Markus

doi:10.5194/acp-17-14485-2017

Cited by 17 publications

(33 citation statements)

References 63 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The shortcomings of low time resolution with filter measurements can be overcome using this kind of instruments to elucidate more information about the chemical processes involved. Such instrumentations include, for instance, TAG-AMS (thermal desorption aerosol gas chromatograph-AMS) [359][360][361], EESI-TOF-MS (extractive electrospray ionization-time of flight-MS) [362][363][364][365][366], or different inlets associated to PTR-MS (proton-transfer reaction-MS) or CIMS (chemical ionization MS) such as FIGAERO (filter inlet for gases and aerosols) [367], CHARON (chemical analysis of aerosol online) or thermo-desorption (TD) systems [37,[368][369][370][371], which have been successfully applied to apportion SOC in details. However, these instruments are still costly and only appropriate for short term studies.…”

Section: Conclusion and Future Implicationsmentioning

confidence: 99%

Comparison of Measurement-Based Methodologies to Apportion Secondary Organic Carbon (SOC) in PM2.5: A Review of Recent Studies

et al. 2018

View full text Add to dashboard Cite

Secondary organic aerosol (SOA) is known to account for a major fraction of airborne particulate matter, with significant impacts on air quality and climate at the global scale. Despite the substantial amount of research studies achieved during these last decades, the source apportionment of the SOA fraction remains difficult due to the complexity of the physicochemical processes involved. The selection and use of appropriate approaches are a major challenge for the atmospheric science community. Several methodologies are nowadays available to perform quantitative and/or predictive assessments of the SOA amount and composition. This review summarizes the current knowledge on the most commonly used approaches to evaluate secondary organic carbon (SOC) contents: elemental carbon (EC) tracer method, chemical mass balance (CMB), SOA tracer method, radiocarbon (14C) measurement and positive matrix factorization (PMF). The principles, limitations, challenges and good practices of each of these methodologies are discussed in the present article. Based on a comprehensive—although not exhaustive—review of research papers published during the last decade (2006–2016), SOC estimates obtained using these methodologies are also summarized for different regions across the world. Conclusions of some studies which are directly comparing the performances of different methodologies are then specifically discussed. An overall picture of SOC contributions and concentrations obtained worldwide for urban sites under similar conditions (i.e., geographical and seasonal ones) is also proposed here. Finally, further needs to improve SOC apportionment methodologies are also identified and discussed.

show abstract

Section: Conclusion and Future Implicationsmentioning

confidence: 99%

Comparison of Measurement-Based Methodologies to Apportion Secondary Organic Carbon (SOC) in PM2.5: A Review of Recent Studies

et al. 2018

View full text Add to dashboard Cite

show abstract

“…Traditional techniques for rapid online measurements of OA without sample handling rely on the combination of mass spectrometry with thermal desorption. Most single-particle instruments, e.g., ATOFMS (Gard et al, 1997), SPLAT (Zelenyuk and Imre, 2005), and PALMS (Murphy et al, 2006), utilize simultaneous laser desorption/ionization, which is not quantitative due to matrix effects and can also result in fragmentation of organic molecules. In contrast, the Aerodyne aerosol mass spectrometer (AMS) utilizes a high vaporization temperature (600 • C) and electron ionization (EI, 70 eV) to remain quantitative but at the cost of extensive thermal decomposition and ionization-induced fragmentation (Canagaratna et al, 2007).…”

Section: Introductionmentioning

confidence: 99%

An extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles

et al. 2019

Self Cite

View full text Add to dashboard Cite

Abstract. Real-time, online measurements of atmospheric organic aerosol (OA) composition are an essential tool for determining the emissions sources and physicochemical processes governing aerosol effects on climate and health. However, the reliance of current techniques on thermal desorption, hard ionization, and/or separated collection/analysis stages introduces significant uncertainties into OA composition measurements, hindering progress towards these goals. To address this gap, we present a novel, field-deployable extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which provides online, near-molecular (i.e., molecular formula) OA measurements at atmospherically relevant concentrations without analyte fragmentation or decomposition. Aerosol particles are continuously sampled into the EESI-TOF, where they intersect a spray of charged droplets generated by a conventional electrospray probe. Soluble components are extracted and then ionized as the droplets are evaporated. The EESI-TOF achieves a linear response to mass, with detection limits on the order of 1 to 10 ng m−3 in 5 s for typical atmospherically relevant compounds. In contrast to conventional electrospray systems, the EESI-TOF response is not significantly affected by a changing OA matrix for the systems investigated. A slight decrease in sensitivity in response to increasing absolute humidity is observed for some ions. Although the relative sensitivities to a variety of commercially available organic standards vary by more than a factor of 30, the bulk sensitivity to secondary organic aerosol generated from individual precursor gases varies by only a factor of 15. Further, the ratio of compound-by-compound sensitivities between the EESI-TOF and an iodide adduct FIGAERO-I-CIMS varies by only ±50 %, suggesting that EESI-TOF mass spectra indeed reflect the actual distribution of detectable compounds in the particle phase. Successful deployments of the EESI-TOF for laboratory environmental chamber measurements, ground-based ambient sampling, and proof-of-concept measurements aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.

show abstract

“…2 and 3) (Davies and Feld, 1958;Jayanthi and Koshore, 1997). The main application of the TPP-TPPO method is the determination of hydroperoxides from the autoxidation of oils and fats (Gotoh et al, 2011;Nakamura and Maeda, 1991;Wang et al, 2016). Compared to iodometric peroxide determination, the TPP-TPPO method is insensitive to moisture, and the reaction with oxygen is much slower.…”

Section: Introductionmentioning

confidence: 99%

Application of time-of-flight aerosol mass spectrometry for the real-time measurement of particle-phase organic peroxides: an online redox derivatization–aerosol mass spectrometer (ORD-AMS)

Weloe

Hoffmann

2020

Atmos. Meas. Tech.

View full text Add to dashboard Cite

Abstract. Aerosol mass spectrometers (AMS) are frequently applied in atmospheric aerosol research in connection with climate, environmental or health-related projects. This is also true for the measurement of the organic fraction of particulate matter, still the least understood group of components contributing to atmospheric aerosols. While quantification of the organic and/or inorganic aerosol fractions is feasible, more detailed information about individual organic compounds or compound classes can usually not be provided by AMS measurements. In this study, we present a new method to detect organic peroxides in the particle phase in real-time using an AMS. Peroxides (ROOR') are of high interest to the atmospheric aerosol community due to their potentially high mass contribution to SOA, their important role in new particle formation and their function as “reactive oxygen species” in aerosol–health-related topics. To do so, supersaturated gaseous triphenylphosphine (TPP) was continuously mixed with the aerosol flow of interest in a condensation/reaction volume in front of the AMS inlet. The formed triphenylphosphine oxide (TPPO) from the peroxide–TPP reaction was then detected by an aerosol mass spectrometer (AMS), enabling the semiquantitative determination of peroxide with a time resolution of 2 min. The method was tested with freshly formed and aged biogenic VOC and ozone SOA as well as in a short proof-of-principle study with ambient aerosol.

show abstract

Online molecular characterisation of organic aerosols in an atmospheric chamber using extractive electrospray ionisation mass spectrometry

Cited by 17 publications

References 63 publications

Comparison of Measurement-Based Methodologies to Apportion Secondary Organic Carbon (SOC) in PM2.5: A Review of Recent Studies

Comparison of Measurement-Based Methodologies to Apportion Secondary Organic Carbon (SOC) in PM2.5: A Review of Recent Studies

An extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) for online measurement of atmospheric aerosol particles

Application of time-of-flight aerosol mass spectrometry for the real-time measurement of particle-phase organic peroxides: an online redox derivatization–aerosol mass spectrometer (ORD-AMS)

Contact Info

Product

Resources

About