scholarly journals 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)

2020 ◽  
Vol 13 (10) ◽  
pp. 5725-5738
Author(s):  
Marcel Weloe ◽  
Thorsten Hoffmann
Keyword(s):  
Real Time ◽  
Mass Spectrometer ◽  
Atmospheric Aerosol ◽  
Condensation Reaction ◽  
High Mass ◽  
Organic Peroxides ◽  
Particle Phase ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Health Related

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.

scholarly journals 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)

2019 ◽  
Author(s):  
Marcel Weloe ◽  
Thorsten Hoffmann
Keyword(s):  
Real Time ◽  
Mass Spectrometer ◽  
Atmospheric Aerosol ◽  
Condensation Reaction ◽  
High Mass ◽  
Organic Peroxides ◽  
Particle Phase ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Health Related

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/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 detected 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 quantitative determination of peroxide with a time resolution of one to two minutes. The method was tested with freshly formed and aged biogenic VOC/ozone SOA as well as in a short proof-of-principle study with ambient aerosol.

scholarly journals A missing source of aerosols in Antarctica – beyond long-range transport, phytoplankton, and photochemistry

2017 ◽  
Vol 17 (1) ◽  
pp. 1-20 ◽  
Author(s):  
Michael R. Giordano ◽  
Lars E. Kalnajs ◽  
Anita Avery ◽  
J. Douglas Goetz ◽  
Sean M. Davis ◽  
...  
Keyword(s):  
Chemical Composition ◽  
High Resolution ◽  
Real Time ◽  
Mass Spectrometer ◽  
Formation Mechanisms ◽  
Second Phase ◽  
Austral Spring ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
The Antarctic

Abstract. Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS – soot particle aerosol mass spectrometer – or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition. The second phase appears as a transitional phase during the extended polar sunrise. The third phase is marked by an increased importance of biogenically derived sulfate to the total aerosol population (photolysis of dimethyl sulfate and methanesulfonic acid (DMS and MSA)). The increased importance of MSA is identified both through the direct, real-time measurement of aerosol MSA and through the use of positive matrix factorization on the sulfur-containing ions in the high-resolution mass-spectral data. Given the importance of sub-250 nm particles, the aforementioned second phase suggests that early austral spring is the season where new particle formation mechanisms are likely to have the largest contribution to the aerosol population in Antarctica.

scholarly journals Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

2011 ◽  
Vol 11 (10) ◽  
pp. 27383-27420 ◽  
Author(s):  
C. Mohr ◽  
P. F. DeCarlo ◽  
M. F. Heringa ◽  
R. Chirico ◽  
J. G. Slowik ◽  
...  
Keyword(s):  
Mass Spectrometer ◽  
Biomass Burning ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Data Matrix ◽  
High Mass ◽  
Organic Mass ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Data Points

Abstract. PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O/C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O/C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the organic mass fragments at m/z 55, 57, and 44 is developed here and allows for a first-order-estimation of COA in urban air. This study emphasizes the importance of cooking activities for ambient air quality and confirms the importance of chemical composition measurements with a high mass and time resolution.

scholarly journals Real-Time Measurements of Engine-Out Trace Elements: Application of a Novel Soot Particle Aerosol Mass Spectrometer for Emissions Characterization

2012 ◽  
Vol 134 (7) ◽  
Author(s):  
E. S. Cross ◽  
A. Sappok ◽  
E. C. Fortner ◽  
J. F. Hunter ◽  
J. T. Jayne ◽  
...  
Keyword(s):  
Trace Elements ◽  
Trace Element ◽  
Real Time ◽  
Mass Spectrometer ◽  
Soot Particle ◽  
Fast Time ◽  
Engine Fuel ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass ◽  
Measurement Validation

Lubricant-derived trace element emissions are the largest contributors to the accumulation of incombustible ash in diesel particulate filters (DPF), eventually leading to filter plugging and an increase in engine fuel consumption. Particulate trace element emissions also pose adverse health effects and are the focus of increasingly stringent air quality regulations. To date, the rates and physical and chemical properties of lubricant-derived additive emissions are not well characterized, largely due to the difficulties associated with conducting the measurements. This work investigated the potential for conducting real-time measurements of lubricant-derived particle emissions. The experiment used the Soot Particle Aerosol Mass Spectrometer (SP-AMS) developed by Aerodyne Research to measure the size, mass and composition of submicron particles in the exhaust. Results confirm the ability of the SP-AMS to measure engine-out emissions of calcium, zinc, magnesium, phosphorous, and sulfur. Further, emissions of previously difficult to detect elements, such as boron, and low-level engine wear metals, such as lead, were also measured. This paper provides an overview of the results obtained with the SP-AMS, and demonstrates the utility of applying real-time techniques to engine-out and tailpipe-out trace element emissions. Application of the SP-AMS for engine exhaust characterization followed a two-part approach: (1) measurement validation, and (2) measurement of engine-out exhaust. Measurement validation utilized a diesel burner with precise control of lubricant consumption. Results showed a good correlation between CJ-4 oil consumption and measured levels of lubricant-derived trace elements in the particle phase. Following measurement validation, the SP-AMS measured engine-out emissions from a medium-duty diesel engine, operated over a standard speed/load matrix. This work demonstrates the utility of state-of-the-art online techniques (such as the SP-AMS) to measure engine-out emissions, including trace species derived from lubricant additives. Results help optimize the combined engine-lubricant-aftertreatment system and provide a real-time characterization of emissions. As regulations become more stringent and emission controls more complex, advanced measurement techniques with high sensitivity and fast time response will become an increasingly important part of engine characterization studies.

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