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Title: Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

Abstract

The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that themore » biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.« less

Authors:
; ; ; ORCiD logo; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1236649
Grant/Contract Number:  
SC000602
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 16 Journal Issue: 2; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English

Citation Formats

Xu, L., Williams, L. R., Young, D. E., Allan, J. D., Coe, H., Massoli, P., Fortner, E., Chhabra, P., Herndon, S., Brooks, W. A., Jayne, J. T., Worsnop, D. R., Aiken, A. C., Liu, S., Gorkowski, K., Dubey, M. K., Fleming, Z. L., Visser, S., Prévôt, A. S. H., and Ng, N. L. Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area. Germany: N. p., 2016. Web. doi:10.5194/acp-16-1139-2016.
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Xu, L., Williams, L. R., Young, D. E., Allan, J. D., Coe, H., Massoli, P., Fortner, E., Chhabra, P., Herndon, S., Brooks, W. A., Jayne, J. T., Worsnop, D. R., Aiken, A. C., Liu, S., Gorkowski, K., Dubey, M. K., Fleming, Z. L., Visser, S., Prévôt, A. S. H., & Ng, N. L. Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area. Germany. https://doi.org/10.5194/acp-16-1139-2016
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Xu, L., Williams, L. R., Young, D. E., Allan, J. D., Coe, H., Massoli, P., Fortner, E., Chhabra, P., Herndon, S., Brooks, W. A., Jayne, J. T., Worsnop, D. R., Aiken, A. C., Liu, S., Gorkowski, K., Dubey, M. K., Fleming, Z. L., Visser, S., Prévôt, A. S. H., and Ng, N. L. Tue . "Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area". Germany. https://doi.org/10.5194/acp-16-1139-2016.
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@article{osti_1236649,
title = {Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area},
author = {Xu, L. and Williams, L. R. and Young, D. E. and Allan, J. D. and Coe, H. and Massoli, P. and Fortner, E. and Chhabra, P. and Herndon, S. and Brooks, W. A. and Jayne, J. T. and Worsnop, D. R. and Aiken, A. C. and Liu, S. and Gorkowski, K. and Dubey, M. K. and Fleming, Z. L. and Visser, S. and Prévôt, A. S. H. and Ng, N. L.},
abstractNote = {The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS) at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and hydrocarbon-like OA, these three factors have similar volatility, which is inferred from the change in mass concentration after heating at 120 °C. Finally, we discuss the relationship between the mass fraction remaining (MFR) of OA after heating in the TD and atomic O : C of OA and find that particles with a wide range of O : C could have similar MFR after heating. This analysis emphasizes the importance of understanding the distribution of volatility and O : C in bulk OA.},
doi = {10.5194/acp-16-1139-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 2,
volume = 16,
place = {Germany},
year = {Tue Feb 02 00:00:00 EST 2016},
month = {Tue Feb 02 00:00:00 EST 2016}
}
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Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 1: measurement and simulation of organic aerosol evolution
journal, January 2009

  • Grieshop, A. P.; Logue, J. M.; Donahue, N. M.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 4
  • DOI: 10.5194/acp-9-1263-2009

Influence of aerosol chemical composition on N 2 O 5 uptake: airborne regional measurements in northwestern Europe
journal, January 2015

  • Morgan, W. T.; Ouyang, B.; Allan, J. D.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 2
  • DOI: 10.5194/acp-15-973-2015

Emissions and photochemistry of oxygenated VOCs in urban plumes in the Northeastern United States
journal, January 2011

  • Sommariva, R.; de Gouw, J. A.; Trainer, M.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 14
  • DOI: 10.5194/acp-11-7081-2011

Review: Untangling the influence of air-mass history in interpreting observed atmospheric composition
journal, February 2012

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