Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area
The composition of PM<sub>1</sub> (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 a...
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2016-02-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://www.atmos-chem-phys.net/16/1139/2016/acp-16-1139-2016.pdf |
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| author | L. Xu L. R. Williams D. E. Young D. E. Young J. D. Allan J. D. Allan H. Coe P. Massoli E. Fortner P. Chhabra P. Chhabra S. Herndon W. A. Brooks J. T. Jayne D. R. Worsnop A. C. Aiken S. Liu S. Liu K. Gorkowski K. Gorkowski M. K. Dubey Z. L. Fleming Z. L. Fleming S. Visser A. S. H. Prévôt N. L. Ng N. L. Ng |
| author_facet | L. Xu L. R. Williams D. E. Young D. E. Young J. D. Allan J. D. Allan H. Coe P. Massoli E. Fortner P. Chhabra P. Chhabra S. Herndon W. A. Brooks J. T. Jayne D. R. Worsnop A. C. Aiken S. Liu S. Liu K. Gorkowski K. Gorkowski M. K. Dubey Z. L. Fleming Z. L. Fleming S. Visser A. S. H. Prévôt N. L. Ng N. L. Ng |
| author_sort | L. Xu |
| collection | DOAJ |
| description | The composition of PM<sub>1</sub> (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
PM<sub>1</sub>. 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.<br><br>
A suite of instruments was deployed downstream of a thermal denuder (TD) to
investigate the volatility of PM<sub>1</sub> 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. |
| first_indexed | 2024-12-23T21:13:53Z |
| format | Article |
| id | doaj.art-7d3c03fe004844aa8f930c6b57da2ef0 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-12-23T21:13:53Z |
| publishDate | 2016-02-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-7d3c03fe004844aa8f930c6b57da2ef02022-12-21T17:30:59ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-02-01161139116010.5194/acp-16-1139-2016Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London areaL. Xu0L. R. Williams1D. E. Young2D. E. Young3J. D. Allan4J. D. Allan5H. Coe6P. Massoli7E. Fortner8P. Chhabra9P. Chhabra10S. Herndon11W. A. Brooks12J. T. Jayne13D. R. Worsnop14A. C. Aiken15S. Liu16S. Liu17K. Gorkowski18K. Gorkowski19M. K. Dubey20Z. L. Fleming21Z. L. Fleming22S. Visser23A. S. H. Prévôt24N. L. Ng25N. L. Ng26School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USAAerodyne Research Inc., Billerica, MA, USASchool of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UKnow at: Department of Environmental Toxicology, University of California, Davis, CA, USASchool of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UKNational Centre for Atmospheric Science, University of Manchester, Manchester, UKSchool of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UKAerodyne Research Inc., Billerica, MA, USAAerodyne Research Inc., Billerica, MA, USAAerodyne Research Inc., Billerica, MA, USAnow at: PerkinElmer Inc., Hopkinton, MA, USAAerodyne Research Inc., Billerica, MA, USAAerodyne Research Inc., Billerica, MA, USAAerodyne Research Inc., Billerica, MA, USAAerodyne Research Inc., Billerica, MA, USAEarth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, USAEarth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, USAnow at: Cooperative Institute for Research in the Environmental Sciences, University of Colorado, Boulder, CO, USAEarth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, USAnow at: Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USAEarth and Environmental Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, USADepartment of Chemistry, University of Leicester, Leicester, UKNational Centre for Atmospheric Science, University of Leicester, Leicester, UKLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, SwitzerlandLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, SwitzerlandSchool of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USASchool of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USAThe composition of PM<sub>1</sub> (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 PM<sub>1</sub>. 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.<br><br> A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM<sub>1</sub> 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.https://www.atmos-chem-phys.net/16/1139/2016/acp-16-1139-2016.pdf |
| spellingShingle | L. Xu L. R. Williams D. E. Young D. E. Young J. D. Allan J. D. Allan H. Coe P. Massoli E. Fortner P. Chhabra P. Chhabra S. Herndon W. A. Brooks J. T. Jayne D. R. Worsnop A. C. Aiken S. Liu S. Liu K. Gorkowski K. Gorkowski M. K. Dubey Z. L. Fleming Z. L. Fleming S. Visser A. S. H. Prévôt N. L. Ng N. L. Ng Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area Atmospheric Chemistry and Physics |
| title | Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area |
| title_full | Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area |
| title_fullStr | Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area |
| title_full_unstemmed | Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area |
| title_short | Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area |
| title_sort | wintertime aerosol chemical composition volatility and spatial variability in the greater london area |
| url | https://www.atmos-chem-phys.net/16/1139/2016/acp-16-1139-2016.pdf |
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