Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013
During winter 2013, extremely high concentrations (i.e., 4–20 times higher than the World Health Organization guideline) of PM<sub>2.5</sub> (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including...
| Main Authors: | , , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Copernicus Publications
2015-02-01
|
| Series: | Atmospheric Chemistry and Physics |
| Online Access: | http://www.atmos-chem-phys.net/15/1299/2015/acp-15-1299-2015.pdf |
| _version_ | 1811281677972930560 |
|---|---|
| author | Y.-L. Zhang R.-J. Huang I. El Haddad K.-F. Ho J.-J. Cao Y. Han P. Zotter C. Bozzetti K. R. Daellenbach F. Canonaco J. G. Slowik G. Salazar M. Schwikowski J. Schnelle-Kreis G. Abbaszade R. Zimmermann U. Baltensperger A. S. H. Prévôt S. Szidat |
| author_facet | Y.-L. Zhang R.-J. Huang I. El Haddad K.-F. Ho J.-J. Cao Y. Han P. Zotter C. Bozzetti K. R. Daellenbach F. Canonaco J. G. Slowik G. Salazar M. Schwikowski J. Schnelle-Kreis G. Abbaszade R. Zimmermann U. Baltensperger A. S. H. Prévôt S. Szidat |
| author_sort | Y.-L. Zhang |
| collection | DOAJ |
| description | During winter 2013, extremely high concentrations (i.e., 4–20 times higher
than the World Health Organization guideline) of PM<sub>2.5</sub> (particulate matter
with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were
found in four major cities in China including Xi'an,
Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set
from elemental carbon (EC), organic carbon (OC), <sup>14</sup>C and
biomass-burning marker measurements using Latin hypercube sampling allowed a
quantitative source apportionment of carbonaceous aerosols. Based on
<sup>14</sup>C measurements of EC fractions (six samples each city), we found that
fossil emissions from coal combustion and vehicle exhaust dominated EC with
a mean contribution of 75 ± 8% across all sites. The remaining
25 ± 8% was exclusively attributed to biomass combustion, consistent
with the measurements of biomass-burning markers such as anhydrosugars
(levoglucosan and mannosan) and water-soluble potassium (K<sup>+</sup>). With a
combination of the levoglucosan-to-mannosan and levoglucosan-to-K<sup>+</sup> ratios, the major source of biomass burning in winter in China is
suggested to be combustion of crop residues. The contribution of fossil
sources to OC was highest in Beijing (58 ± 5%) and decreased from
Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou
(35 ± 7%). Generally, a larger fraction of fossil OC was from
secondary origins than primary sources for all sites. Non-fossil sources
accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC),
respectively, which suggests that non-fossil emissions were very important
contributors of urban carbonaceous aerosols in China. The primary
biomass-burning emissions accounted for 40 ± 8, 48 ± 18,
53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing,
Shanghai and Guangzhou, respectively. Other non-fossil sources excluding
primary biomass burning were mainly attributed to formation of secondary
organic carbon (SOC) from non-fossil precursors such as biomass-burning
emissions. For each site, we also compared samples from moderately to
heavily polluted days according to particulate matter mass. Despite a
significant increase of the absolute mass concentrations of primary emissions
from both fossil and non-fossil sources during the heavily polluted events,
their relative contribution to TC was even decreased, whereas the portion of
SOC was consistently increased at all sites. This observation indicates that
SOC was an important fraction in the increment of carbonaceous aerosols
during the haze episode in China. |
| first_indexed | 2024-04-13T01:37:59Z |
| format | Article |
| id | doaj.art-d11d1f1b51f547b8adedb5ef10eb0170 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-04-13T01:37:59Z |
| publishDate | 2015-02-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-d11d1f1b51f547b8adedb5ef10eb01702022-12-22T03:08:17ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242015-02-011531299131210.5194/acp-15-1299-2015Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013Y.-L. Zhang0R.-J. Huang1I. El Haddad2K.-F. Ho3J.-J. Cao4Y. Han5P. Zotter6C. Bozzetti7K. R. Daellenbach8F. Canonaco9J. G. Slowik10G. Salazar11M. Schwikowski12J. Schnelle-Kreis13G. Abbaszade14R. Zimmermann15U. Baltensperger16A. S. H. Prévôt17S. Szidat18Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, 3012 Bern, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandSchool of Public Health and Primary Care, Chinese University of Hong Kong, Hong Kong, ChinaKey Laboratory of Aerosol Chemistry and Physics, Institute of Earth Environment, Chinese Academy of Sciences, 710061 Xi'an, ChinaKey Laboratory of Aerosol Chemistry and Physics, Institute of Earth Environment, Chinese Academy of Sciences, 710061 Xi'an, ChinaPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandDepartment of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, 3012 Bern, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandHelmholtz Zentrum München, German Research Center for Environmental Health (GmbH), Joint Mass Spectrometry Centre, Cooperation Group Comprehensive Molecular Analytics, and Helmholtz Virtual Institute of Complex Molecular Systems in Environmental Health – Aerosol and Health (HICE), 85764 Neuherberg, GermanyHelmholtz Zentrum München, German Research Center for Environmental Health (GmbH), Joint Mass Spectrometry Centre, Cooperation Group Comprehensive Molecular Analytics, and Helmholtz Virtual Institute of Complex Molecular Systems in Environmental Health – Aerosol and Health (HICE), 85764 Neuherberg, GermanyHelmholtz Zentrum München, German Research Center for Environmental Health (GmbH), Joint Mass Spectrometry Centre, Cooperation Group Comprehensive Molecular Analytics, and Helmholtz Virtual Institute of Complex Molecular Systems in Environmental Health – Aerosol and Health (HICE), 85764 Neuherberg, GermanyPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandPaul Scherrer Institute (PSI), Villigen, 5232 Villigen-PSI, SwitzerlandDepartment of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, 3012 Bern, SwitzerlandDuring winter 2013, extremely high concentrations (i.e., 4–20 times higher than the World Health Organization guideline) of PM<sub>2.5</sub> (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), <sup>14</sup>C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on <sup>14</sup>C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K<sup>+</sup>). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K<sup>+</sup> ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass-burning emissions. For each site, we also compared samples from moderately to heavily polluted days according to particulate matter mass. Despite a significant increase of the absolute mass concentrations of primary emissions from both fossil and non-fossil sources during the heavily polluted events, their relative contribution to TC was even decreased, whereas the portion of SOC was consistently increased at all sites. This observation indicates that SOC was an important fraction in the increment of carbonaceous aerosols during the haze episode in China.http://www.atmos-chem-phys.net/15/1299/2015/acp-15-1299-2015.pdf |
| spellingShingle | Y.-L. Zhang R.-J. Huang I. El Haddad K.-F. Ho J.-J. Cao Y. Han P. Zotter C. Bozzetti K. R. Daellenbach F. Canonaco J. G. Slowik G. Salazar M. Schwikowski J. Schnelle-Kreis G. Abbaszade R. Zimmermann U. Baltensperger A. S. H. Prévôt S. Szidat Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013 Atmospheric Chemistry and Physics |
| title | Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013 |
| title_full | Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013 |
| title_fullStr | Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013 |
| title_full_unstemmed | Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013 |
| title_short | Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013 |
| title_sort | fossil vs non fossil sources of fine carbonaceous aerosols in four chinese cities during the extreme winter haze episode of 2013 |
| url | http://www.atmos-chem-phys.net/15/1299/2015/acp-15-1299-2015.pdf |
| work_keys_str_mv | AT ylzhang fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT rjhuang fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT ielhaddad fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT kfho fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT jjcao fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT yhan fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT pzotter fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT cbozzetti fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT krdaellenbach fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT fcanonaco fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT jgslowik fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT gsalazar fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT mschwikowski fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT jschnellekreis fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT gabbaszade fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT rzimmermann fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT ubaltensperger fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT ashprevot fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 AT sszidat fossilvsnonfossilsourcesoffinecarbonaceousaerosolsinfourchinesecitiesduringtheextremewinterhazeepisodeof2013 |