scholarly journals Source apportionment of the carbonaceous aerosol in Norway – quantitative estimates based on <sup>14</sup>C, thermal-optical and organic tracer analysis

2011 ◽  
Vol 11 (3) ◽  
pp. 7375-7422 ◽  
Author(s):  
K. E. Yttri ◽  
D. Simpson ◽  
K. Stenström ◽  
H. Puxbaum ◽  
T. Svendby

Abstract. In the present study, source apportionment of the ambient summer and winter time particulate carbonaceous matter (PCM) in aerosol particles (PM1 and PM10) has been conducted for the Norwegian urban and rural background environment. Statistical treatment of data from thermal-optical, 14C and organic tracer analysis using Latin Hypercube Sampling has allowed for quantitative estimates of seven different sources contributing to the ambient carbonaceous aerosol. These are: elemental carbon from combustion of biomass (ECbb) and fossil fuel (ECff), organic carbon from combustion of biomass (OCbb), fossil fuel (OCff), primary biological aerosol particles (OCPBAP, which includes plant debris, OCpbc, and fungal spores, OCpbs), and secondary organic aerosol from biogenic precursors (OCBSOA). Our results show that emissions from natural sources were particularly abundant in summer, and with a more pronounced influence at the rural compared to the urban background site. 80% of total carbon (TCp, corrected for the positive artefact) in PM10 and 70% of TCp in PM1 could be attributed to natural sources at the rural background site in summer. Natural sources account for about 50% of TCp in PM10 at the urban background site as well. The natural source contribution was always dominated by OCBSOA, regardless of season, site and size fraction. During winter anthropogenic sources totally dominated the carbonaceous aerosol (83–90%). Combustion of biomass contributed slightly more than fossil-fuel sources in winter, whereas emissions from fossil-fuel sources were more abundant in summer. Mass closure calculations show that PCM likely dominated the mass concentration of the ambient PM regardless of size fraction, season, and site. A larger fraction of PM1 (64–69%) was accounted for by carbonaceous matter compared to PM10 (51–67%), but only by a small margin. In general, there were no pronounced differences in the relative contribution of carbonaceous matter to PM with respect to season or between the two sites.

2011 ◽  
Vol 11 (17) ◽  
pp. 9375-9394 ◽  
Author(s):  
K. E. Yttri ◽  
D. Simpson ◽  
K. Stenström ◽  
H. Puxbaum ◽  
T. Svendby

Abstract. In the present study, source apportionment of the ambient summer and winter time particulate carbonaceous matter (PCM) in aerosol particles (PM1 and PM10) has been conducted for the Norwegian urban and rural background environment. Statistical treatment of data from thermal-optical, 14C and organic tracer analysis using Latin Hypercube Sampling has allowed for quantitative estimates of seven different sources contributing to the ambient carbonaceous aerosol. These are: elemental carbon from combustion of biomass (ECbb) and fossil fuel (ECff), primary and secondary organic carbon arising from combustion of biomass (OCbb) and fossil fuel (OCff), primary biological aerosol particles (OCPBAP, which includes plant debris, OCpbc, and fungal spores, OCpbs), and secondary organic aerosol from biogenic precursors (OCBSOA). Our results show that emissions from natural sources were particularly abundant in summer, and with a more pronounced influence at the rural compared to the urban background site. 80% of total carbon (TCp, corrected for the positive artefact) in PM10 and ca. 70% of TCpin PM1 could be attributed to natural sources at the rural background site in summer. Natural sources account for about 50% of TCp in PM10 at the urban background site as well. The natural source contribution was always dominated by OCBSOA, regardless of season, site and size fraction. During winter anthropogenic sources totally dominated the carbonaceous aerosol (80–90%). Combustion of biomass contributed slightly more than fossil-fuel sources in winter, whereas emissions from fossil-fuel sources were more abundant in summer. Mass closure calculations show that PCM made significant contributions to the mass concentration of the ambient PM regardless of size fraction, season, and site. A larger fraction of PM1 (ca. 40–60%) was accounted for by carbonaceous matter compared to PM10 (ca. 40–50%), but only by a small margin. In general, there were no pronounced differences in the relative contribution of carbonaceous matter to PM with respect to season or between the two sites.


2016 ◽  
Vol 180 ◽  
pp. 262-273 ◽  
Author(s):  
Stefania Squizzato ◽  
Mauro Masiol ◽  
Chiara Agostini ◽  
Flavia Visin ◽  
Gianni Formenton ◽  
...  

2020 ◽  
Vol 11 (12) ◽  
pp. 2202-2214
Author(s):  
Valentina Gluščić ◽  
Mirjana Čačković ◽  
Gordana Pehnec ◽  
Ivan Bešlić

2021 ◽  
Vol 245 ◽  
pp. 117993
Author(s):  
Katarzyna Juda-Rezler ◽  
Elwira Zajusz-Zubek ◽  
Magdalena Reizer ◽  
Katarzyna Maciejewska ◽  
Eliza Kurek ◽  
...  

2019 ◽  
Vol 19 (7) ◽  
pp. 4211-4233 ◽  
Author(s):  
Karl Espen Yttri ◽  
David Simpson ◽  
Robert Bergström ◽  
Gyula Kiss ◽  
Sönke Szidat ◽  
...  

Abstract. Carbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources. OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %–50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring. Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites. Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general.


2018 ◽  
Author(s):  
Karl Espen Yttri ◽  
David Simpson ◽  
Robert Bergström ◽  
Gyula Kiss ◽  
Sönke Szidat ◽  
...  

Abstract. Source apportionment (SA) of carbonaceous aerosol was performed as part of the EMEP Intensive Measurement Periods (EIMPs), conducted in fall 2008 and winter/spring 2009. Levels of elemental carbon (EC), particulate organic carbon (OCp), particulate total carbon (TCp), levoglucosan and 14C in PM10, observed at nine European rural background sites, were used as input for the SA, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting when ambient concentrations were combined with appropriate emission ratios. Five predefined sources/subcategories of carbonaceous aerosol were apportioned: Elemental and organic carbon from combustion of biomass (ECbb and OCbb) and from fossil fuel (ECff and OCff) sources, as well as remaining non-fossil organic carbon (OCrnf), typically dominated by natural sources. The carbonaceous aerosol concentration decreased from South to North, as did the concentration of the apportioned carbonaceous aerosol. OCrnf was more abundant in fall compared to winter/spring, reflecting the vegetative season, and made a larger contribution to TCp than anthropogenic sources (here: ECbb, OCbb, ECff and OCff) at four of the sites, whereas anthropogenic sources dominated at all but one sites in winter/spring. Levels of OCbb and ECbb were typically higher in winter/spring than in fall, due to larger residential wood burning emissions in the heating season, whereas there was no consistent seasonal pattern for fossil fuel emissions. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the Central European sites in fall, whereas fossil fuel sources dominated at the southernmost and the two northernmost sites. In winter/spring, biomass burning was the major anthropogenic source at all but two sites. Addressing EC in particular, fossil fuel sources dominated at all sites in fall, whereas there was as shift towards biomass burning in winter/spring for the southernmost sites. Influence of residential wood burning emissions was substantial already in the first week of sampling in fall, constituting 30–50 % of TCp at most sites, showing that this source can be dominating even at a time of the year when the ambient temperature in Europe is still rather high. Model calculations were made, attempting to reproduce LHS-derived OCbb and ECbb, using two different residential wood burning emission inventories. Both simulations strongly under-predicted the LHS-derived values at most sites outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential combustion (and including intermediate volatility compounds, IVOC) improved model results at most sites compared to the base-case emissions (based mainly on officially reported national emissions), but at the three southernmost sites the modelled OCbb and ECbb concentrations were still much lower than the LHS source apportioned results. The current study shows that natural sources is a major contributor to the carbonaceous aerosol in Europe even in fall and in winter/spring, and that residential wood burning emissions can be equally large or larger than that of fossil fuel sources, depending on season and region. Our results suggest that residential wood burning emissions are still poorly constrained for large parts of Europe. The need to improve emission inventories is obvious, with harmonization of emission factors between countries likely being the most important step to improve model calculations, not only for biomass burning emissions, but for European PM2.5 concentrations in general.


2019 ◽  
Author(s):  
Jaime Benavides ◽  
Michelle Snyder ◽  
Marc Guevara ◽  
Albert Soret ◽  
Carlos Pérez García-Pando ◽  
...  

Abstract. The NO2 annual air quality limit value is systematically exceeded in many European cities. In this context, understanding human exposure, improving policy and planning, and providing forecasts requires the development of accurate air quality models at urban (street–level) scale. We describe CALIOPE-Urban, a system coupling CALIOPE – an operational mesoscale air quality forecast system based on HERMES (emissions), WRF (meteorology) and CMAQ (chemistry) models – with the urban roadway dispersion model R-LINE. Our developments have focused on Barcelona city (Spain), but the methodology may be replicated for other cities in the future. WRF drives pollutant dispersion and CMAQ provides background concentrations to R-LINE. Key features of our system include the adaptation of R-LINE to street canyons, the use of a new methodology that considers upwind grid cells in CMAQ to avoid double counting traffic emissions, a new method to estimate local surface roughness within street canyons, and a vertical mixing parametrization that considers urban geometry and atmospheric stability to calculate surface level background concentrations. We show that the latter is critical to correct the nighttime overestimations in our system. Both CALIOPE and CALIOPE-Urban are evaluated using two sets of observations. The temporal variability is evaluated against measurements from five traffic sites and one urban background site for April–May 2013. While both systems show a fairly good agreement at the urban background site, CALIOPE-Urban shows a better agreement in traffic sites. The spatial variability is evaluated using 182 passive dosimeters that were distributed across Barcelona during two weeks for February–March 2017. In this case, also the coupled system shows a more realistic distribution than the mesoscale system, which systematically underpredicts NO2 close to traffic emission sources. Overall CALIOPE-Urban improves mesoscale model results, demonstrating that the combination of both scales provides a more realistic representation of NO2 spatio-temporal variability in Barcelona.


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