Annual dynamics of the black carbon size distribution in the near-ground submicron aerosol in western Siberia

Author(s):  
Elena Yausheva ◽  
Valerii Kozlov ◽  
Panchenko Mikhail ◽  
Dmitry Chernov ◽  
Vladimir Shmargunov
2013 ◽  
Vol 13 (7) ◽  
pp. 3603-3618 ◽  
Author(s):  
J.-M. Diesch ◽  
F. Drewnick ◽  
T. Klimach ◽  
S. Borrmann

Abstract. Measurements of the ambient aerosol, various trace gases and meteorological quantities using a mobile laboratory (MoLa) were performed on the banks of the Lower Elbe in an emission control area (ECA) which is passed by numerous private and commercial marine vessels reaching and leaving the port of Hamburg, Germany. From 25–29 April 2011 a total of 178 vessels were probed at a distance of about 0.8–1.2 km with high temporal resolution. 139 ship emission plumes were of sufficient quality to be analyzed further and to determine emission factors (EFs). Concentrations of aerosol number and mass as well as polycyclic aromatic hydrocarbons (PAH) and black carbon were measured in PM1 and size distribution instruments covered the diameter range from 6 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase species analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) in the air and a weather station provided wind, precipitation, solar radiation data and other quantities. Together with ship information for each vessel obtained from Automatic Identification System (AIS) broadcasts a detailed characterization of the individual ship types and of features affecting gas and particulate emissions is provided. Particle number EFs (average 2.6e+16 # kg−1) and PM1 mass EFs (average 2.4 g kg−1) tend to increase with the fuel sulfur content. Observed PM1 composition of the vessel emissions was dominated by organic matter (72%), sulfate (22%) and black carbon (6%) while PAHs only account for 0.2% of the submicron aerosol mass. Measurements of gaseous components showed an increase of SO2 (average EF: 7.7 g kg−1) and NOx (average EF: 53 g kg−1) while O3 decreased when a ship plume reached the sampling site. The particle number size distributions of the vessels are generally characterized by a bimodal size distribution, with the nucleation mode in the 10–20 nm diameter range and a combustion aerosol mode centered at about 35 nm while particles \\textgreater 1 μm were not found. "High particle number emitters" are characterized by a dominant nucleation mode. By contrast, increased particle concentrations around 150 nm primarily occurred for "high black carbon emitters". Classifying the vessels according to their gross tonnage shows a decrease of the number, black carbon and PAH EFs while EFs of SO2, NO, NO2, NOx, AMS species (particulate organics, sulfate) and PM1 mass concentration increase with increasing gross tonnages.


2012 ◽  
Vol 12 (8) ◽  
pp. 22269-22307
Author(s):  
J.-M. Diesch ◽  
F. Drewnick ◽  
T. Klimach ◽  
S. Borrmann

Abstract. Measurements of the ambient aerosol, various trace gases and meteorological parameters using a mobile laboratory (MoLa) were performed on the banks of the Lower Elbe in an emission control area (ECA) which is passed by numerous private and commercial marine vessels reaching and leaving the port of Hamburg, Germany. From 25–30 April 2011 a total of 178 vessels were probed at a distance of about 0.8–2 km with high temporal resolution. 139 ship emission plumes were of sufficient quality to be analyzed further and to determine emission factors (EFs). Concentrations of aerosol number and mass as well as polycyclic aromatic hydrocarbons (PAH) and black carbon were measured in PM1 and size distribution instruments covered the size diameter range from 6 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase species analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) in the air and a weather station provided wind, precipitation, solar radiation and other parameters. Together with ship information for each vessel obtained from Automatic Identification System (AIS) broadcasts a detailed characterization of the individual ship types and of features affecting gas and particulate emissions is provided. Particle number EFs (average 2.6×1016 # kg −1) and PM1 mass EFs (average 2.4 g kg −1) positively correlate with the fuel sulfur content and depend on the engine type and performance. Observed PM1 composition of the vessel emissions was dominated by organic matter (72%), sulfate (22%) and black carbon (6%) while PAHs only account for 0.2% of the submicron aerosol mass. Measurements of gaseous components showed an increase of SO2 (average EF: 7.7 g kg−1) and NOx (average EF: 53 g kg−1) while O3 decreased when a ship plume reached the sampling site. The particle number size distributions of the vessels are generally characterized by a bimodal size distribution, with the nucleation mode in the 10–20 nm diameter range and a combustion aerosol mode centered at about 35 nm while particles >1 μm were not found. "High particle number emitters" are characterized by a dominant nucleation mode. By contrast, a third weaker mode at 150 nm primarily occurred for "high black carbon emitters". Classifying the vessels according to their gross tonnage shows a decrease of the number, black carbon and PAH EFs while EFs of SO2, NO, NO2, NOx, AMS species (particulate organics, sulfate) and PM1 mass concentration increase with increasing gross tonnages.


2016 ◽  
Vol 16 (14) ◽  
pp. 9435-9455 ◽  
Author(s):  
Matthew J. Alvarado ◽  
Chantelle R. Lonsdale ◽  
Helen L. Macintyre ◽  
Huisheng Bian ◽  
Mian Chin ◽  
...  

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.


2014 ◽  
Vol 14 (18) ◽  
pp. 10061-10084 ◽  
Author(s):  
D. Liu ◽  
J. D. Allan ◽  
D. E. Young ◽  
H. Coe ◽  
D. Beddows ◽  
...  

Abstract. Black carbon aerosols (BC) at a London urban site were characterised in both winter- and summertime 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorisation (PMF) factors of organic aerosol mass spectra measured by a high-resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However, the size distribution of Dc (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different Dc distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC–AMS–PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), and easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm and 169 ± 29 nm, respectively. The corresponding bulk relative coating thickness of BC (coated particle size/BC core – Dp/Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0.16 and 1.65 ± 0.19. For W, SE and E air masses, the number fraction of BCsf ranged from 6 ± 2% to 11 ± 5% to 18 ± 10%, respectively, but importantly the larger BC core sizes lead to an increased fraction of BCsf in terms of mass than number (for W, SE and E air masses, the BCsf mass fractions ranged from 16 ± 6%, 24 ± 10% and 39 ± 14%, respectively). An increased fraction of non-BC particles (particles that did not contain a BC core) was also observed when SF sources were more significant. The BC mass attribution by the SP2 method agreed well with the BC–AMS–PMF multiple linear regression method (BC–AMS–PMF : SP2 ratio = 1.05, r2 = 0.80) over the entire experimental period. Good agreement was found between BCsf attributed with the Aethalometer model and the SP2. However, the assumed absorption Ångström exponent (αwb) had to be changed according to the different air mass sectors to yield the best comparison with the SP2. This could be due to influences of fuel type or burn phase.


2006 ◽  
Author(s):  
Svetlana A. Terpugova ◽  
Mikhail V. Panchenko ◽  
Valerii S. Kozlov

2016 ◽  
Vol 9 (1) ◽  
pp. 103-114 ◽  
Author(s):  
G. I. Gkatzelis ◽  
D. K. Papanastasiou ◽  
K. Florou ◽  
C. Kaltsonoudis ◽  
E. Louvaris ◽  
...  

Abstract. An experimental methodology was developed to measure the nonvolatile particle number concentration using a thermodenuder (TD). The TD was coupled with a high-resolution time-of-flight aerosol mass spectrometer, measuring the chemical composition and mass size distribution of the submicrometer aerosol and a scanning mobility particle sizer (SMPS) that provided the number size distribution of the aerosol in the range from 10 to 500 nm. The method was evaluated with a set of smog chamber experiments and achieved almost complete evaporation (> 98 %) of secondary organic as well as freshly nucleated particles, using a TD temperature of 400 °C and a centerline residence time of 15 s. This experimental approach was applied in a winter field campaign in Athens and provided a direct measurement of number concentration and size distribution for particles emitted from major pollution sources. During periods in which the contribution of biomass burning sources was dominant, more than 80 % of particle number concentration remained after passing through the thermodenuder, suggesting that nearly all biomass burning particles had a nonvolatile core. These remaining particles consisted mostly of black carbon (60 % mass contribution) and organic aerosol (OA; 40 %). Organics that had not evaporated through the TD were mostly biomass burning OA (BBOA) and oxygenated OA (OOA) as determined from AMS source apportionment analysis. For periods during which traffic contribution was dominant 50–60 % of the particles had a nonvolatile core while the rest evaporated at 400 °C. The remaining particle mass consisted mostly of black carbon with an 80 % contribution, while OA was responsible for another 15–20 %. Organics were mostly hydrocarbon-like OA (HOA) and OOA. These results suggest that even at 400 °C some fraction of the OA does not evaporate from particles emitted from common combustion processes, such as biomass burning and car engines, indicating that a fraction of this type of OA is of extremely low volatility.


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