scholarly journals Investigation of gaseous and particulate emissions from various marine vessel types measured on the banks of the Elbe in Northern Germany

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.


2019 ◽  
Vol 19 (1) ◽  
pp. 39-55 ◽  
Author(s):  
Roy M. Harrison ◽  
David C. S. Beddows ◽  
Mohammed S. Alam ◽  
Ajit Singh ◽  
James Brean ◽  
...  

Abstract. Particle number size distributions have been measured simultaneously by scanning mobility particle sizers (SMPSs) at five sites in central London for a 1 month campaign in January–February 2017. These measurements were accompanied by condensation particle counters (CPCs) to measure total particle number count at four of the sites and Aethalometers measuring black carbon (BC) at five sites. The spatial distribution and inter-relationships of the particle size distribution and SMPS total number counts with CPC total number counts and black carbon measurements have been analysed in detail as well as variations in the size distributions. One site (Marylebone Road) was in a street canyon with heavy traffic, one site (Westminster University) was on a rooftop adjacent to the Marylebone Road sampler, and a further sampler was located at Regent's University within a major park to the north of Marylebone Road. A fourth sampler was located nearby at 160 m above ground level on the BT tower and a fifth sampler was located 4 km to the west of the main sampling region at North Kensington. Consistent with earlier studies it was found that the mode in the size distribution had shifted to smaller sizes at the Regent's University (park) site, the mean particle shrinkage rate being 0.04 nm s−1 with slightly lower values at low wind speeds and some larger values at higher wind speeds. There was evidence of complete evaporation of the semi-volatile nucleation mode under certain conditions at the elevated BT Tower site. While the SMPS total count and black carbon showed typical traffic-dominated diurnal profiles, the CPC count data typically peaked during night-time as did CPC∕SMPS and CPC∕BC ratios. This is thought to be due to the presence of high concentrations of small particles (2.5–15 nm diameter) probably arising from condensational growth from traffic emissions during the cooler night-time conditions. Such behaviour was most marked at the Regent's University and Westminster University sites and less so at Marylebone Road, while at the elevated BT Tower site the ratio of particle number (CPC) to black carbon peaked during the morning rush hour and not at night-time, unlike the other sites. An elevation in nucleation mode particles associated with winds from the west and WSW sector was concluded to result from emissions from London Heathrow Airport, despite a distance of 22 km from the central London sites.


2018 ◽  
Author(s):  
Roy M. Harrison ◽  
David C. S. Beddows ◽  
Mohammed S. Alam ◽  
Ajit Singh ◽  
James Brean ◽  
...  

Abstract. Particle number size distributions have been measured simultaneously by Scanning Mobility Particle Sizers (SMPS) at five sites in Central London for a one month campaign in January–February 2017. These measurements were accompanied by condensation particle counters (CPC) to measure total particle number count at four of the sites and aethalometers measuring Black Carbon (BC) at five sites. The spatial distribution and inter-relationships of the particle size distribution and SMPS total number counts with CPC total number counts and Black Carbon measurements have been analysed in detail as well as variations in the size distributions. One site (Marylebone Road) was in a heavily-trafficked street canyon, one site (Westminster University) was on a rooftop adjacent to the Marylebone Road sampler, a further sampler was located at Regent's University within a major park to the north of Marylebone Road. A fourth sampler was located nearby at 160 m above ground level on the BT tower and a fifth sampler was located 4 km to the west of the main sampling region at North Kensington. Consistent with earlier studies it was found that the mode in the size distribution had shifted to smaller sizes at the Regent's University (park) site, the mean particle shrinkage rate being 0.04 nm s−1 with slightly lower values at low wind speeds and some larger values at higher wind speeds. There was evidence of complete evaporation of the semi-volatile nucleation mode under certain conditions at the elevated BT Tower site. Whereas SMPS total count and Black Carbon showed typical traffic-dominated diurnal profiles, the CPC count data typically peaked during nighttime as did CPC/SMPS and CPC/BC ratios. This is thought to be due to the presence of high concentrations of small particles (2.5–15 nm diameter) probably arising from condensational growth from traffic emissions during the cooler nighttime conditions. Such behaviour was most marked at the Regent's University and Westminster University sites and less so at Marylebone Road, while at the elevated BT Tower site the ratio of particle number (CPC) to Black Carbon peaked during the morning rush hour and not at nighttime, unlike the other sites. An elevation in nucleation mode particles associated with winds from the West and WSW sector was concluded to result from emissions from London Heathrow Airport, despite a distance of 22 km from the Central London sites.


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.


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.


2013 ◽  
Vol 395-396 ◽  
pp. 399-402 ◽  
Author(s):  
Li Bao Mei ◽  
Xiao Qin Xiao ◽  
Yong Li ◽  
Yan Lin Sun

The nucleation mode of emulsion polymerization of styrene under different emulsifier (SDS) concentrations is studied in this paper. Some factors such as conversion, particle number (Np), fraction of coverage, polydispersion index (PDI) and particle size distribution (PSD) of the reactions were investigated. The results show that when [SD is less than its CMC, homogeneous nucleation dominates. But when [SD is more than its CMC, micelle nucleation plays the major role.


2010 ◽  
Vol 10 (10) ◽  
pp. 4643-4660 ◽  
Author(s):  
W. Birmili ◽  
K. Heinke ◽  
M. Pitz ◽  
J. Matschullat ◽  
A. Wiedensohler ◽  
...  

Abstract. Aerosol particle number size distributions (size range 0.003–10 μm) in the urban atmosphere of Augsburg (Germany) were examined with respect to the governing anthropogenic sources and meteorological factors. The two-year average particle number concentration between November 2004 and November 2006 was 12 200 cm−3, i.e. similar to previous observations in other European cities. A seasonal analysis yielded twice the total particle number concentrations in winter as compared to summer as consequence of more frequent inversion situations and enhanced particulate emissions. The diurnal variations of particle number were shaped by a remarkable maximum in the morning during the peak traffic hours. After a mid-day decrease along with the onset of vertical mixing, an evening concentration maximum could frequently be observed, suggesting a re-stratification of the urban atmosphere. Overall, the mixed layer height turned out to be the most influential meteorological parameter on the particle size distribution. Its influence was even greater than that of the geographical origin of the prevailing synoptic-scale air mass. Size distributions below 0.8 μm were also measured downstream of a thermodenuder (temperature: 300 °C), allowing to retrieve the volume concentration of non-volatile compounds. The balance of particle number upstream and downstream of the thermodenuder suggests that practically all particles >12 nm contain a non-volatile core while additional nucleation of particles smaller than 6 nm could be observed after the thermodenuder as an interfering artifact of the method. The good correlation between the non-volatile volume concentration and an independent measurement of the aerosol absorption coefficient (R2=0.9) suggests a close correspondence of the refractory and light-absorbing particle fractions. Using the "summation method", an average diameter ratio of particles before and after volatilisation could be determined as a function of particle size. The results indicated that particles >60 nm contain a significantly higher fraction of non-volatile compounds, most likely black carbon, than particles <60 nm. The results are relevant for future health-related studies in that they explore the size distribution and time-dependent behaviour of the refractory component of the urban aerosol over an extended time period.


Author(s):  
James Brooks ◽  
James D. Allan ◽  
Paul I. Williams ◽  
Dantong Liu ◽  
Cathryn Fox ◽  
...  

<p><strong>Abstract.</strong> The vertical distribution in the physical and chemical properties of submicron aerosol has been characterised across northern India for the first time using airborne in-situ measurements. This study focusses primarily on the Indo-Gangetic Plain, a low-lying area in the north of India which commonly experiences high aerosol mass concentrations prior to the monsoon season. Data presented are from the UK Facility for Airborne Atmospheric Measurements BAe-146 research aircraft that performed flights in the region during the 2016 pre-monsoon (11<sup>th</sup> and 12<sup>th</sup> June) and monsoon (30<sup>th</sup> June to 11<sup>th</sup> July) seasons.</p> <p> Inside the Indo-Gangetic Plain boundary layer, organic matter dominated the submicron aerosol mass (43&amp;thinsp;%) followed by sulphate (29&amp;thinsp;%), ammonium (14&amp;thinsp;%), nitrate (7&amp;thinsp;%) and black carbon (7&amp;thinsp;%). However, outside the Indo-Gangetic Plain, sulphate was the dominant species contributing 44&amp;thinsp;% to the total submicron aerosol mass in the boundary layer, followed by organic matter (30&amp;thinsp;%), ammonium (14&amp;thinsp;%), nitrate (6&amp;thinsp;%) and black carbon (6&amp;thinsp;%). Chlorine mass concentrations were negligible throughout the campaign. Black carbon mass concentrations were higher inside the Indo-Gangetic Plain (2&amp;thinsp;µg/m<sup>3</sup> std) compared to outside (1&amp;thinsp;µg/m<sup>3</sup> std). Nitrate appeared to be controlled by thermodynamic processes, with increased mass concentration in conditions of lower temperature and higher relative humidity. Increased mass and number concentrations were observed inside the Indo-Gangetic Plain and the aerosol was more absorbing in this region, whereas outside the Indo-Gangetic Plain the aerosol was larger in size and more scattering in nature, suggesting greater dust presence especially in northwest India. The aerosol composition remained largely similar as the monsoon season progressed, but the total aerosol mass concentrations decreased by ~&amp;thinsp;50&amp;thinsp;% as the rainfall arrived; the pre-monsoon average total mass concentration was 30&amp;thinsp;µg/m<sup>3</sup> std compared to a monsoon average total mass concentration of 10&amp;ndash;20&amp;thinsp;µg/m<sup>3</sup> std. However, this mass concentration decrease was less noteworthy (~&amp;thinsp;20&amp;ndash;30&amp;thinsp;%) over the Indo-Gangetic Plain, likely due to the strength of emission sources in this region. Decreases occurred in coarse mode aerosol, with the fine mode fraction increasing with monsoon arrival. In the aerosol vertical profile, inside the Indo-Gangetic Plain during the pre-monsoon, organic aerosol and absorbing aerosol species dominated in the lower atmosphere (<&amp;thinsp;1.5&amp;thinsp;km) with sulphate, dust and other scattering aerosol species enhanced in an elevated aerosol layer above 1.5&amp;thinsp;km with maximum aerosol height ~&amp;thinsp;6&amp;thinsp;km. As the monsoon progressed into this region, the elevated aerosol layer diminished, the aerosol maximum height reduced to ~&amp;thinsp;2&amp;thinsp;km and the total mass concentrations decreased by ~&amp;thinsp;50&amp;thinsp;%. The dust and sulphate-dominated aerosol layer aloft was removed upon monsoon arrival, highlighted by an increase in fine mode fraction throughout the profile.</p>


2014 ◽  
Vol 14 (10) ◽  
pp. 15149-15189 ◽  
Author(s):  
J. F. Peng ◽  
M. Hu ◽  
Z. B. Wang ◽  
X. F. Huang ◽  
P. Kumar ◽  
...  

Abstract. Understanding the particle number size distributions in diversified atmospheric environments is important in order to design mitigation strategies related to submicron particles and their effect on regional air quality, haze and human health. In this study, we conducted 15 different field measurement campaigns, each one-month long, between 2007 and 2011 at 13 individual sites in China. These were 5 urban sites, 4 regional sites, 3 coastal/background sites and one ship cruise measurement along eastern coastline of China. Size resolved particles were measured in the 15–600 nm size range. The median particle number concentrations (PNC) were found to vary in the range of 1.1–2.2 × 104 cm−3 at urban sites, 0.8–1.5 × 104 cm−3 at regional sites, 0.4–0.6 × 104 cm−3 at coastal/background sites, and 0.5 × 104 cm−3 during cruise measurements. Peak diameters at each of these sites varied greatly from 24 nm to 115 nm. Particles in the 15–25 nm (nucleation mode), 25–100 nm (Aitken mode) and 100–600 nm (accumulation mode) range showed different characteristics at each of the studied sites, indicating the features of primary emissions and secondary formation in these diversified atmospheric environments. Diurnal variations show a build-up of accumulation mode particles belt at regional sites, suggesting the contribution of regional secondary aerosol pollution. Frequencies of new particle formation (NPF) events were much higher at urban and regional sites than at coastal sites and cruise measurement. The average growth rates (GRs) of nucleation mode particles were 8.0–10.9 nm h−1 at urban sites, 7.4–13.6 nm h−1 at regional sites and 2.8–7.5 nm h−1 at both coastal and cruise measurement sites. The high gaseous precursors and strong oxidation at urban and regional sites not only favored the formation of particles, but also accelerated the growth rate of the nucleation mode particles. No significant difference in condensation sink (CS) during NPF days were observed among different site types, suggesting that the NPF events in background area were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal and cruise measurement sites had little impact on potential production of CCN. This study provides a large dataset of aerosol size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particles formation and corresponding CCN activity of submicron aerosols in Chinese environments.


Sign in / Sign up

Export Citation Format

Share Document