scholarly journals Properties and emission factors of CCN from biomass cookstoves – observations of a strong dependency on potassium content in the fue

2020 ◽  
Author(s):  
Thomas Bjerring Kristensen ◽  
John Falk ◽  
Robert Lindgren ◽  
Christina Andersen ◽  
Vilhelm B. Malmborg ◽  
...  

Abstract. Residential biomass combustion is a significant source of aerosol particles on regional and global scales influencing climate and human health. The main objective of the current study was to investigate the properties of cloud condensation nuclei (CCN) emitted from biomass burning of solid fuels in different cookstoves mostly of relevance to Sub-Saharan East Africa. The traditional 3-stone fire (3S) and a rocket stove (RS) were used for combustion of wood logs of sesbania (ses) and casuarina (cas) with birch (bir) used as a reference. A natural draft (ND) and a forced draft (FD) pellet stove were used for combustion of pelletized sesbania and pelletized Swedish softwood (sw) alone or in mixtures with pelletized coffee husk (ch), rice husk (rh) or water hyacinth (wh). The CCN activity and the effective density were measured for particles with mobility diameters of ∼65, ∼100 and ∼200 nm, respectively, and occasionally for ∼350 nm particles. Particle number size distributions were measured online with a fast particle analyzer. The chemical composition of the fuel ash was measured by application of standard protocols. The average particle number size distributions were by number typically dominated by an ultrafine mode, and in most cases a soot mode was centered around a mobility diameter of ∼150 nm. The CCN activities decreased with increasing particle size for all experiments and ranged in terms of the hygroscopicity parameter, κ, from ∼0.1 to ∼0.8 for the ultrafine mode and from ∼0.0 to ∼0.15 for the soot mode. The CCN activity of the ultrafine mode increased with increasing combustion temperature for a given fuel, and it typically increased with increasing potassium concentration in the investigated fuels. The primary CCN and the estimated particulate matter (PM) emission factors were typically found to increase significantly with increasing potassium concentration in the fuel for a given stove. In order to link CCN emission factors to PM emission factors, knowledge about stove technology, stove operation and the inorganic fuel ash composition is needed. This complicates the use of ambient PM levels alone for estimation of CCN concentrations in regions dominated by biomass combustion aerosol, with the relation turning even more complex when accounting for atmospheric ageing of the aerosol.

2021 ◽  
Vol 21 (10) ◽  
pp. 8023-8044
Author(s):  
Thomas Bjerring Kristensen ◽  
John Falk ◽  
Robert Lindgren ◽  
Christina Andersen ◽  
Vilhelm B. Malmborg ◽  
...  

Abstract. Residential biomass combustion is a significant source of aerosol particles on regional and global scales influencing climate and human health. The main objective of the current study was to investigate the properties of cloud condensation nuclei (CCN) emitted from biomass burning of solid fuels in different cookstoves mostly of relevance to sub-Saharan east Africa. The traditional three-stone fire and a rocket stove were used for combustion of wood logs of Sesbania and Casuarina with birch used as a reference. A natural draft and a forced-draft pellet stove were used for combustion of pelletised Sesbania and pelletised Swedish softwood alone or in mixtures with pelletised coffee husk, rice husk or water hyacinth. The CCN activity and the effective density were measured for particles with mobility diameters of ∽65, ∽100 and ∽200 nm, respectively, and occasionally for 350 nm particles. Particle number size distributions were measured online with a fast particle analyser. The chemical composition of the fuel ash was measured by application of standard protocols. The average particle number size distributions were by number typically dominated by an ultrafine mode, and in most cases a soot mode was centred around a mobility diameter of ∽150 nm. The CCN activities decreased with increasing particle size for all experiments and ranged in terms of the hygroscopicity parameter, κ, from ∽0.1 to ∽0.8 for the ultrafine mode and from ∽0.001 to ∽0.15 for the soot mode. The CCN activity (κ) of the ultrafine mode increased (i) with increasing combustion temperature for a given fuel, and (ii) it typically increased with increasing potassium concentration in the investigated fuels. The primary CCN and the estimated particulate matter (PM) emission factors were typically found to increase significantly with increasing potassium concentration in the fuel for a given stove. In order to link CCN emission factors to PM emission factors, knowledge about stove technology, stove operation and the inorganic fuel ash composition is needed. This complicates the use of ambient PM levels alone for estimation of CCN concentrations in regions dominated by biomass combustion aerosol, with the relation turning even more complex when accounting for atmospheric ageing of the aerosol.


2019 ◽  
Author(s):  
Samuel A. Atwood ◽  
Sonia M. Kreidenweis ◽  
Paul J. DeMott ◽  
Markus D. Petters ◽  
Gavin C. Cornwell ◽  
...  

Abstract. Aerosol particle and cloud condensation nuclei (CCN) measurements from a littoral location on the northern coast of California at Bodega Bay Marine Laboratory (BML) are presented for approximately six weeks of observations during the CalWater-2015 field campaign. A combination of aerosol microphysical and meteorological parameters was used to classify variability in the properties of the BML surface aerosol using a K-means cluster model. Eight aerosol population types were identified that were associated with a range of impacts from both marine and terrestrial sources. Average measured total particle number concentrations, size distributions, hygroscopicities, and activated fraction spectra between 0.08 % and 1.1 % supersaturation are given for each of the identified aerosol population types, along with meteorological observations and transport pathways during time periods associated with each type. Five terrestrially influenced aerosol population types represented different degrees of aging of the continental outflow from the coast and interior of California and their appearance at the BML site was often linked to changes in wind direction and transport pathway. In particular, distinct aerosol populations, associated with diurnal variations in source region induced by land/sea-breeze shifts, were classified by the clustering technique. A terrestrial type representing fresh emissions, and/or a recent new particle formation event, occurred in approximately 10 % of the observations. Over the entire study period, three marine influenced population types were identified that typically occurred when the regular diurnal land/sea-breeze cycle collapsed and BML was continuously ventilated by air masses from marine regions for multiple days. These marine types differed from each other primarily in the degree of cloud processing evident in the size distributions, and in the presence of an additional large-particle mode for the type associated with the highest wind speeds. One of the marine types was associated with a multi-day period during which an atmospheric river made landfall at BML. The generally higher total particle number concentrations but lower activated fractions of four of the terrestrial types yielded similar CCN number concentrations to two of the marine types for supersaturations below about 0.4 %. Despite quite different activated fraction spectra, the two remaining marine and terrestrial types had CCN spectral number concentrations very similar to each other, due in part to higher number concentrations associated with the terrestrial type.


2008 ◽  
Vol 8 (4) ◽  
pp. 15537-15594 ◽  
Author(s):  
W. Birmili ◽  
B. Alaviippola ◽  
D. Hinneburg ◽  
O. Knoth ◽  
T. Tuch ◽  
...  

Abstract. Atmospheric particle number size distributions of airborne particles (diameter range 10–500 nm) were measured over ten weeks at three sites in the vicinity of the A100 urban motorway in Berlin, Germany. The A100 carries about 180 000 vehicles on a weekday, and roadside particle size distributions showed a number maximum between 20 and 60 nm clearly related to the motorway emissions. The average total number concentration at roadside was 28 000 cm−3 with a total range between 1200 and 168 000 cm−3. At distances of 80 and 400 m from the motorway the concentrations decreased to mean levels of 11 000 and 9 000 cm−3, respectively. An obstacle-resolving dispersion model was applied to simulate the 3-D flow field and traffic tracer transport in the urban environment around the motorway. By inverse modelling, vehicle emission factors were derived, representative of a relative share of 6% lorry-like vehicles, and a driving speed of about 80 km h−1. Three different calculation approaches were compared, which differ in the choice of the experimental winds driving the flow simulation. The average emission factor per vehicle was 2.1(±0.2) · 1014 km−1 for particle number and 0.077(±0.01) · 1014 cm3 km−1 for particle volume. Regression analysis suggested that lorry-like vehicles emit 116 (± 21) times more particulate number than passenger car-like vehicles, and that lorry-like vehicles account for about 91% of particulate number emissions on weekdays. Our work highlights the increasing applicability of 3-D flow models in urban microscale environments and their usefulness in determining traffic emission factors.


2009 ◽  
Vol 9 (1) ◽  
pp. 3763-3809 ◽  
Author(s):  
S. Klose ◽  
W. Birmili ◽  
J. Voigtländer ◽  
T. Tuch ◽  
B. Wehner ◽  
...  

Abstract. A biennial dataset of ambient particle number size distributions (diameter range 4–800 nm) collected in urban air in Leipzig, Germany, was analysed with respect to the influence of traffic emissions. Size distributions were sampled continuously in 2005 and 2006 inside a street canyon trafficked by ca. 10 000 motor vehicles per day, and at a background reference site distant at 1.5 km. Auto-correlation analysis showed that the impact of fresh traffic emissions could be seen most intensely below particle sizes of 60 nm. The traffic-induced concentration increment at roadside was estimated by subtracting the urban background values from the street canyon measurement. To describe the variable dispersion conditions inside the street canyon, micro-meteorological dilution factors were calculated using the Operational Street Pollution Model (OSPM), driven by above-roof wind speed and wind direction observations. The roadside increment concentrations, dilution factor, and real-time traffic counts were used to calculate vehicle emission factors (aerosol source rates) that are representative of the prevailing driving conditions, i.e. stop-and-go traffic including episodes of fluent traffic flow at speeds up to 40 km h−1. The size spectrum of traffic-derived particles was essentially bimodal – with mode diameters around 12 and 100 nm, while statistical analysis suggested that the emitted number concentration varied with time of day, wind direction, particle size and fleet properties. Significantly, the particle number emissions depended on ambient temperature, ranging between 4.8 (±1.8) and 7.8 (±2.9).1014 p. veh−1 km−1 in summer and winter, respectively. A separation of vehicle types according to vehicle length suggested that lorry-like vehicles emit about 80 times more particle number than passenger car-like vehicles. Using nitrogen oxide (NOx) measurements, specific total particle number emissions of 338 p. (pg NOx)−1 were inferred. The calculated traffic emission factors, considering particle number and size, are anticipated to provide useful input for future air quality and particle exposure modelling in densely populated urban areas.


2018 ◽  
Vol 18 (4) ◽  
pp. 2853-2881 ◽  
Author(s):  
Julia Schmale ◽  
Silvia Henning ◽  
Stefano Decesari ◽  
Bas Henzing ◽  
Helmi Keskinen ◽  
...  

Abstract. Aerosol–cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set – ready to be used for model validation – of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles > 20 nm) across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2–0.3). We performed closure studies based on κ–Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of κ. The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating “migrating-CCNCs” to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.


2013 ◽  
Vol 13 (13) ◽  
pp. 6227-6237 ◽  
Author(s):  
Z. Z. Deng ◽  
C. S. Zhao ◽  
N. Ma ◽  
L. Ran ◽  
G. Q. Zhou ◽  
...  

Abstract. Precise quantification of the cloud condensation nuclei (CCN) number concentration is crucial for understanding aerosol indirect effects and characterizing these effects in models. An evaluation of various methods for CCN parameterization was carried out in this paper based on in situ measurements of aerosol activation properties within HaChi (Haze in China) project. Comparisons were made by closure studies between methods using CCN spectra, bulk activation ratios, cut-off diameters and size-resolved activation ratios. The estimation of CCN number concentrations by the method using aerosol size-resolved activation ratios, either averaged over a day or with diurnal variation, was found to be most satisfying and straightforward. This could be well expected since size-resolved activation ratios include information regarding the effects of size-resolved chemical compositions and mixing states on aerosol activation properties. The method using the averages of critical diameters, which were inferred from measured CCN number concentrations and particle number size distributions, also provided a good prediction of the CCN number concentration. Based on comparisons of all these methods in this paper, it was recommended that the CCN number concentration be predicted using particle number size distributions with inferred critical diameters or size-resolved activation ratios.


2009 ◽  
Vol 9 (1) ◽  
pp. 1669-1702 ◽  
Author(s):  
S. M. King ◽  
T. Rosenoern ◽  
J. E. Shilling ◽  
Q. Chen ◽  
S. T. Martin

Abstract. The effect of organic particle mass loading from 1 to ≥100 μg m−3 on the cloud condensation nuclei (CCN) properties of mixed organic-sulfate particles was investigated in the Harvard Environmental Chamber. Mixed particles were produced by the condensation of organic molecules onto ammonium sulfate particles during the dark ozonolysis of α-pinene. A continuous-flow mode of the chamber provided stable conditions over long time periods, allowing for signal integration and hence increased measurement precision at low organic mass loadings representative of atmospheric conditions. CCN activity was measured at eight mass loadings for 80- and 100-nm particles grown on 50-nm sulfate seeds. A two-component (organic/sulfate) Köhler model, which included the particle heterogeneity arising from DMA size selection and from organic volume fraction for the selected 80- and 100-nm particles, was used to predict CCN activity. For organic mass loadings of 2.9 μg m−3 and greater, the observed activation curves were well predicted using a single set of physicochemical parameters for the organic component. For mass loadings of 1.74 μg m−3 and less, the observed CCN activity increased beyond predicted values using the same parameters, implying changed physicochemical properties of the organic component. Of possible changes in surface tension, effective molecular weight, and effective density, a sensitivity analysis implicated a decrease of up to 10% in surface tension at low mass loadings as the plausible dominant mechanism for the observed increase in CCN activity.


2010 ◽  
Vol 10 (4) ◽  
pp. 8553-8594 ◽  
Author(s):  
F. Wang ◽  
P. Roldin ◽  
A. Massling ◽  
A. Kristensson ◽  
E. Swietlicki ◽  
...  

Abstract. Aerosol particles in the submicrometer size range (PM1) have serious impacts on human health and climate. This work aims at studying the processes relevant for physical particle properties in and downwind Copenhagen and evaluating the capability of a detailed aerosol dynamics and chemistry model (ADCHEM) to describe the submicrometer aerosol dynamics in a complex urbanized region, subjected to a variety of important anthropogenic sources. The study area is the Oresund Region with Copenhagen (about 1.8 million people) as the major city, including the strait separating Denmark and Sweden with intense ship traffic. Modeled aerosol particle number size distributions and NOx concentrations are evaluated against ground-based measurements from two stations in the Copenhagen area in Denmark and one station in southern Sweden. The measured and modeled increments in NOx concentrations from rural background to the urban area showed satisfactory agreement, indicating that the estimated NOx emissions and modeled atmospheric dispersion are reasonable. For three out of five case studies, the modeled particle number concentrations and size distributions are in satisfactory agreement with the measurements at all stations along the trajectories. For the remaining cases the model significantly underestimates the particle number concentration over Copenhagen, but reaches acceptable agreement with the measurements at the downwind background station in Sweden. The major causes for this were identified as being the lack of spatial resolution in the meteorological data in describing boundary layer mixing heights and the uncertainty in the exact air mass trajectory path over Copenhagen. In addition, particle emission factors may also have been too low. It was shown that aerosol dynamics play a minor role from upwind to urban background, but are important 1–2 h downwind the city. Real-world size-resolved traffic number emission factors which take into account the initial ageing in the street canyon can be used to model traffic emissions in urban plume studies.


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