scholarly journals The aerosol radiative effects of uncontrolled combustion of domestic waste

2016 ◽  
Author(s):  
John K. Kodros ◽  
Rachel Cucinotta ◽  
David A. Ridley ◽  
Christine Wiedinmyer ◽  
Jeffrey R. Pierce

Abstract. Open, uncontrolled combustion of domestic waste is a potentially significant source of aerosol; however, this aerosol source is not generally included in many global emissions inventories. To provide a first estimate of the aerosol radiative impacts from domestic-waste combustion, we incorporate the Wiedinmyer et al. (2014) emissions inventory into GEOS-Chem-TOMAS, a global chemical-transport model with online aerosol microphysics. We find domestic-waste combustion increases global-mean black carbon and organic aerosol concentrations by 8 % and 6 %, respectively, and by greater than 40 % in some regions. Due to uncertainties regarding aerosol optical properties, we estimate the globally averaged aerosol direct radiative effect to range from −5 mW m−2 to −20 mW m−2; however, this range increases to −40 mW m−2 to +4 mW m−2 when we consider uncertainties in emission mass and size distribution. In some regions with significant waste combustion, such as India and China, the aerosol direct radiative effect may exceed −0.4 W m−2. Similarly, we estimate a cloud-albedo aerosol indirect effect of −13 mW m−2, with a range of −4 mW m−2 to −49 mW m−2 due to emission uncertainties. In the regions with significant waste combustion, the cloud-albedo aerosol indirect effect may exceed −0.4 W m−2.

2016 ◽  
Vol 16 (11) ◽  
pp. 6771-6784 ◽  
Author(s):  
John K. Kodros ◽  
Rachel Cucinotta ◽  
David A. Ridley ◽  
Christine Wiedinmyer ◽  
Jeffrey R. Pierce

Abstract. Open, uncontrolled combustion of domestic waste is a potentially significant source of aerosol; however, this aerosol source is not generally included in many global emissions inventories. To provide a first estimate of the aerosol radiative impacts from domestic-waste combustion, we incorporate the Wiedinmyer et al. (2014) emissions inventory into GEOS-Chem-TOMAS, a global chemical-transport model with online aerosol microphysics. We find domestic-waste combustion increases global-mean black carbon and organic aerosol concentrations by 8 and 6 %, respectively, and by greater than 40 % in some regions. Due to uncertainties regarding aerosol optical properties, we estimate the globally averaged aerosol direct radiative effect to range from −5 to −20 mW m−2; however, this range increases from −40 to +4 mW m−2 when we consider uncertainties in emission mass and size distribution. In some regions with significant waste combustion, such as India and China, the aerosol direct radiative effect may exceed −0.4 W m−2. Similarly, we estimate a cloud-albedo aerosol indirect effect of −13 mW m−2, with a range of −4 to −49 mW m−2 due to emission uncertainties. In the regions with significant waste combustion, the cloud-albedo aerosol indirect effect may exceed −0.4 W m−2.


2012 ◽  
Vol 12 (12) ◽  
pp. 33127-33163 ◽  
Author(s):  
J. R. Pierce ◽  
M. J. Evans ◽  
C. E. Scott ◽  
S. D. D'Andrea ◽  
D. K. Farmer ◽  
...  

Abstract. H2SO4 vapor is important for the nucleation of atmospheric aerosols and the growth of ultrafine particles to cloud condensation nuclei (CCN) sizes. Recent studies have found that reactions of stabilized Criegee intermediates (CIs, formed from the ozonolysis of alkenes) with SO2 may be an important source of H2SO4 that has been missing from atmospheric aerosol models. In this paper, we use the chemical transport model, GEOS-Chem, with the online aerosol microphysics module, TOMAS, to estimate the possible impact of CIs on present-day H2SO4, CCN, and the cloud-albedo aerosol indirect effect (AIE). We extend the standard GEOS-Chem chemistry with CI-forming reactions (ozonolysis of isoprene, methyl vinyl ketone, methacrolein, propene, and monoterpenes) from the Master Chemical Mechanism. Using a fast rate constant for CI+SO2, we find that the addition of this chemistry increases the global production of H2SO4 by 4%. H2SO4 concentrations increase by over 100% in forested tropical boundary layers and by over 10–25% in forested NH boundary layers (up to 100% in July) due to CI + SO2 chemistry, but the change is generally negligible elsewhere. The predicted changed in CCN were strongly dampened to the CI + SO2 changes in H2SO4 in these regions: less than 15% in tropical forests and less than 2% in most mid-latitude locations. The global-mean CCN change was less than 1% both in the boundary layer and the free troposphere. The associated cloud-albedo AIE change was less than 0.03 W m−2. The model global sensitivity of CCN and the AIE to CI + SO2 chemistry is significantly (approximately one order-of-magnitude) smaller than the sensitivity of CCN and AIE to other uncertain model inputs, such as nucleation mechanisms, primary emissions, SOA and deposition. Similarly, comparisons to size-distribution measurements show that uncertainties in other model parameters dominate model biases in the model-predicted size distributions. We conclude that improvement in the modeled CI + SO2 chemistry would not likely to lead to significant improvements in present-day CCN and AIE predictions.


2008 ◽  
Vol 8 (5) ◽  
pp. 16981-17036 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
I. De Smedt ◽  
M. Van Roozendael ◽  
G. R. van der Werf ◽  
...  

Abstract. A new one-decade dataset of formaldehyde (HCHO) columns retrieved from GOME and SCIAMACHY is compared with HCHO columns simulated by an updated version of the IMAGES global chemical transport model. This model version includes an optimized chemical scheme with respect to HCHO production, where the short-term and final HCHO yields from pyrogenically emitted non-methane volatile organic compounds (NMVOCs) are estimated from the Master Chemical Mechanism (MCM) and an explicit speciation profile of pyrogenic emissions. The model is driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, whereas biogenic emissions are provided either by the Global Emissions Inventory Activity (GEIA), or by a newly developed inventory based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) algorithms driven by meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). The comparisons focus on tropical ecosystems, North America and China, which experience strong biogenic and biomass burning NMVOC emissions reflected in the enhanced measured HCHO columns. These comparisons aim at testing the ability of the model to reproduce the observed features of the HCHO distribution on the global scale and at providing a first assessment of the performance of the current emission inventories. The high correlation coefficients (r>0.8) between the observed and simulated columns over most regions indicate a very good consistency between the model, the implemented inventories and the HCHO dataset. The use of the MEGAN-ECMWF inventory improves the model/data agreement in almost all regions, but biases persist over parts of Africa and the Northern Australia. Although neither GFED version is consistent with the data over all regions, a better match is achieved over Indonesia and Southern Africa when GFEDv2 is used, but GFEDv1 succeeds better in getting the correct seasonal patterns and intensities of the fire episodes over the Amazon basin, as reflected by the higher correlations calculated in this region.


2014 ◽  
Vol 14 (11) ◽  
pp. 5513-5527 ◽  
Author(s):  
C. L. Heald ◽  
D. A. Ridley ◽  
J. H. Kroll ◽  
S. R. H. Barrett ◽  
K. E. Cady-Pereira ◽  
...  

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.


2019 ◽  
Vol 19 (9) ◽  
pp. 6561-6577 ◽  
Author(s):  
Emily Ramnarine ◽  
John K. Kodros ◽  
Anna L. Hodshire ◽  
Chantelle R. Lonsdale ◽  
Matthew J. Alvarado ◽  
...  

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models have ignored sub-grid coagulation and instantly mixed fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem–TOMAS (TwO-Moment Aerosol Sectional) global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This cloud condensation nuclei (CCN) reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2, with assumed external mixing of black carbon and from −188 to −197 mW m−2 and with assumed internal mixing of black carbon with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories to various assumptions about the fresh biomass burning aerosol size distribution and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.


2011 ◽  
Vol 11 (17) ◽  
pp. 9067-9087 ◽  
Author(s):  
D. V. Spracklen ◽  
K. S. Carslaw ◽  
U. Pöschl ◽  
A. Rap ◽  
P. M. Forster

Abstract. Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (CCN) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to CCN has not been evaluated on the global scale. By combining extensive observations of CCN concentrations with the GLOMAP global aerosol model, we find that the model is biased low (normalised mean bias = −77 %) unless carbonaceous combustion aerosol act as CCN. We show that carbonaceous combustion aerosol accounts for more than half (52–64 %) of global CCN with the range due to uncertainty in the emitted size distribution of carbonaceous combustion particles. The model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean cloud albedo aerosol indirect effect of −0.34 W m−2, with stronger cooling if we assume smaller particle emission size. We calculate that carbonaceous combustion aerosol from pollution sources cause a global mean aerosol indirect effect of −0.23 W m−2. The small size of carbonaceous combustion particles from fossil fuel sources means that whilst pollution sources account for only one-third of the emitted mass they cause two-thirds of the cloud albedo aerosol indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for, along with other cloud effects not studied here, to ensure that black carbon emissions controls that reduce the high number concentrations of fossil fuel particles have the desired net effect on climate.


2018 ◽  
Author(s):  
Emily Ramnarine ◽  
John K. Kodros ◽  
Anna L. Hodshire ◽  
Chantelle R. Lonsdale ◽  
Matthew J. Alvarado ◽  
...  

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models ignore sub-grid coagulation and instantly mix fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem-TOMAS global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This CCN reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2 with assumed external mixing and from −188 to −197 mW m−2 with assumed internal mixing with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories, to various assumptions about the fresh biomass burning aerosol size distribution, and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.


Atmosphere ◽  
2021 ◽  
Vol 12 (11) ◽  
pp. 1478
Author(s):  
Andreas Pseftogkas ◽  
Maria-Elissavet Koukouli ◽  
Ioanna Skoulidou ◽  
Dimitrios Balis ◽  
Charikleia Meleti ◽  
...  

The aim of this paper is to apply a new lane separation methodology for the maritime sector emissions attributed to the different vessel types and marine traffic loads in the Mediterranean and the Black Sea defined via the European Marine and Observation Data network (EMODnet), developed in 2016. This methodology is implemented for the first time on the Copernicus Atmospheric Monitoring Service Global Shipping (CAMS-GLOB-SHIP v2.1) nitrogen oxides (NOX) emissions inventory, on the Sentinel-5 Precursor Tropospheric Monitoring Instrument (TROPOMI) nitrogen dioxide (NO2) tropospheric vertical column densities, and on the LOTOS-EUROS (Long Term Ozone Simulation—European Operational Smog) CTM (chemical transport model) simulations. By applying this new EMODnet-based lane separation method to the CAMS-GLOB-SHIP v2.1 emission inventory, we find that cargo and tanker vessels account for approximately 80% of the total emissions in the Mediterranean, followed by fishing, passenger, and other vessel emissions with contributions of 8%, 7%, and 5%, respectively. Tropospheric NO2 vertical column densities sensed by TROPOMI for 2019 and simulated by the LOTOS-EUROS CTM have been successfully attributed to the major vessel activities in the Mediterranean; the mean annual NO2 load of the observations and the simulations reported for the entire maritime EMODnet-reported fleet of the Mediterranean is in satisfactory agreement, 1.26 ± 0.56 × 1015 molecules cm−2 and 0.98 ± 0.41 × 1015 molecules cm−2, respectively. The spatial correlation of the annual maritime NO2 loads of all vessel types between observation and simulation ranges between 0.93 and 0.98. On a seasonal basis, both observations and simulations show a common variability. The wintertime comparisons are in excellent agreement for the highest emitting sector, cargo vessels, with the observations reporting a mean load of 0.98 ± 0.54 and the simulations of 0.81 ± 0.45 × 1015 molecules cm−2 and correlation of 0.88. Similarly, the passenger sector reports 0.45 ± 0.49 and 0.39 ± 0.45 × 1015 molecules cm−2 respectively, with correlation of 0.95. In summertime, the simulations report a higher decrease in modelled tropospheric columns than the observations, however, still resulting in a high correlation between 0.85 and 0.94 for all sectors. These encouraging findings will permit us to proceed with creating a top-down inventory for NOx shipping emissions using S5P/TROPOMI satellite observations and a data assimilation technique based on the LOTOS-EUROS chemical transport model.


2013 ◽  
Vol 13 (6) ◽  
pp. 3163-3176 ◽  
Author(s):  
J. R. Pierce ◽  
M. J. Evans ◽  
C. E. Scott ◽  
S. D. D'Andrea ◽  
D. K. Farmer ◽  
...  

Abstract. H2SO4 vapor is important for the nucleation of atmospheric aerosols and the growth of ultrafine particles to cloud condensation nuclei (CCN) sizes with important roles in the global aerosol budget and hence planetary radiative forcing. Recent studies have found that reactions of stabilized Criegee intermediates (CIs, formed from the ozonolysis of alkenes) with SO2 may be an important source of H2SO4 that has been missing from atmospheric aerosol models. For the first time in a global model, we investigate the impact of this new source of H2SO4 in the atmosphere. We use the chemical transport model, GEOS-Chem, with the online aerosol microphysics module, TOMAS, to estimate the possible impact of CIs on present-day H2SO4, CCN, and the cloud-albedo aerosol indirect effect (AIE). We extend the standard GEOS-Chem chemistry with CI-forming reactions (ozonolysis of isoprene, methyl vinyl ketone, methacrolein, propene, and monoterpenes) from the Master Chemical Mechanism. Using a fast rate constant for CI+SO2, we find that the addition of this chemistry increases the global production of H2SO4 by 4%. H2SO4 concentrations increase by over 100% in forested tropical boundary layers and by over 10–25% in forested NH boundary layers (up to 100% in July) due to CI+SO2 chemistry, but the change is generally negligible elsewhere. The predicted changes in CCN were strongly dampened to the CI+SO2 changes in H2SO4 in some regions: less than 15% in tropical forests and less than 2% in most mid-latitude locations. The global-mean CCN change was less than 1% both in the boundary layer and the free troposphere. The associated cloud-albedo AIE change was less than 0.03 W m−2. The model global sensitivity of CCN and the AIE to CI+SO2 chemistry is significantly (approximately one order-of-magnitude) smaller than the sensitivity of CCN and AIE to other uncertain model inputs, such as nucleation mechanisms, primary emissions, SOA (secondary organic aerosol) and deposition. Similarly, comparisons to size-distribution measurements show that uncertainties in other model parameters dominate model biases in the model-predicted size distributions. We conclude that improvement in the modeled CI+SO2 chemistry would not likely lead to significant improvements in present-day CCN and AIE predictions.


2017 ◽  
Vol 17 (10) ◽  
pp. 6305-6322 ◽  
Author(s):  
Anahita Amiri-Farahani ◽  
Robert J. Allen ◽  
David Neubauer ◽  
Ulrike Lohmann

Abstract. One component of aerosol–cloud interactions (ACI) involves dust and marine stratocumulus clouds (MSc). Few observational studies have focused on dust–MSc interactions, and thus this effect remains poorly quantified. We use observations from multiple sensors in the NASA A-Train satellite constellation from 2004 to 2012 to obtain estimates of the aerosol–cloud radiative effect, including its uncertainty, of dust aerosol influencing Atlantic MSc off the coast of northern Africa between 45° W and 15° E and between 0 and 35° N. To calculate the aerosol–cloud radiative effect, we use two methods following Quaas et al. (2008) (Method 1) and Chen et al. (2014) (Method 2). These two methods yield similar results of −1.5 ± 1.4 and −1.5 ± 1.6 W m−2, respectively, for the annual mean aerosol–cloud radiative effect. Thus, Saharan dust modifies MSc in a way that acts to cool the planet. There is a strong seasonal variation, with the aerosol–cloud radiative effect switching from significantly negative during the boreal summer to weakly positive during boreal winter. Method 1 (Method 2) yields −3.8 ± 2.5 (−4.3 ± 4.1) during summer and 1 ± 2.9 (0.6 ± 1) W m−2 during winter. In Method 1, the aerosol–cloud radiative effect can be decomposed into two terms, one representing the first aerosol indirect effect and the second representing the combination of the second aerosol indirect effect and the semidirect effect (i.e., changes in liquid water path and cloud fraction in response to changes in absorbing aerosols and local heating). The first aerosol indirect effect is relatively small, varying from −0.7 ± 0.6 in summer to 0.1 ± 0.5 W m−2 in winter. The second term, however, dominates the overall radiative effect, varying from −3.2 ± 2.5 in summer to 0.9 ± 2.9 W m−2 during winter. Studies show that the semidirect effect can result in a negative (i.e., absorbing aerosol lies above low clouds like MSc) or positive (i.e., absorbing aerosol lies within low clouds) aerosol–cloud radiative effect. The semipermanent MSc are low and confined within the boundary layer. CALIPSO shows that 61.8 ± 12.6 % of Saharan dust resides above North Atlantic MSc during summer for our study area. This is consistent with a relatively weak first aerosol indirect effect and also suggests the second aerosol indirect effect plus semidirect effect (the second term in Method 1) is dominated by the semidirect effect. In contrast, the percentage of Saharan dust above North Atlantic MSc in winter is 11.9 ± 10.9 %, which is much lower than in summer. CALIPSO also shows that 88.3 ± 8.5 % of dust resides below 2.2 km the winter average of MSc top height. During summer, however, there are two peaks, with 35.6 ± 13 % below 1.9 km (summer average of MSc top height) and 44.4 ± 9.2 % between 2 and 4 km. Because the aerosol–cloud radiative effect is positive during winter, and is also dominated by the second term, this again supports the importance of the semidirect effect. We conclude that Saharan dust–MSc interactions off the coast of northern Africa are likely dominated by the semidirect effect.


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