Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 2: Chemical properties and characterization

There are many fuels used for domestic purposes in east Africa, producing a significant atmospheric burden of the resulting aerosols, which includes biomass burning particles. However, the aerosol physicochemical properties are poorly understood. Here, the combustion of eucalyptus, acacia, and olive fuels was performed at 500 and 800 ∘C in a tube furnace, followed by immediate filter collection for fresh samples or introduction into a photochemical chamber to simulate atmospheric photochemical aging under the influence of anthropogenic emissions. The aerosol generated in the latter experiment was collected onto filters after 12 h of photochemical aging. 500 and 800 ∘C were selected to simulate smoldering and flaming combustion, respectively, and to cover a range of combustion conditions. Methanol extracts from Teflon filters were analyzed by ultra-performance liquid chromatography interfaced to both a diode array detector and an electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer (UPLC/DAD-ESI-HR-QTOFMS) to determine the light absorption properties of biomass burning organic aerosol constituents chemically characterized at the molecular level. Few chemical or UV–visible (UV: ultraviolet) differences were apparent between samples for the fuels when combusted at 800 ∘C. Differences in single-scattering albedo (SSA) between fresh samples at this temperature were attributed to compounds not captured in this analysis, with eucalyptol being one suspected missing component. For fresh combustion at 500 ∘C, many species were present; lignin pyrolysis and distillation products are more prevalent in eucalyptus, while pyrolysis products of cellulose and at least one nitro-aromatic species were more prevalent in acacia. SSA trends are consistent with this, particularly if the absorption of those chromophores extends to the 500–570 nm region. Upon aging, both show that resorcinol or catechol was removed to the highest degree, and both aerosol types were dominated by loss of pyrolysis and distillation products, though they differed in the specific compounds being consumed by the photochemical aging process.

Overview of aerosol optical properties over southern West Africa from DACCIWA aircraft measurements

Southern West Africa (SWA) is an African pollution hotspot but a relatively poorly sampled region of the world. We present an overview of in situ aerosol optical measurements collected over SWA in June and July 2016 as part as of the DACCIWA (Dynamics-Aerosol-Chemistry-Clouds Interactions in West Africa) airborne campaign. The aircraft sampled a wide range of air masses, including anthropogenic pollution plumes emitted from the coastal cities, long-range transported biomass burning plumes from central and southern Africa and dust plumes from the Sahara and Sahel region, as well as mixtures of these plumes. The specific objective of this work is to characterize the regional variability of the vertical distribution of aerosol particles and their spectral optical properties (single scattering albedo: SSA, asymmetry parameter, extinction mass efficiency, scattering Ångström exponent and absorption Ångström exponent: AAE). The first findings indicate that aerosol optical properties in the planetary boundary layer were dominated by a widespread and persistent biomass burning loading from the Southern Hemisphere. Despite a strong increase in aerosol number concentration in air masses downwind of urban conglomerations, spectral SSA were comparable to the background and showed signatures of the absorption characteristics of biomass burning aerosols. In the free troposphere, moderately to strongly absorbing aerosol layers, dominated by either dust or biomass burning particles, occurred occasionally. In aerosol layers dominated by mineral dust particles, SSA varied from 0.81 to 0.92 at 550 nm depending on the variable proportion of anthropogenic pollution particles externally mixed with the dust. For the layers dominated by biomass burning particles, aerosol particles were significantly more light absorbing than those previously measured in other areas (e.g. Amazonia, North America), with SSA ranging from 0.71 to 0.77 at 550 nm. The variability of SSA was mainly controlled by variations in aerosol composition rather than in aerosol size distribution. Correspondingly, values of AAE ranged from 0.9 to 1.1, suggesting that lens-coated black carbon particles were the dominant absorber in the visible range for these biomass burning aerosols. Comparison with the literature shows a consistent picture of increasing absorption enhancement of biomass burning aerosol from emission to remote location and underscores that the evolution of SSA occurred a long time after emission. The results presented here build a fundamental basis of knowledge about the aerosol optical properties observed over SWA during the monsoon season and can be used in climate modelling studies and satellite retrievals. In particular and regarding the very high absorbing properties of biomass burning aerosols over SWA, our findings suggest that considering the effect of internal mixing on absorption properties of black carbon particles in climate models should help better assess the direct and semi-direct radiative effects of biomass burning particles.

Laboratory studies of fresh and aged biomass burning aerosols emitted from east African biomass fuels – Part 2: Chemical properties and characterization

There are many fuels used for domestic purposes in east Africa, producing a significant atmospheric burden of the resulting aerosols, which includes biomass burning particles. However, the aerosol physicochemical properties are poorly understood. Here, combustion of Eucalyptus and Acacia fuels was performed at 500 and 800 °C in a tube furnace, followed by immediate filter collection for fresh samples or introduction into a photochemical chamber to simulate atmospheric photochemical aging under the influence of anthropogenic emissions. The aerosol generated in the latter experiment was collected onto filters after 12 hours of photochemical aging. 500 and 800 °C were selected to simulate smoldering and flaming combustion, respectively, and to cover a range of combustion conditions. Methanol extracts from Teflon filters were analyzed by ultra-performance liquid chromatography interfaced to both a diode array detector and an electrospray ionization high-resolution quadrupole time-of-flight mass spectrometer (UPLC/DAD-ESI-HR-QTOFMS) to determine the light-absorption properties of biomass burning organic aerosol constituents chemically characterized at the molecular level. Few chemical or UV/Visible differences were apparent between samples for either fuel when combusted at 800 °C. Differences in single scattering albedo (SSA) between fresh samples at this temperature were attributed to compounds not captured in this analysis, with eucalyptol being one suspected missing component. For fresh combustion at 500 °C, many species were present, where lignin pyrolysis and distillation products are more prevalent in Eucalyptus, while pyrolysis products of cellulose and at least one nitroaromatic species were more prevalent in Acacia. SSA trends are consistent with this, particularly if the absorption of those chromophores extends to the 500–570 nm region. Upon aging, both show that resorcinol or catechol was removed to the highest degree, and both aerosol types were dominated by loss of pyrolysis and distillation products, though both differed in the specific compounds being consumed by the photochemical aging process.

Interaction between biomass-burning aerosol and clouds under different climate/weather regimes

<p>The maritime continent in Southeast Asia is characterized by the frequent convective activities on a wide range of scales, as well as by the seasonal emissions of biomass-burning particles. The emission of biomass-burning particles in this region typically peaks in September and October, whereas its intensity varies considerably from year to year. Since the atmospheric circulation over the region is heavily influenced by a range of meteorological and climatological variabilities, such as ENSO, it is important to quantitatively examine the impacts of biomass-burning particles on clouds while taking weather/climate regimes into account. We investigate the effects of biomass-burning particles on clouds, especially convective ones, with cloud-resolving simulations by the WRF-CHEM model. Instead of focusing on a particular case, our simulations cover an extended period of time in the month of September, allowing us to examine both individual convection and an ensemble of convective clouds developing under different weather/climate regimes and hence different aerosol abundance and distributions. Such long-term and high-resolution simulations over the region will give us an insight into the climate-regime dependent two-way interaction between aerosols and clouds.</p>

Optical Properties of Canadian Biomass Burning Particles Over Europe Observed with Calipso and Ground-Based Lidar Systems

A long-lasting biomass burning event affected Europe from 27 August to 3 September 2018. The biomass burning aerosol layers were observed with ground- and space-based lidars in heights ranged between 2-7 km (a.s.l.). The mean backscatter coefficient for the ground-based stations ranged between 0.29 and 1.51 Mm-1sr-1, while the CALIPSO retrieved values ranged between 0.43 and 1.83 Mm-1sr-1. Moreover, the mean Ångström exponent (AEb) values, relevant to backscatter, ranged from 0.83 to 1.04 for the aforementioned lidar stations. At the same time, the mean AEb values obtained from CALIPSO ranged between 0.17 and 1.89. The mean particle depolarization ratio ranged between 0.037 and 0.080.

Light absorption properties of aerosols over Southern West Africa

Southern West Africa (SWA) is an African pollution hotspot but a relatively poorly sampled region of the world. We present an overview of in-situ aerosol optical measurements collected over SWA in June and July 2016 as part as the DACCIWA (Dynamics–Aerosol–Chemistry–Clouds Interactions in West Africa) airborne campaign. The aircraft sampled a wide range of air masses, including anthropogenic pollution plumes emitted from the coastal cities, long-range transported biomass burning plumes from Central and Southern Africa and dust plumes from the Sahara and Sahel region, as well as mixtures of these plumes. The specific objective of this work is to characterize the regional variability of the vertical distribution of aerosol particles and their spectral optical properties (single scattering albedo: SSA, asymmetry parameter, extinction mass efficiency, scattering Ångström exponent and absorption Ångström exponent: AAE). First findings indicate that aerosol optical properties in the planetary boundary layer were dominated by a widespread and persistent biomass burning loading from the Southern Hemisphere. Despite a strong increase of aerosol number concentration in air masses downwind of urban conglomerations, spectral SSA were comparable to the background and showed signatures of the absorption characteristics of biomass burning aerosols. In the free troposphere, moderately to strongly absorbing aerosol layers, dominated by either dust or biomass burning particles, occurred occasionally. In aerosol layers dominated by mineral dust particles, SSA varied from 0.81 to 0.92 at 550 nm depending on the variable proportion of anthropogenic pollution particles externally mixed with the dust. Biomass burning aerosol particles were significantly more light absorbing than those previously measured in other areas (e.g. Amazonia, North America) with SSA ranging from 0.71 to 0.77 at 550 nm. The variability of SSA was mainly controlled by variations in aerosol composition rather than in aerosol size distribution. Correspondingly, values of AAE ranged from 0.9 to 1.1, suggesting that lens-coated black carbon particles were the dominant absorber in the visible range for these biomass burning aerosols. Comparison with literature shows a consistent picture of increasing absorption enhancement of biomass burning aerosol from emission to remote location and underscores that the evolution of SSA occurred a long time after emission. The results presented here build a fundamental basis of knowledge about the aerosol optical properties observed over SWA during the monsoon season and can be used in climate modelling studies and satellite retrievals. In particular and regarding the very high absorbing properties of biomass burning aerosols over SWA, our findings suggest that considering the effect of internal mixing on absorption properties of black carbon particles in climate models should help better assessing the direct and semi-direct radiative effects of biomass burning particles.