The aim was to identify relationships between combustion conditions, particle characteristics, and optical properties of fresh and photochemically processed emissions from biomass combustion. The combustion conditions included nominal and high burn rate operation and individual combustion phases from a conventional wood stove. Low temperature pyrolysis upon fuel addition resulted in "tar-ball" type particles dominated by organic aerosol with an absorption Ångström exponent (AAE) of 2.5-2.7 and estimated Brown Carbon contributions of 50-70% to absorption at the climate relevant aethalometer-wavelength (520 nm). High temperature combustion during the intermediate (flaming) phase was dominated by soot agglomerates with AAE 1.0-1.2 and 85-100% of absorption at 520 nm attributed to Black Carbon. Intense photochemical processing of high burn rate flaming combustion emissions in an oxidation flow reactor led to strong formation of Secondary Organic Aerosol, with no or weak absorption. PM1 mass emission factors (mg/kg) of fresh emissions were about an order of magnitude higher for low temperature pyrolysis compared to high temperature combustion. However, emission factors describing the absorption cross section emitted per kg of fuel consumed (m(2)/kg) were of similar magnitude at 520 nm for the diverse combustion conditions investigated in this study. These results provide a link between biomass combustion conditions, emitted particle types, and their optical properties in fresh and processed plumes which can be of value for source apportionment and balanced mitigation of biomass combustion emissions from a climate and health perspective.

In this study, ash transformation and release of critical ash-forming elements during single-pellet combustion of different types of agricultural opportunity fuels were investigated. The work focused on potassium (K) and phosphorus (P). Single pellets of poplar, wheat straw, grass, and wheat grain residues were combusted in a macro-thermogravimetric analysis reactor at three different furnace temperatures (600, 800, and 950 °C). In order to study the transformation of inorganic matters at different stages of the thermal conversion process, the residues were collected before and after full devolatilization, as well as after complete char conversion. The residual char/ash was characterized by scanning electron microscopy–energy-dispersive X-ray spectroscopy, X-ray diffraction, inductively coupled plasma, and ion chromatography, and the interpretation of results was supported by thermodynamic equilibrium calculations. During combustion of poplar, representing a Ca–K-rich woody energy crop, the main fraction of K remained in the residual ash primarily in the form of K2Ca­(CO3)2 at lower temperatures and in a K–Ca-rich carbonate melt at higher temperatures. Almost all P retained in the ash and was mainly present in the form of hydroxyapatite. For the Si–K-rich agricultural biomass fuels with a minor (wheat straw) or moderate (grass) P content, the main fraction of K remained in the residual ash mostly in K–Ca-rich silicates. In general, almost all P was retained in the residual ash both in K–Ca–P–Si-rich amorphous structures, possibly in phosphosilicate-rich melts, and in crystalline forms as hydroxyapatite, CaKPO4, and calcium phosphate silicate. For the wheat grain, representing a K–P-rich fuel, the main fraction of K and P remained in the residual ash in the form of K–Mg-rich phosphates. The results showed that in general for all studied fuels, the main release of P occurred during the devolatilization stage, while the main release of K occurred during char combustion. Furthermore, less than 20% of P and 35% of K was released at the highest furnace temperature for all fuels.

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In this study, ash transformation during fixed-bed combustion of different agricultural opportunity fuels was investigated with a special focus on potassium (K) and phosphorus (P). The fuel pellets were combusted in an underfed fixed-bed pellet burner. Residual ashes (bottom ash and slag) and particulate matter were collected and characterized by scanning electron microscopy–energy-dispersive X-ray spectroscopy, X-ray diffraction, inductively coupled plasma, and ion chromatography. The interpretation of the results was supported by thermodynamic equilibrium calculations. For all fuels, almost all P (>97%) was found in residual-/coarse ash fractions, while K showed different degrees of volatilization, depending on fuel composition. During combustion of poplar, which represents Ca–K-rich fuels, a carbonate melt rich in K and Ca decomposed into CaO, CO2, and gaseous K species at sufficiently high temperatures. Ca5(PO4)3OH was the main P-containing crystalline phase in the bottom ash. For wheat straw and grass, representing Si–K-rich fuels, a lower degree of K volatilization was observed than for poplar. P was found here in amorphous phosphosilicates and CaKPO4. For wheat grain residues, representing P–K-rich fuels, a high degree of both K and P retention was observed due to the interaction of K and P with the fuel-bed constituents, i.e., char, ash, and slag. The residual ash was almost completely melted and rich in P, K, and Mg. P was found in amorphous phosphates and different crystalline phases such as KMgPO4, K2CaP2O7, K2MgP2O7, and K4Mg4(P2O7)3. In general, the results therefore imply that an interaction between ash-forming elements in a single burning fuel particle and the surrounding bed ash or slag is important for the overall retention of P and K during fuel conversion in fixed-bed combustion of agricultural biomass fuels.

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Abstract. This research was part of the Salutary Umeå Study of Aerosols in Biomass Cookstove Emissions (SUSTAINE) laboratory experiment campaign. We studied ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves, using a portable ice nuclei counter, Spectrometer Ice Nuclei (SPIN). These emissions were generated from two traditional cookstove types commonly used for household cooking in sub-Saharan Africa and two advanced gasifier stoves under research to promote sustainable development alternatives. The solid fuels studied included biomass from two different African tree species, Swedish softwood and agricultural residue products relevant to the region. Measurements were performed with a modified version of the standard water boiling test on polydisperse samples from flue gas during burning and size-selected accumulation mode soot particles from a 15 m3 aerosol-storage chamber. The studied soot particle sizes in nanometers were 250, 260, 300, 350, 400, 450 and 500. From this chamber, the particles were introduced to water-supersaturated freezing conditions (−32 to −43 ∘C) in the SPIN. Accumulation mode soot particles generally produced an ice-activated fraction of 10−3 in temperatures 1–1.5 ∘C higher than that required for homogeneous freezing at fixed RHw=115 %. In five special experiments, the combustion performance of one cookstove was intentionally modified. Two of these exhibited a significant increase in the ice-nucleating ability of the particles, resulting in a 10−3 ice activation at temperatures up to 5.9 ∘C higher than homogeneous freezing and the observed increased ice-nucleating ability. We investigated six different physico-chemical properties of the emission particles but found no clear correlation between them and increasing ice-nucleating ability. We conclude that the freshly emitted combustion aerosols form ice via immersion and condensation freezing at temperatures only moderately above homogeneous freezing conditions.

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