We present an emission inventory of primary black carbon (BC) and primary organic carbon (OC) aerosols from fossil fuel and biofuel combustion between 1850 and 2000. We reconstruct fossil fuel consumption and represent changes in technology on a national and sectoral basis. Our estimates rely on new estimates of biofuel consumption, and updated emission factors for old technologies. Emissions of black carbon increase almost linearly, totaling about 1000 Gg in 1850, 2200 Gg in 1900, 3000 Gg in 1950, and 4400 Gg in 2000. Primary organic carbon shows a similar pattern, with emissions of 4100 Gg, 5800 Gg, 6700 Gg, and 8700 Gg in 1850, 1900, 1950, and 2000, respectively. Biofuel is responsible for over half of BC emission until about 1890, and dominates energy‐related primary OC emission throughout the entire period. Coal contributes the greatest fraction of BC emission between 1880 and 1975, and is overtaken by emissions from biofuel around 1975, and by diesel engines around 1990. Previous work suggests a rapid rise in BC emissions between 1950 and 2000. This work supports a more gradual increase between 1950 and 2000, similar to the increase between 1850 and 1925; implementation of clean technology is a primary reason.

It is estimated that the combustion of biofuel generates 20% of all carbonaceous aerosols, yet these particles are studied less than those of other common sources. We designed and built a portable battery-operated emission-sampling cart to measure the real-time optical properties and other emission characteristics of biofuel cookstoves. In a field study in Honduras, we measured emission factors averaging 8.5 g/kg, higher than those found in previous laboratory studies. Strong flaming events emitted very dark particles with the optical properties of black particles. The elemental carbon to total carbon ratios ranged from 0.07 to 0.64, confirming that high elemental carbon fractions can be emitted from biofuel combustion and may not be used to distinguish fossil-fuel from biofuel sources when cooking is the dominant usage. Absorption Angstrom exponents, representing the dependence of absorption on wavelength, ranged from 1 (black) to 5 (yellow). Strongly absorbing particles with absorption inversely dependent on wavelength were emitted separately from particles with weak absorption and strong wavelength dependence; the latter probably contained conjugated aromatic compounds. Because combustion occurs in distinct phases, different types of carbonaceous aerosols from biofuel combustion are externally mixed at emission and may have different atmospheric fates.

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Particulate emissions from low-temperature biomass burning are dominated by organic matter. Here, we show that such emissions have a liquid, bead-like appearance when collected on fibrous filters, and the number of these beads are far less than expected for solid spherical particles. These shapes are in line with published drop-on-fiber theories for liquids entrained on filaments. A smoldering pine sample is yellowish, with organic carbon over 99% of the total carbon, and chars substantially in thermal-optical analysis (TOA), indicating that such liquid organic particles could affect both absorption measurements and TOA of such samples. Similar colored samples collected in the field from rice-straw burning and cook stove emissions also show a similar liquid appearance.