Characterization and dark oxidation of the emissions of a pellet stove

Abstract

Pellet combustion in residential heating stoves has increased globally during the last decade. Despite their high combustion efficiency, the widespread use of pellet stoves is expected to adversely impact air quality. The atmospheric aging of pellet emissions has received even less attention, focusing mainly on daytime conditions, while the degree to which pellet emissions undergo night-time aging as well as the role of relative humidity remain poorly understood. In this study, environmental simulation chamber experiments were performed to characterize the fresh and aged organic aerosol (OA) emitted by a pellet stove. The fresh pellet stove PM₁ (particulate matter with an aerodynamic diameter less than 1 μm) emissions consisted mainly of OA (93 ± 4%, mean ± standard deviation) and black carbon (5 ± 3%). The primary OA (POA) oxygen-to-carbon ratio (O : C) was 0.58 ± 0.04, higher than that of fresh logwood emissions. The fresh OA at a concentration of 70 μg m⁻³ (after dilution and equilibration in the chamber) consisted of semi-volatile (68%), low and extremely low volatility (16%) and intermediate-volatility (16%) compounds. The oxidation of pellet emissions under dark conditions was investigated by injecting nitrogen dioxide (NO₂) and ozone (O₃) into the chamber, at different (10–80%) relative humidity (RH) levels. In all dark aging experiments secondary organic aerosol (SOA) formation was observed, increasing the OA levels after a few hours of exposure to NO₃ radicals. The change in the aerosol composition and the extent of oxidation depended on RH. For low RH, the SOA mass formed was up to 30% of the initial OA, accompanied by a moderate change in both O : C levels (7–8% increase) and the OA spectrum. Aging under higher RH conditions (60–80%) led to a more oxygenated aerosol (increase in O : C of 11–18%), but only a minor (1–10%) increase in OA mass. The increase in O : C at high RH indicates the importance of heterogeneous aqueous reactions in this system, that oxidize the original OA with a relatively small net change in the OA mass. These results show that the OA in pellet emissions can chemically evolve under low photochemical activity (e.g. the wintertime period) with important enhancement in SOA mass under certain conditions.