Abstract

Interactions between anthropogenic and biogenic emissions, and implications for aerosol production, have raised particular scientific interest. Despite active research in this area, real anthropogenic emission sources have not been exploited for anthropogenic-biogenic interaction studies until now. This work examines these interactions using α-pinene and pellet boiler emissions as a model test system. The impact of pellet boiler emissions on secondary organic aerosol (SOA) formation from α-pinene photo-oxidation was studied under atmospherically relevant conditions in an environmental chamber. The aim of this study was to identify which of the major pellet exhaust components (including high nitrogen oxide (NOx), primary particles, or a combination of the two) affected SOA formation from α-pinene. Results demonstrated that high NOx concentrations emitted by the pellet boiler reduced SOA yields from α-pinene, whereas the chemical properties of the primary particles emitted by the pellet boiler had no effect on observed SOA yields. The maximum SOA yield of α-pinene in the presence of pellet boiler exhaust (under high-NOx conditions) was 18.7% and in the absence of pellet boiler exhaust (under low-NOx conditions) was 34.1%. The reduced SOA yield under high-NOx conditions was caused by changes in gas-phase chemistry that led to the formation of organonitrate compounds.

Highlights

  • Volatile organic compounds (VOCs) are emitted into the atmosphere from biogenic and anthropogenic sources. Once they are in the atmosphere, VOCs undergo a number of chemical and physical processes that result in the formation of secondary pollutants, such as ozone and secondary organic aerosols (SOA).[1,2]

  • We first characterize the primary emissions from the pellet boiler to provide context for the possible interactions that could occur between pellet boiler emissions and α-pinene

  • We characterize SOA formation from pellet boiler emissions with and without α-pinene. These results demonstrated that the primary source of SOA in these experiments was derived from the oxidation of α-pinene and not from the oxidation of the pellet boiler emissions themselves

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Summary

Introduction

Volatile organic compounds (VOCs) are emitted into the atmosphere from biogenic and anthropogenic sources. Once they are in the atmosphere, VOCs undergo a number of chemical and physical processes that result in the formation of secondary pollutants, such as ozone and secondary organic aerosols (SOA).[1,2] SOA, a major component of atmospheric aerosols, impacts climate by influencing the size distribution, chemical composition, and radiative and cloud formation properties of the atmospheric particle population.[3,4] accurate representations of SOA production are crucial for reducing uncertainties in climate change estimates. Models continue to underestimate SOA production when compared to field measurements.[4] The largest source of atmospheric VOCs that lead to SOA formation is emissions from vegetation, called biogenic volatile organic compounds (BVOCs). Anthropogenic emissions can dominate VOCs in urban areas[8−10] and are a major source of primary particulate pollution with a global estimate of 65 Tg yr−1.11

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