Brown Carbon Formation Potential of the Biacetyl–Ammonium Sulfate Reaction System

The contribution of organic aerosol from biomass burning is poorly constrained, and the lack of consensus regarding its overall contribution to global radiative forcing leads to significant uncertainties in climate modeling. Identification of potential brown carbon chromophores from common biomass b...

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Veröffentlicht in:ACS earth and space chemistry 2020-07, Vol.4 (7), p.1104-1113
Hauptverfasser: Grace, Daisy N, Lugos, Emily N, Ma, Shiqing, Griffith, Daniel R, Hendrickson, Heidi P, Woo, Joseph L, Galloway, Melissa M
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Sprache:eng
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Zusammenfassung:The contribution of organic aerosol from biomass burning is poorly constrained, and the lack of consensus regarding its overall contribution to global radiative forcing leads to significant uncertainties in climate modeling. Identification of potential brown carbon chromophores from common biomass burning emissions may reduce this uncertainty. Biacetyl (BA) is found in emissions from industry and biomass burning from various ecosystems and shares structural similarities with other small carbonyls that react with ammonium sulfate (AS) to produce brown carbon compounds. Like previous carbonyl + AS studies, the BA + AS system results in the formation of hundreds of different products; these were separated and identified using supercritical fluid chromatography–tandem mass spectrometry, isotopic substitution experiments, and comparisons to standards. Kinetic information was obtained through spectral decomposition of experimentally measured UV–visible absorbance data. Theoretical TDDFT calculations were utilized to extract more information on the light absorbance of identified products and to determine how these individual chromophores would contribute to the light absorbance of organic aerosol. This information could provide insight into unknown organic aerosol behavior by furthering our understanding of the reactivity of a common biomass burning emission product like biacetyl.
ISSN:2472-3452
2472-3452
DOI:10.1021/acsearthspacechem.0c00096