Brown Carbon Formation Potential of the Biacetyl–Ammonium Sulfate Reaction System,ACS Earth and Space Chemistry

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Brown Carbon Formation Potential of the Biacetyl–Ammonium Sulfate Reaction System
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-06-08 , DOI: 10.1021/acsearthspacechem.0c00096
Daisy N. Grace ₁ , Emily N. Lugos ₁ , Shiqing Ma ₂ , Daniel R. Griffith ₁ , Heidi P. Hendrickson ₁ , Joseph L. Woo ₂ , Melissa M. Galloway ₁

Affiliation

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.

中文翻译：

联乙酰-硫酸铵反应体系的褐碳形成潜能

生物质燃烧过程中有机气溶胶的贡献受到限制，并且就其对全球辐射强迫的总体贡献缺乏共识，导致气候模型的重大不确定性。从常见的生物质燃烧排放中识别出潜在的棕色碳发色团可以减少这种不确定性。在工业和各种生态系统燃烧的生物质的排放物中发现了联乙酰（BA），并且与其他小羰基具有结构相似性，这些小羰基与硫酸铵（AS）反应生成棕色碳化合物。像以前的羰基+ AS研究一样，BA + AS系统导致形成数百种不同的产物。使用超临界流体色谱-串联质谱，同位素替代实验以及与标准品的比较对这些化合物进行分离和鉴定。动力学信息是通过光谱分解实验测得的紫外可见吸光度数据而获得的。理论TDDFT计算用于提取有关已鉴定产品的吸光度的更多信息，并确定这些单个生色团如何促进有机气溶胶的吸光度。通过加深我们对常见生物质燃烧排放产物（如联乙酰）的反应性的了解，该信息可以提供有关未知有机气溶胶行为的见解。理论TDDFT计算用于提取有关已鉴定产品的吸光度的更多信息，并确定这些单个生色团如何促进有机气溶胶的吸光度。通过加深我们对常见生物质燃烧排放产物（如联乙酰）的反应性的了解，该信息可以提供对未知有机气溶胶行为的了解。理论TDDFT计算用于提取有关已鉴定产品的吸光度的更多信息，并确定这些单个生色团如何促进有机气溶胶的吸光度。通过加深我们对常见生物质燃烧排放产物（如联乙酰）的反应性的了解，该信息可以提供有关未知有机气溶胶行为的见解。

更新日期：2020-07-16

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