Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.
Department of Chemistry, University of California , Irvine, California 92697, United States.
Environ Sci Technol. 2016 Nov 1;50(21):11815-11824. doi: 10.1021/acs.est.6b03024. Epub 2016 Oct 18.
Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly emitted biomass burning organic aerosol (BBOA) samples collected during test burns of sawgrass, peat, ponderosa pine, and black spruce. We demonstrate that both the BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels. Common BrC chromophores in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as source-specific markers of BrC. On average, ∼50% of the light absorption in the solvent-extractable fraction of BBOA can be attributed to a limited number of strong BrC chromophores. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of ∼16 h. A "molecular corridor" analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low saturation mass concentration (<1 μg m) and will be retained in the particle phase under atmospherically relevant conditions.
生物质燃烧排放物是大气中棕色碳 (BrC) 的重要来源。在本研究中,我们研究了在锯齿草、泥炭、黄松和黑云杉的测试燃烧过程中收集的新鲜生物质燃烧有机气溶胶 (BBOA) 样品的分子组成。我们证明,BrC 吸收和光吸收化合物的化学成分都显著取决于生物质燃料的类型。在选定的 BBOA 样品中,常见的 BrC 生色团包括硝基芳烃、多环芳烃衍生物和多酚,它们具有广泛的分子量、结构和光吸收特性。观察到一些生物燃料特有的 BrC 生色团,表明其中一些可能被用作 BrC 的特定来源标记物。平均而言,BBOA 中可溶剂萃取部分的光吸收的约 50%可归因于少数强 BrC 生色团。BBOA 的吸收系数受太阳光解的影响。具体来说,在典型的大气条件下,300nm 的吸光度衰减半衰期约为 16 小时。BBOA 挥发性分布的“分子走廊”分析表明,新鲜 BBOA 中的许多 BrC 化合物的饱和质量浓度较低(<1μg m),并且在大气相关条件下将保留在颗粒相中。