State Key Laboratory of Loess Science, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China.
Institute of Global Environmental Change, Xi'an Jiaotong University, Xi'an 710049, China.
Environ Sci Technol. 2024 Oct 1;58(39):17344-17354. doi: 10.1021/acs.est.4c05558. Epub 2024 Sep 19.
Brown carbon (BrC) from biomass burning constitutes a significant portion of light-absorbing components in the atmosphere. Although the aging of BrC surrogates from biomass burning has been studied in many laboratory settings, BrC aging behavior in real-world urban environments is not well understood. In this study, through a combination of online dynamic monitoring and offline molecular characterization, the ambient optical aging of BrC was linked to its dynamic changes in molecular composition. Enhanced light absorption by BrC was consistently observed during the periods dominated by oxygenated biomass burning organic aerosol (BBOA), in contrast to periods dominated by primary emissions or secondary formation in aqueous-phase. This enhancement was linked to the formation of nitrogen-containing compounds during the ambient aging of BBOA. Detailed molecular characterization, alongside analysis of environmental parameters, revealed that an increased atmospheric oxidizing capacity, marked by elevated levels of ozone and nighttime NO radicals, facilitated the formation of nitrated aromatic BrC chromophores. These chromophores were primarily responsible for the enhanced light absorption during the ambient aging of BBOA. This study elucidates the nitration processes that enhance BrC light absorption for ambient BBOA, and highlights the crucial role of meteorological conditions. Furthermore, our findings shed light on the chemical and optical aging processes of biomass burning BrC in ambient air, offering insights into its environmental behavior and effects.
棕色碳(BrC)来自生物质燃烧,构成了大气中光吸收成分的重要部分。尽管在许多实验室环境中已经研究了生物质燃烧的 BrC 示踪物的老化,但在现实城市环境中,BrC 的老化行为还没有得到很好的理解。在这项研究中,通过在线动态监测和离线分子特征化的结合,将 BrC 的环境光老化与其分子组成的动态变化联系起来。在含氧生物质燃烧有机气溶胶(BBOA)主导的时期,BrC 的光吸收增强一直被观察到,而在以一次排放或水相二次形成为主的时期则没有这种现象。这种增强与 BBOA 环境老化过程中含氮化合物的形成有关。详细的分子特征化,以及环境参数的分析,表明大气氧化能力的增强,以臭氧和夜间 NO 自由基水平的升高为标志,促进了硝化芳香族 BrC 生色团的形成。这些生色团是 BBOA 环境老化过程中增强光吸收的主要原因。本研究阐明了增强 BrC 光吸收的硝化过程,强调了气象条件的关键作用。此外,我们的发现揭示了大气中生物质燃烧 BrC 的化学和光学老化过程,为其环境行为和影响提供了新的认识。