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- Title
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon.
- Authors
Ji, Yuemeng; Shi, Zhang; Li, Wenjian; Wang, Jiaxin; Shi, Qiuju; Li, Yixin; Gao, Lei; Ma, Ruize; Lu, Weijun; Xu, Lulu; Gao, Yanpeng; Li, Guiying; An, Taicheng
- Abstract
The aqueous-phase chemistry of glyoxal (GL) with reduced nitrogen compounds (RNCs) is a significant source for secondary brown carbon (SBrC), which is one of the largest uncertainties in climate predictions. However, a few studies have revealed that SBrC formation is affected by multifunctional RNCs, which have a non-negligible atmospheric abundance. Hence, we assessed theoretical and experimental approaches to investigate the reaction mechanisms and kinetics of the mixtures for ammonium sulfate (AS), multifunctional amine monoethanolamine (MEA), and GL. Our experiments indicate that light absorption and growth rate are enhanced more efficiently in the MEA–GL mixture relative to AS–GL and MEA–AS–GL mixtures and MEA reactions of the chromophores than in the analogous AS reactions. Quantum chemical calculations show that the formation and propagation of oligomers proceed via four-step nucleophilic addition reactions in three reaction systems. The presence of MEA provides the two extra branched chains that affect the natural charges and steric hindrance of intermediates, facilitating the formation of chromophores. Molecule dynamics simulations reveal that the interfacial and interior attraction on the aqueous aerosols with MEA is more pronounced for small α -dicarbonyls to facilitate further engagement in the aqueous-phase reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
- Subjects
GLYOXAL; NUCLEOPHILIC reactions; STERIC hindrance; ADDITION reactions; LIGHT absorption; AMMONIUM sulfate; NITROGEN compounds
- Publication
Atmospheric Chemistry & Physics, 2024, Vol 24, Issue 5, p3079
- ISSN
1680-7316
- Publication type
Article
- DOI
10.5194/acp-24-3079-2024