Insight into the molecular photooxidation evolution mechanism of brown carbon released from residential solid fuel combustion

Wang, Diwei; Shen, Zhenxing; Bai, Gezi; Zhang, Leiming; Huang, Shasha; Sun, Jian; Xu, Hongmei; Cao, Junji

Insight into the molecular photooxidation evolution mechanism of brown carbon released from residential solid fuel combustion

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dc.contributor.author: Wang, Diwei; Shen, Zhenxing; Bai, Gezi; Zhang, Leiming; Huang, Shasha; Sun, Jian; Xu, Hongmei; Cao, Junji
dc.date.accepted: 2024-12-17
dc.date.accessioned: 2025-05-29T17:29:47Z
dc.date.available: 2025-05-29T17:29:47Z
dc.date.issued: 2024-12-30
dc.date.submitted: 2024-06-19
dc.description.abstract - en: Solid fuels were one of the important emission sources of brown carbon (BrC). This study investigates molecular composition of BrC derived from combustion of five types of residential solid fuels (i.e., firewood, corn cob, bituminous coal, anthracite, and biomass briquette) and their photooxidation evolution mechanisms using an oxidation flow reactor. Results show that nitrogen-containing and sulfur-containing organic compounds are the main components of molecular composition of methanol-soluble organic compounds (MSOC) emitted from these fuels, with their intensity being 33%~43% and 23%~56%, respectively, depending on fuel type. The photooxidation processes mediated by NO3∙ and ∙OH significantly altered the molecular composition and distribution of aged MSOC. The formation of typical nitrogen-containing BrC chromophores (e.g., nitro-aromatic compounds) also proves the role of NO3∙ in the photooxidation reaction. However, the photo-enhancement effect of NO3∙ mediated photooxidation reaction could not offset the destruction of the molecular conjugation degree and aromaticity of BrC by ∙OH oxidation, resulting in a significant reduction in the light absorption capacity of BrC. The mass absorption coefficient at 365 nm of BrC aged for 12 days derived from the remaining fuels decreased by 47.0% to 55.8% compared to that of fresh BrC, except for firewood, which only decreased by 5.3%. These findings on the molecular evolution and oxidation mechanism of BrC generated from solid fuels are useful in reducing uncertainties in climate change studies involving BrC aerosol.
dc.description.fosrcfull - en: An edited version of this paper was published by AGU. Published 2024 American Geophysical Union.
dc.description.fosrcfull-fosrctranslation - fr: Une version éditée de cet article a été publiée par l'AGU. Publié 2024 American Geophysical Union.
dc.identifier.issn: 2169-8996; 2169-897X
dc.identifier.uri: https://open-science.canada.ca/handle/123456789/3635
dc.language.iso: en
dc.publisher - en: American Geophysical Union
dc.publisher - fr: American Geophysical Union
dc.relation.isreplacedby: https://doi.org/10.1029/2024JD041827
dc.rights - en: Other
dc.rights - fr: Autre
dc.rights.openaccesslevel - en: Green
dc.rights.openaccesslevel - fr: Vert
dc.rights.uri - en: #description-element
dc.rights.uri - fr: #description-element
dc.subject - en: Fuels; Atmospheric emissions; Air quality
dc.subject - fr: Combustible; Émissions atmosphériques; Qualité de l'air
dc.subject.en - en: Fuels; Atmospheric emissions; Air quality
dc.subject.fr - fr: Combustible; Émissions atmosphériques; Qualité de l'air
dc.title - en: Insight into the molecular photooxidation evolution mechanism of brown carbon released from residential solid fuel combustion
dc.type - en: Accepted manuscript
dc.type - fr: Manuscrit accepté
local.article.journalissue: 1
local.article.journaltitle - en: Journal of Geophysical Research: Atmospheres
local.article.journalvolume: 130
local.pagination: 35 pages
local.peerreview - en: Yes
local.peerreview - fr: Oui