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Discussion papers
https://doi.org/10.5194/acp-2019-584
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-584
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 07 Aug 2019

Submitted as: research article | 07 Aug 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Molecular compositions and optical properties of dissolved brown carbon in smoke particles illuminated by excitation-emission matrix spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis

Jiao Tang1,4, Jun Li1, Tao Su1,4, Yong Han2, Yangzhi Mo1, Hongxing Jiang1,4, Min Cui2, Bin Jiang1, Yingjun Chen2, Jianhui Tang3, Jianzhong Song1, Ping'an Peng1, and Gan Zhang1 Jiao Tang et al.
  • 1State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China
  • 2Department of Environmental Science and Engineering, Fudan University, Shanghai 200092, P. R. China
  • 3Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003, China
  • 4University of Chinese Academy of Sciences, Beijing 100049, China

Abstract. We investigated the fluorescence and chemical-structural characteristics of dissolved brown carbon (BrC) in smoke particulates emitted from the combustion of biomass and fossil fuels (coal and vehicle exhaust) by excitation-emission matrix (EEM) spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI). Six components were resolved by parallel factor analysis (PARAFAC) of the water-soluble and methanol-soluble organic carbon (MSOC) fractions, respectively. These fluorescent components varied among sources. Combined with FT-ICR MS ion groups, we found that the fluorescent components agreed well with the functional groups, particularly with nitrogen (N)- and sulfur (S)-containing groups. Among the six PARAFAC components (P1–6) retrieved from the water-soluble organic carbon (WSOC) fraction, except for the P3 component, the other components exhibited different values among the three types of emission sources tested. Vehicle exhaust was characterized by high P1 and P6 components, which are mainly associated with aromatic organosulfate compounds, and a high P5 component, mainly associated with sulfonates; coal combustion was characterized by a high P4 component, which is associated with nitrooxy-organosulfate (nitrooxy-OS) compounds; and biomass burning was characterized by the P2 component. Similar results were observed in the case of the MSOC fraction. This study reveals the source contribution and possible structures of previously unclear excitation-emission matrix (EEM) fluorescent components in combustion-derived aerosols. These are the first findings of this type and are potentially applicable to further studies on EEM-based source apportionment of dissolved BrC in aerosols.

Jiao Tang et al.
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Short summary
This article provides a method to identify the dissolved chromophores from simulated combustion of biomass and fossil fuel by EEM-PARAFAC. Further, the application of FT-ICR MS is expected to enable us to deduce the molecular composition of these chromophores. We identified the probable chemical structures of these independent chromophores and found that fluorescence characteristic varied from source to source, which will provide a quick and simple method for the identification of dissolved BrC.
This article provides a method to identify the dissolved chromophores from simulated combustion...
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