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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 14 Nov 2019

Submitted as: research article | 14 Nov 2019

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This preprint is currently under review for the journal ACP.

The evolutionary behavior of chromophoric brown carbon during ozone aging of fine particles from biomass burning

Xingjun Fan1,3, Tao Cao2,4, Xufang Yu1, Yan Wang1, Xin Xiao1, Feiyue Li1,3, Yue Xie1, Wenchao Ji1, Jianzhong Song2, and Ping'an Peng2 Xingjun Fan et al.
  • 1College of Resource and Environment, Anhui Science and Technology University, Fengyang 233100, P. R. China
  • 2State Key Laboratory of Organic Geochemistry, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, P. R. China
  • 3Anhui Province Key Laboratory of Biochar and Cropland Pollution Prevention, Bengbu 233400, P. R. China
  • 4University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Abstract. Biomass burning (BB) emits large amounts of brown carbon (BrC), however, little is known about the evolutionary behavior of BrC produced by BB (BB-BrC) in atmospheric processes. In this study, the transformation of levels and the chromophoric characteristics of BrC in smoke particles emitted by the burning of rice straw (RS), corn straw (CS) and pine wood (PW) under O3 aging are investigated. The O3 aging induced the reduction of light absorption and fluorescence for the BB-BrC, suggesting the decomposition of chromophores and fluorophores. These changes were accompanied by a decrease of aromaticity, average molecular weight and the light absorption capacity for the chromophores, and an increase of humification for the fluorophores. The excitation emission matrix combined with a parallel factor analysis revealed that protein-like components (C3) were predominantly decomposed by O3 aging, while the relative distribution of a humic-like component with highly oxygenated chromophores (C4) gradually increased. In general, the humic-like substances (C1+C2+C4) were transformed to be the most abundant fluorophores for all the BB-BrC samples, which accounted for 84 %–87 % of the total fluorophores in final O3-aged BB-BrC. Two dimensional correlation spectroscopy (2D-COS) was performed on the synchronous fluorescence, which suggested that the RS- and CS- BrC exhibits the same susceptible fluorophores changes upon O3 aging. It showed that O3 firstly reacted with protein-like fractions (263–289 nm), and then with fulvic-like fractions (333–340 nm). In comparison, the changing sequence of susceptible fluorophores in the PW-BrC to O3 were in the order of fulvic-like with shorter wavelengths (309 nm) > protein-like fluorophores (276 nm) > fulvic-like fluorophores with longer wavelengths (358 nm). The 2D-FTIR-COS analysis showed conjugated C=O and aromatic C=C and C=O groups were the most susceptible functional groups to O3 aging for all BB-BrC. Moreover, it also revealed a consistent sequential changes, which is in the order of aromatic OH, conjugated C=O groups and aromatic C=O, aromatic COO, and finally lignin-derived C-C, C-H and C-O groups. Our results provide new insights into the evolutionary behavior of the chromophoric and fluorescent properties of BB-BrC during O3 aging. They have important implications for the heterogeneous oxidation of BB emission to form BrC, and are of great significance for improving the accuracy of climate models and source apportionment models parameterized by the optical properties of BrC.

Xingjun Fan et al.

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Xingjun Fan et al.

Xingjun Fan et al.


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Short summary
A particle-phase O3 oxidation of biomass burning (BB) smoke particles was conducted to investigate the evolution of brown carbon (BrC) therein. The O3 aging induced the decomposition of chromophores and fluorophores. EEM-PARAFAC showed a predominant decomposition of protein-like substances, and a gradual increase proportion of humic-like substances for BB-BrC during O3 aging. The dynamic spectral behaviors of chromophores and functional groups within BrC were further explored by 2D-COS.
A particle-phase O3 oxidation of biomass burning (BB) smoke particles was conducted to...