Molecular Composition of Beijing PM2.5 Brown Carbon Revealed by an Untargeted Approach Based on Gas Chromatography and Time-of-Flight Mass Spectrometry.

ABSTRACT

The knowledge of the chemical composition of brown carbon (BrC) is limited to the categories of components or parts of specific organic components. In this paper, the light-absorbing properties and molecular compositions of lipid-soluble organic components in fine particulate matter of Beijing from 2016 to 2018, characterized by an ultraviolet-visible spectrometer and gas chromatography coupled with time-of-flight mass spectrometry, respectively, were combined to untargetedly screen the key BrC molecules by a partial least squares regression model for the first time. A total of 421 molecules were obtained, where 61 molecules were identified qualitatively and 22 molecules quantitatively. To the best of our knowledge, 11 molecules were newly identified BrC species. These qualitative molecules included polycyclic aromatic hydrocarbons with higher ambient concentrations and mass absorbing efficiencies (MAEs), as well as oxygen- and nitrogen-containing aromatic components with relatively lower concentrations and MAEs. The absorption contribution at 365 nm of quantified BrC species to lipid-soluble BrC during heating seasons was 39.1 ± 17.0%, which was about 5 times as high as previous studies. These results help establish a complete BrC molecular database and provide data support for better evaluating the climate effect of atmospheric carbonaceous aerosols and formulating air pollution control strategies.