Molecular Absorption and Evolution Mechanisms of PM2.5 Brown Carbon Revealed by Electrospray Ionization Fourier Transform-Ion Cyclotron Resonance Mass Spectrometry During a Severe Winter Pollution Episode in Xi'an, China
Abstract
Knowledge of the molecular-level chemistry of brown carbon (BrC) is important in reducing the uncertainties in aerosol radiative forcing. Time-resolved ambient PM2.5 samples were collected during a severe pollution episode in January 2017 over Xi'an, China for a comprehensive nontarget and full scanning of BrC molecules and their absorption properties using electrospray ionization Fourier transform-ion cyclotron resonance mass spectrometry combined with partial least squares regression analysis, which apportioned the overall ultraviolet absorption to individual molecules. The estimated absorption of CHNO and CHNOS molecules exhibited nighttime prevalence, whereas CHOS, CHNS, CHN, CHO, CHS, and CH molecules presented a dynamic trend. Carbon conjugation was positively correlated with estimated absorption by CHO and CHNO molecules, while exhibiting a mixed relationship with CHNOS. Higher nitrogen content was associated with enhanced light-absorption properties of BrC molecules, while higher oxygen and sulfur content appeared to be associated with photobleaching during secondary transformation.
- Publication:
-
Geophysical Research Letters
- Pub Date:
- May 2020
- DOI:
- 10.1029/2020GL087977
- Bibcode:
- 2020GeoRL..4787977Z
- Keywords:
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- brown carbon;
- molecular absorption;
- carbon conjugation;
- N-addition;
- oxidation and sulfur addition