Revealing Brown Carbon Chromophores Produced in Reactions of Methylglyoxal with Ammonium Sulfate
Abstract
Atmospheric brown carbon (BrC) is an important contributor to light absorption and climate forcing by aerosols. Reactions between small water-soluble carbonyls and ammonia or amines have been identified as one of the potential pathways of BrC formation. However, detailed chemical characterization of BrC chromophores has been challenging and their formation mechanisms are still poorly understood. Understanding BrC formation is impeded by the lack of suitable methods which can unravel the variability and complexity of BrC mixtures. This study applies high performance liquid chromatography (HPLC) coupled to photodiode array (PDA) detector and high resolution mass spectrometry (HRMS) to investigate optical properties and chemical composition of individual BrC components produced through reactions of methylglyoxal (MG) and ammonium sulfate (AS), both of which are abundant in the atmospheric environment. A direct relationship between optical properties and chemical composition of 30 major BrC chromophores was established. Nearly all of these chromophores are nitrogen-containing compounds that account for >70% of the overall light absorption by the MG+AS system in the 300-500 nm range. These results suggest that reduced-nitrogen organic compounds formed in reactions between atmospheric carbonyls and ammonia/amines are important BrC chromophores. It is also demonstrated that improved separation of BrC chromophores by HPLC willmore »
- Authors:
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1239490
- Report Number(s):
- PNNL-SA-112156
Journal ID: ISSN 0013-936X; 48336; 47915; KP1704020
- DOE Contract Number:
- AC05-76RL01830
- Resource Type:
- Journal Article
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 49; Journal Issue: 24; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- Environmental Molecular Sciences Laboratory
Citation Formats
Lin, Peng, Laskin, Julia, Nizkorodov, Sergey A., and Laskin, Alexander. Revealing Brown Carbon Chromophores Produced in Reactions of Methylglyoxal with Ammonium Sulfate. United States: N. p., 2015.
Web. doi:10.1021/acs.est.5b03608.
Lin, Peng, Laskin, Julia, Nizkorodov, Sergey A., & Laskin, Alexander. Revealing Brown Carbon Chromophores Produced in Reactions of Methylglyoxal with Ammonium Sulfate. United States. https://doi.org/10.1021/acs.est.5b03608
Lin, Peng, Laskin, Julia, Nizkorodov, Sergey A., and Laskin, Alexander. 2015.
"Revealing Brown Carbon Chromophores Produced in Reactions of Methylglyoxal with Ammonium Sulfate". United States. https://doi.org/10.1021/acs.est.5b03608.
@article{osti_1239490,
title = {Revealing Brown Carbon Chromophores Produced in Reactions of Methylglyoxal with Ammonium Sulfate},
author = {Lin, Peng and Laskin, Julia and Nizkorodov, Sergey A. and Laskin, Alexander},
abstractNote = {Atmospheric brown carbon (BrC) is an important contributor to light absorption and climate forcing by aerosols. Reactions between small water-soluble carbonyls and ammonia or amines have been identified as one of the potential pathways of BrC formation. However, detailed chemical characterization of BrC chromophores has been challenging and their formation mechanisms are still poorly understood. Understanding BrC formation is impeded by the lack of suitable methods which can unravel the variability and complexity of BrC mixtures. This study applies high performance liquid chromatography (HPLC) coupled to photodiode array (PDA) detector and high resolution mass spectrometry (HRMS) to investigate optical properties and chemical composition of individual BrC components produced through reactions of methylglyoxal (MG) and ammonium sulfate (AS), both of which are abundant in the atmospheric environment. A direct relationship between optical properties and chemical composition of 30 major BrC chromophores was established. Nearly all of these chromophores are nitrogen-containing compounds that account for >70% of the overall light absorption by the MG+AS system in the 300-500 nm range. These results suggest that reduced-nitrogen organic compounds formed in reactions between atmospheric carbonyls and ammonia/amines are important BrC chromophores. It is also demonstrated that improved separation of BrC chromophores by HPLC will significantly advance understanding of BrC chemistry.},
doi = {10.1021/acs.est.5b03608},
url = {https://www.osti.gov/biblio/1239490},
journal = {Environmental Science and Technology},
issn = {0013-936X},
number = 24,
volume = 49,
place = {United States},
year = {Tue Dec 15 00:00:00 EST 2015},
month = {Tue Dec 15 00:00:00 EST 2015}
}