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Formation and optical properties of brown carbon from small α-dicarbonyls and amines

Marrero-Ortiz, Wilmarie and Hu, Min and Du, Zhuofei and Ji, Yuemeng and Wang, Yujue and Guo, Song and Lin, Yun and Gomez-Hermandez, Mario and Peng, Jianfei and Li, Yixin and Secrest, Jeremiah and Zamora, Misti L. and Wang, Yuan and An, Taicheng and Zhang, Renyi (2019) Formation and optical properties of brown carbon from small α-dicarbonyls and amines. Environmental Science and Technology, 53 (1). pp. 117-126. ISSN 0013-936X. https://resolver.caltech.edu/CaltechAUTHORS:20181130-095502623

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Abstract

Brown Carbon (BrC) aerosols scatter and absorb solar radiation, directly affecting the Earth’s radiative budget. However, considerable uncertainty exists concerning the chemical mechanism leading to BrC formation and their optical properties. In this work, BrC particles were prepared from mixtures of small α-dicarbonyls (glyoxal and methylglyoxal) and amines (methylamine, dimethylamine, and trimethylamine). The absorption and scattering of BrC particles were measured using a photoacoustic extinctometer (405 and 532 nm), and the chemical composition of the α-dicarbonyl-amine mixtures was analyzed using orbitrap-mass spectrometry and thermal desorption-ion drift-chemical ionization mass spectrometry. The single scattering albedo for methylglyoxal-amine mixtures is smaller than that of glyoxal-amine mixtures and increases with the methyl substitution of amines. The mass absorption cross-section for methylglyoxal-amine mixtures is two times higher at 405 nm wavelength than that at 532 nm wavelength. The derived refractive indexes at the 405 nm wavelength are 1.40–1.64 for the real part and 0.002–0.195 for the imaginary part. Composition analysis in the α-dicarbonyl-amine mixtures reveals N-heterocycles as the dominant products, which are formed via multiple steps involving nucleophilic attack, steric hindrance, and dipole–dipole interaction between α-dicarbonyls and amines. BrC aerosols, if formed from the particle-phase reaction of methylglyoxal with methylamine, likely contribute to atmospheric warming.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.est.8b03995DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/acs.est.8b03995PublisherSupporting Information
ORCID:
AuthorORCID
Wang, Yujue0000-0003-4563-9214
Wang, Yuan0000-0001-6657-8401
An, Taicheng0000-0001-6918-8070
Additional Information:© 2018 American Chemical Society. Received: July 20, 2018; Revised: November 28, 2018; Accepted: November 30, 2018; Published: November 30, 2018. This research was supported by National Natural Science Foundation of China (91544214, 41421064, 41675122, 41373102, 21577177, and 41425015), the Robert A. Welch Foundation (A-1417), National Key Research and Development Program of China (2016YFC0202000: Task 3), Science and Technology Program of Guangzhou City (201707010188), and Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01Z032). W.M.-O. was supported by the National Science Foundation Graduate Research Fellowship Program. Helpful discussion with Dr. Sasha Mandronich of the National Center for Atmospheric Research was appreciated.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China91544214
National Natural Science Foundation of China41421064
National Natural Science Foundation of China41675122
National Natural Science Foundation of China41373102
National Natural Science Foundation of China21577177
National Natural Science Foundation of China41425015
Robert A. Welch FoundationA-1417
National Key Research and Development Program of China2016YFC0202000
Guangzhou City201707010188
Guangdong Pearl River Talents Program2017BT01Z032
NSF Graduate Research FellowshipUNSPECIFIED
Issue or Number:1
Record Number:CaltechAUTHORS:20181130-095502623
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20181130-095502623
Official Citation:Formation and Optical Properties of Brown Carbon from Small α-Dicarbonyls and Amines. Wilmarie Marrero-Ortiz, Min Hu, Zhuofei Du, Yuemeng Ji, Yujue Wang, Song Guo, Yun Lin, Mario Gomez-Hermandez, Jianfei Peng, Yixin Li, Jeremiah Secrest, Misti L. Zamora, Yuan Wang, Taicheng An, and Renyi Zhang. Environmental Science & Technology 2019 53 (1), 117-126 DOI: 10.1021/acs.est.8b03995
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:91358
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:30 Nov 2018 18:28
Last Modified:03 Oct 2019 20:34

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