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Effect of Relative Humidity on Secondary Brown Carbon Formation in Aqueous Droplets
Kasthuriarachchi, Nethmi Y.1; Rivellini, Laura Hélèna2; Chen, Xi3; Li, Yong Jie3; Lee, Alex K.Y.1,2
2020-10-20
Source PublicationEnvironmental Science and Technology
ABS Journal Level3
ISSN0013-936X
Volume54Issue:20Pages:13207-13216
Abstract

Atmospheric brown carbon (BrC) is a significant contributor to particulate light absorption. Reactions between small aldehydes and reduced nitrogen species have been shown to produce secondary BrC in atmospheric droplets. These reactions can be substantially accelerated upon droplet evaporation. Despite aqueous droplets undergoing continuous water evaporation and uptake in response to the surrounding relative humidity (RH), secondary BrC formation in these droplets under various RH conditions remains poorly understood. In this work, we investigate BrC formation from reactions of two aqueous-phase precursors, glyoxal and methylglyoxal, with ammonium sulfate or glycine in aqueous droplets after drying at a range of RH (30-90%). Our results illustrate, for the first time, that BrC production varies as a function of RH. For all four chemical reaction systems being investigated, mass absorption efficiencies (MAE, m2/g C) of aqueous aerosol products (from 270 to 512 nm wavelength range) generally increase with reducing RH to reach a maximum at ∼55-65% RH and subsequently decrease, caused by further drying. Chemical characterization using high-resolution aerosol mass spectrometry shows that the formation of nitrogen-containing organic species also follows a similar variation with RH. Our observations reveal that the acceleration of BrC production from evaporation of water may be diminished by other factors, such as limited particle-phase water content, phase transition, and volatility of reactants and products. Overall, our results highlight that intermediate RH conditions in the atmosphere may be more efficient in secondary BrC formation, indicating that the effect of RH needs to be included in atmospheric models for a more accurate representation of light-absorbing aerosol formation in aqueous droplets.

DOI10.1021/acs.est.0c01239
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaEngineering ; Environmental Sciences & Ecology
WOS SubjectEngineering ; Environmental Sciences & Ecology
WOS IDWOS:000584422500042
Scopus ID2-s2.0-85093885024
Fulltext Access
FWCI0.93518496
Citation statistics
Document TypeJournal article
CollectionDEPARTMENT OF CIVIL AND ENVIRONMENTAL ENGINEERING
Corresponding AuthorLee, Alex K.Y.
Affiliation1.Department of Civil and Environmental Engineering, National University of Singapore, Singapore, 117576, Singapore
2.Nus Environmental Research Institute, National University of Singapore, Singapore, 117411, Singapore
3.Department of Civil and Environmental Engineering, Faculty of Science and Technology, University of Macau, Macao
Recommended Citation
GB/T 7714
Kasthuriarachchi, Nethmi Y.,Rivellini, Laura Hélèna,Chen, Xi,et al. Effect of Relative Humidity on Secondary Brown Carbon Formation in Aqueous Droplets[J]. Environmental Science and Technology,2020,54(20):13207-13216.
APA Kasthuriarachchi, Nethmi Y.,Rivellini, Laura Hélèna,Chen, Xi,Li, Yong Jie,&Lee, Alex K.Y..(2020).Effect of Relative Humidity on Secondary Brown Carbon Formation in Aqueous Droplets.Environmental Science and Technology,54(20),13207-13216.
MLA Kasthuriarachchi, Nethmi Y.,et al."Effect of Relative Humidity on Secondary Brown Carbon Formation in Aqueous Droplets".Environmental Science and Technology 54.20(2020):13207-13216.
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