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Co-photolysis of mixed chromophores affects atmospheric lifetimes of brown carbon
Yalin Wang1; Tian Qiu1; Cong Zhang1; Tianwei Hao1; Beatrix Rosette Go Mabato2; Ruifeng Zhang2; Masao Gen3; Man Nin Chan4; Dan Dan Huang5; Xinlei Ge6; Junfeng Wang6; Lin Du7; Ru-Jin Huang8; Qi Chen9; Ka In Hoi1; Kai Meng Mok1; Chak K. Chan2,10; Yong Jie Li1
2023-08
Source PublicationEnvironmental Science: Atmospheres
ISSN2634-3606
Volume3Issue:8Pages:1127–1244
Abstract

Brown carbon (BrC) affects radiation budget and thus global climate by absorbing light, during which photolysis can also occur and serve as an important sink of BrC. Yet, the interactive roles of mixed chromophores during BrC co-photolysis, which is anticipated in ambient aerosol particles, is seldom explored, making a model representation of atmospheric lifetimes of BrC highly uncertain. Herein, we investigate the photolysis of four typical atmospheric BrC chromophores (two methoxyphenols, MPs, and two nitrophenols, NPs), alone or mixed, with a wide range of concentrations as anticipated in atmospheric cloud/fog and aerosol droplets. The photo-decay rate constants (k) for the photolysis of single chromophores generally decrease as BrC concentration increases, but the effective quantum yields (Fe) are relatively constant in optically thin solutions; the Fe values increase by one order of magnitude in optically thick solutions for most BrC chromophores studied and even exceed 1 when BrC concentrations are high (e.g., 500 mM in isopropanol solutions), presumably due to secondary reactions involving their triplet states. During co-photolysis of two mixed chromophores, MPs increase the Fe values of NPs by factors of 4–26, but NPs affect the Fe values of MPs insignificantly, indicating a stronger sensitizing effect of MPs than NPs. In contrast, NPs mainly exert a shadowing effect on MP degradation, which only affects photo-decay rate constant but not effective quantum yield and is negligible for fine particles. Estimation of atmospheric lifetimes suggests that sensitizing by MPs can accelerate NP degradation by a factor of up to 30 while shadowing between them plays minor roles in fine particles but non-negligibly in coarse particles.

DOI10.1039/d3ea00073g
Indexed ByESCI
WOS Research AreaEnvironmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS SubjectEnvironmental Sciences ; Meteorology & Atmospheric Sciences
WOS IDWOS:001026430800001
PublisherROYAL SOC CHEMISTRYTHOMAS GRAHAM HOUSE, SCIENCE PARK, MILTON RD, CAMBRIDGE CB4 0WF, CAMBS, ENGLAND
Scopus ID2-s2.0-85166301818
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Citation statistics
Document TypeJournal article
CollectionDEPARTMENT OF OCEAN SCIENCE AND TECHNOLOGY
Faculty of Science and Technology
DEPARTMENT OF CIVIL AND ENVIRONMENTAL ENGINEERING
Corresponding AuthorYong Jie Li
Affiliation1.Department of Civil and Environmental Engineering, Department of Ocean Science and Technology, Centre for Regional Oceans, Faculty of Science and Technology, University of Macau, Macau 999078, China
2.School of Energy and Environment, City University of Hong Kong, Hong Kong 999077, China
3.Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1, Katahira, Sendai, Miyagi 980-8577, Japan
4.Earth System Science Programme, Faculty of Science, Institute of Environment, Energy, and Sustainability, The Chinese University of Hong Kong, Hong Kong 999077, China
5.Shanghai Academy of Environmental Sciences, Shanghai 200233, China
6.Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control (AEMPC), School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, Nanjing 210044, China
7.Environment Research Institute, Shandong University, Shanda South Road 27, Shandong 250100, China
8.State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an 710061, China
9.State Key Joint Laboratory of Environmental Simulation and Pollution Control, BIC-ESAT, IJRC, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
10.Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Kingdom of Saudi Arabia
First Author AffilicationFaculty of Science and Technology
Corresponding Author AffilicationFaculty of Science and Technology
Recommended Citation
GB/T 7714
Yalin Wang,Tian Qiu,Cong Zhang,et al. Co-photolysis of mixed chromophores affects atmospheric lifetimes of brown carbon[J]. Environmental Science: Atmospheres, 2023, 3(8), 1127–1244.
APA Yalin Wang., Tian Qiu., Cong Zhang., Tianwei Hao., Beatrix Rosette Go Mabato., Ruifeng Zhang., Masao Gen., Man Nin Chan., Dan Dan Huang., Xinlei Ge., Junfeng Wang., Lin Du., Ru-Jin Huang., Qi Chen., Ka In Hoi., Kai Meng Mok., Chak K. Chan., & Yong Jie Li (2023). Co-photolysis of mixed chromophores affects atmospheric lifetimes of brown carbon. Environmental Science: Atmospheres, 3(8), 1127–1244.
MLA Yalin Wang,et al."Co-photolysis of mixed chromophores affects atmospheric lifetimes of brown carbon".Environmental Science: Atmospheres 3.8(2023):1127–1244.
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