4.7 Article

Measurement report: Long-emission-wavelength chromophores dominate the light absorption of brown carbon in aerosols over Bangkok: impact from biomass burning

期刊

ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 21, 期 14, 页码 11337-11352

出版社

COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-21-11337-2021

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资金

  1. National Natural Science Foundation of China [42030715, 41430645, 41773120]
  2. International Partnership Program of Chinese Academy of Sciences [132744KYSB20170002]
  3. Guangdong Foundation for Program of Science and Technology Research [2017BT01Z134, 2018A030310022, 2019B121205006, 2020B1212060053]
  4. China Postdoctoral Science Foundation [2020M682937]

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The study found that the emission wavelength of fluorescent chromophores in environmental samples tended to increase compared with that of primary combustion emissions, possibly due to secondary formation or aging processes. Fluorescent indices revealed that the light-absorbing chromophores were not significantly humified and consisted of a mixture of organic matter from terrestrial and microbial sources, exhibiting different characteristics from primary biomass burning and coal combustion results. A multiple linear regression analysis showed that larger fluorescent chromophores that were oxygen-rich and highly aromatic with high molecular weights were the key contributors to light absorption, particularly at longer emission wavelengths (lambda(max) > 500 nm). Positive matrix factorization analysis also indicated that up to 50% of these light-absorbing chromophores originated from biomass burning emissions.
Chromophores represent an important portion of light-absorbing species, i.e., brown carbon. Yet knowledge of what and how chromophores contribute to aerosol light absorption is still sparse. To address this problem, we examined soluble independent chromophores in a set of year-round aerosol samples from Bangkok. The water-soluble fluorescent chromophores identified via excitation-emission matrix (EEM) spectroscopy and follow-up parallel factor analysis could be mainly assigned as humic-like substances and protein-like substances, which differed in their EEM pattern from that of the methanol-soluble fraction. The emission wavelength of fluorescent chromophores in environmental samples tended to increase compared with that of the primary combustion emission, which could be attributed to secondary formation or the aging process. Fluorescent indices inferred that these light-absorbing chromophores were not significantly humified and comprised a mixture of organic matter of terrestrial and microbial origin, which exhibited a different characteristic from primary biomass burning and coal-combustion results. A multiple linear regression analysis revealed that larger fluorescent chromophores that were oxygen-rich and highly aromatic with high molecular weights were the key contributors of light absorption, preferably at longer emission wavelengths (lambda(max) > 500 nm). Positive matrix factorization analysis further suggested that up to 50% of these responsible chromophores originated from biomass burning emissions.

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