气候变化领域集成服务门户(CCPortal): Chromophores and chemical composition of brown carbon characterized at anurban kerbside by excitation-emission spectroscopy and mass spectrometry

CCPortal

DOI	10.5194/acp-22-14971-2022
	Chromophores and chemical composition of brown carbon characterized at anurban kerbside by excitation-emission spectroscopy and mass spectrometry
	Jiang, Feng; Song, Junwei; Bauer, Jonas; Gao, Linyu; Vallon, Magdalena; Gebhardt, Reiner; Leisner, Thomas; Norra, Stefan; Saathoff, Harald
发表日期	2022
ISSN	1680-7316
EISSN	1680-7324
起始页码	14971
结束页码	14986
卷号	22 期号:22 页码:16
英文摘要	The optical properties, chemical composition, and potential chromophores of brown carbon (BrC) aerosol particles were studied during typical summertime and wintertime at a kerbside in downtown Karl-sruhe, a city in central Europe. The average absorption coefficient and mass absorption efficiency at 365 nm (Abs(365) and MAE(365)) of methanol-soluble BrC (MS-BrC) were lower in the summer period (1.6 +/- 0.5 Mm(-1), 0.5 +/- 0.2 m(2) g(-1)) than in the winter period (2.8 +/- 1.9 Mm(-1), 1.1 +/- 0.3 m(2) g(-1)). Using a parallel factor (PARAFAC) analysis to identify chromophores, two different groups of highly oxygenated humic-like substances (HO-HULIS) dominated in summer and contributed 96 +/- 6 % of the total fluorescence intensity. In contrast, less-oxygenated HULIS (LO-HULIS) dominated the total fluorescence intensity in winter with 57 +/- 12 %, followed by HO-HULIS with 31 +/- 18 %. Positive matrix factorization (PMF) analysis of organic compounds detected in real time by an online aerosol mass spectrometer (AMS) led to five characteristic organic compound classes. The statistical analysis of PARAFAC components and PMF factors showed that LO-HULIS chromophores were most likely emitted from biomass burning in winter. HO-HULIS chromophores could be low-volatility oxy-genated organic aerosol from regional transport and oxidation of biogenic volatile organic compounds (VOCs) in summer. Five nitro-aromatic compounds (NACs) were identified by a chemical ionization mass spectrometer (C7H7O3N, C7H7O4N, C6H5O5N, C6H5O4N, and C6H5O3N), which contributed 0.03 +/- 0.01 % to the total organic mass but can explain 0.3 +/- 0.1 % of the total absorption of MS-BrC at 365 nm in winter. Furthermore, we identified 316 potential brown carbon molecules which accounted for 2.5 +/- 0.6 % of the organic aerosol mass. Using an average mass absorption efficiency (MAE(365)) of 9.5 m(2)g(-1) for these compounds, we can es-timate their mean light absorption to be 1.2 +/- 0.2 Mm(-1), accounting for 32 +/- 15 % of the total absorption of MS-BrC at 365 nm. This indicates that a small fraction of brown carbon molecules dominates the overall ab-sorption. The potential BrC molecules assigned to the LO-HULIS component had a higher average molecular weight (265 +/- 2 Da) and more nitrogen-containing molecules (62 +/- 1 %) than the molecules assigned to the HOHULIS components. Our analysis shows that the LO-HULIS, with a high contribution of nitrogen-containing molecules originating from biomass burning, dominates aerosol fluorescence in winter, and HO-HULIS, with fewer nitrogen-containing molecules as low-volatility oxygenated organic aerosol from regional transport and oxidation of biogenic volatile organic compounds (VOC), dominates in summer.
学科领域	Environmental Sciences; Meteorology & Atmospheric Sciences
语种	英语
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号	WOS:000890189300001
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/273140
作者单位	Helmholtz Association; Karlsruhe Institute of Technology; Helmholtz Association; Karlsruhe Institute of Technology; Helmholtz Association; Karlsruhe Institute of Technology; Ruprecht Karls University Heidelberg; University of Potsdam
推荐引用方式 GB/T 7714	Jiang, Feng,Song, Junwei,Bauer, Jonas,et al. Chromophores and chemical composition of brown carbon characterized at anurban kerbside by excitation-emission spectroscopy and mass spectrometry[J],2022,22(22):16.
APA	Jiang, Feng.,Song, Junwei.,Bauer, Jonas.,Gao, Linyu.,Vallon, Magdalena.,...&Saathoff, Harald.(2022).Chromophores and chemical composition of brown carbon characterized at anurban kerbside by excitation-emission spectroscopy and mass spectrometry.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(22),16.
MLA	Jiang, Feng,et al."Chromophores and chemical composition of brown carbon characterized at anurban kerbside by excitation-emission spectroscopy and mass spectrometry".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.22(2022):16.