Characterization of Chromophoric Water-Soluble Organic Matter in Urban, Forest, and Marine Aerosols by HR-ToF-AMS Analysis and Excitation–Emission Matrix Spectroscopy

Chen, Qingcai; Miyazaki, Y.; Kawamura, Kimitaka; Matsumoto, Kiyoshi; Coburn, S.; Volkamer, Rainer; Iwamoto, Yoko; Kagami, Sara; Deng, Yange; Ogawa, Shuichi; Ramasamy, Sathiyamurthi; Kato, S.; Ida, Akira; Kajii, Yoshizumi; Mochida, Michihiro

doi:10.1021/acs.est.6b01643

Cited by 165 publications

(206 citation statements)

References 67 publications

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“…They also reported an anticorrelation between Chl a and OM fraction in their model. Contributions of proteins to the submicron WSOC in the same samples are discussed in Chen et al (2016) using excitation-emission matrices.…”

Section: Monosaccharides Fatty Acids and Msa As Marine Biogenic Tramentioning

confidence: 99%

Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

et al. 2016

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Abstract. Stable carbon isotopic compositions of watersoluble organic carbon (WSOC) and organic molecular markers were measured to investigate the relative contributions of the sea surface sources to the water-soluble fraction of submicron organic aerosols collected over the eastern equatorial Pacific during the Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOCs (TORERO)/KA-12-01 cruise. On average, the watersoluble organic fraction of the total carbon (TC) mass in submicron aerosols was ∼ 30-35 % in the oceans with the low chlorophyll a (Chl a) concentrations, whereas it was ∼ 60 % in the high-Chl a regions. The average stable carbon isotope ratio of WSOC (δ 13 C WSOC ) was −19.8 ± 2.0 ‰, which was systematically higher than that of TC (δ 13 C TC ) (−21.8 ± 1.4 ‰). We found that in the oceans with both high and low Chl a concentrations the δ 13 C WSOC was close to the typical values of δ 13 C for dissolved organic carbon (DOC), ranging from −22 to −20 ‰ in surface seawater of the tropical Pacific Ocean. This suggests an enrichment of marine biological products in WSOC aerosols in the study region regardless of the oceanic area. In particular, enhanced levels of WSOC and biogenic organic marker compounds together with high values of WSOC / TC (∼ 60 %) and δ 13 C WSOC were observed over upwelling areas and phytoplankton blooms, which was attributed to planktonic tissues being more enriched in δ 13 C. The δ 13 C analysis estimated that, on average, marine sources contribute ∼ 90 ± 25 % of the aerosol carbon, indicating the predominance of marine-derived carbon in the submicron WSOC. This conclusion is supported by Lagrangian trajectory analysis, which suggests that the majority of the sampling points on the ship had been exposed to marine boundary layer (MBL) air for more than 80 % of the time during the previous 7 days. The combined analysis of the δ 13 C and monosaccharides, such as glucose and fructose, demonstrated that DOC concentration was closely correlated with the concentration levels of submicron WSOC across the study region regardless of the oceanic area. The result implies that DOC may characterize background organic aerosols in the MBL over the study region.

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Section: Monosaccharides Fatty Acids and Msa As Marine Biogenic Tramentioning

confidence: 99%

Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

et al. 2016

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“…The three-dimensional excitation-emission matrix (EEM) method can separate chromophores into several categories according to excitation-emission wavelengths for chromophores that may not be distinguishable by UV-visible absorption spectroscopy (Chen, Miyazaki, et al, 2016and Chen, Ikemori, & Mochida, 2016. Although the EEM method has more difficulty identifying individual molecules than liquid chromatography-mass spectrometry, the EEM method can easily classify compounds with similar optical characteristics, each of which may represent similar chemical structures and photochemical features, and the types and relative contents of chromophores may be used to trace the sources of the chromophores (Chen, Miyazaki, et al, 2016;Yan & Kim, 2017).…”

Section: Introductionmentioning

confidence: 99%

Size‐Resolved Characterization of the Chromophores in Atmospheric Particulate Matter From a Typical Coal‐Burning City in China

Chen

Song

et al. 2019

JGR Atmospheres

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This study reports the size‐resolved characterization of the chromophores in atmospheric particulate matter in Linfen, a typical coal‐burning city in China. The optical properties of both the water‐soluble and water‐insoluble chromophores in atmospheric particulates are studied using excitation‐emission matrix spectroscopy and follow the parallel factor analysis of excitation‐emission matrix data. The mass absorption efficiency and normalized fluorescence volume by mass concentration of the organic carbon in methanol‐soluble matter in the particulate samples are stronger than that of the water‐soluble matter. We found that the total absorption (Abs), fluorescence volume (FV), mass absorption efficiency, and normalized fluorescence volume of particle extracts with sizes less than 10 μm increased with the decreasing particle size. The total concentration of the selected seven polycyclic aromatic hydrocarbons was positively correlated with the Abs365 and FV of both the water‐soluble matter and methanol‐soluble matter, but the average contribution of the selected polycyclic aromatic hydrocarbons to the total Abs and FV was very small (<3%). This study is the first to report a size‐resolved characterization of the chromophores in atmospheric particulate matter. Humic‐like substances tend to be present in small particles, and tryptophan‐like and tyrosine‐like components tend to increase with increasing particle size.

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“…haze events in China , as well as AMS measurements of coarse-mode aerosol and long-term source apportionment studies (Bozzetti, 2017a, b). Such an approach was also used in recent studies for identifying the different types of water-soluble chromophores (Chen et al, 2016). Additionally, such filters are routinely collected and are already available over multi-year periods at many air quality monitoring stations around the world for years and/or decades.…”

Section: Introductionmentioning

confidence: 99%

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

et al. 2017

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Abstract. Long-term monitoring of organic aerosol is important for epidemiological studies, validation of atmospheric models, and air quality management. In this study, we apply a recently developed filter-based offline methodology using an aerosol mass spectrometer (AMS) to investigate the regional and seasonal differences of contributing organic aerosol sources. We present offline AMS measurements for particulate matter smaller than 10 µm at nine stations in central Europe with different exposure characteristics for the entire year of 2013 (819 samples). The focus of this study is a detailed source apportionment analysis (using positive matrix factorization, PMF) including in-depth assessment of the related uncertainties. Primary organic aerosol (POA) is separated in three components: hydrocarbon-like OA related to traffic emissions (HOA), cooking OA (COA), and biomass burning OA (BBOA). We observe enhanced production of secondary organic aerosol (SOA) in summer, following the increase in biogenic emissions with temperature (summer oxygenated OA, SOOA). In addition, a SOA component was extracted that correlated with an anthropogenic secondary inorganic species that is dominant in winter (winter oxygenated OA, WOOA). A factor (sulfur-containing organic, SC-OA) explaining sulfur-containing fragments (CH 3 SO + 2 ), which has an event-driven temporal behaviour, was also identified. The relative yearly average factor contributions range from 4 to 14 % for HOA, from 3 to 11 % for COA, from 11 to 59 % for BBOA, from 5 to 23 % for SC-OA, from 14 to 27 % for WOOA, and from 15 to 38 % for SOOA. The uncertainty of the relative average factor contribution lies between 2 and 12 % of OA. At the sites north of the alpine crest, the sum of HOA, COA, and BBOA (POA) contributes less to OA (POA / OA = 0.3) than at the southern alpine valley sites (0.6). BBOA is the main contributor to POA with 87 % in alpine valleys and 42 % north of the alpine crest. Furthermore, the influence of primary biological particles (PBOAs), not resolved by PMF, is estimated and could contribute significantly to OA in PM 10 .

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Characterization of Chromophoric Water-Soluble Organic Matter in Urban, Forest, and Marine Aerosols by HR-ToF-AMS Analysis and Excitation–Emission Matrix Spectroscopy

Cited by 165 publications

References 67 publications

Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

Size‐Resolved Characterization of the Chromophores in Atmospheric Particulate Matter From a Typical Coal‐Burning City in China

Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment

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