Molecular Characterization of Water- and Methanol-Soluble Organic Compounds Emitted from Residential Coal Combustion Using Ultrahigh-Resolution Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Song, Jianzhong; Li, Meiju; Fan, Xingjun; Zou, Chunlin; Zhu, Mengbo; Jiang, Bin; Yu, Zhiqiang; Jia, Wanglu; Liao, Yuhong; Peng, Ping’an

doi:10.1021/acs.est.9b04331

Cited by 89 publications

(105 citation statements)

References 77 publications

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“…A red shift in the excitation-emission maximum could indicate increased aromaticity and higher molecular weight (Ghidotti et al, 2017). Field observations have demonstrated that chromophore components were associated with chemical structures (Chen et al, 2016a, b;Stubbins et al, 2014). Chen et al (2016b) illustrated that the fluorescent components of HULIS-1 and HULIS-2 were correlated positively with CO + and CO + 2 and C x H + y and C x H y O + 1 groups ions, respectively, using the correlation analysis of the relative intensities of ion groups in high-resolution aerosol mass spectrometers (HR-AMSs) and the relative content of fluo- rescence components.…”

Section: Link Of Molecular Compositions and Optical Propertiesmentioning

confidence: 99%

“…With the advantage of ultrahigh resolution, the accuracy of mass measurements, and high sensitivity (Feng et al, 2016), FT-ICR MS has been successfully used to characterize organic aerosols (Jiang et al, 2016;Song et al, 2018;Mo et al, 2018), cloud water (Zhao et al, 2013), and natural organic matter (Sleighter et al, 2012;Feng et al, 2016). For example, a previous study has determined their molecular families of dissolved organic matter (DOM) associated with fluorescent components by using FT-ICR MS (Stubbins et al, 2014), which could provide more chemical information about chromophores.…”

Section: Introductionmentioning

confidence: 99%

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Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

et al. 2020

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Abstract. Brown carbon (BrC) plays an essential impact on radiative forcing due to its ability to absorb sunlight. In this study, the optical properties and molecular characteristics of water-soluble and methanol-soluble organic carbon (OC; MSOC) emitted from the simulated combustion of biomass and coal fuels and vehicle emissions were investigated using ultraviolet–visible (UV–vis) spectroscopy, excitation–emission matrix (EEM) spectroscopy, and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI). The results showed that these smoke aerosol samples from biomass burning (BB) and coal combustion (CC) had a higher mass absorption efficiency at 365 nm (MAE365) than vehicle emission samples. A stronger MAE365 value was also found in MSOC than water-soluble organic carbon (WSOC), indicating low polar compounds would possess a higher light absorption capacity. Parallel factor (PARAFAC) analysis identified six types of fluorophores (P1–6) in WSOC including two humic-like substances (HULIS-1) (P1 and P6), three protein-like substances (PLOM) (P2, P3, and P5), and one undefined substance (P4). HULIS-1 was mainly from aging vehicle exhaust particles; P2 was only abundant in BB aerosols; P3 was ubiquitous in all tested aerosols; P4 was abundant in fossil burning aerosols; and P5 was more intense in fresh vehicle exhaust particles. The MSOC chromophores (six components; C1–6) exhibited consistent characteristics with WSOC, suggesting the method could be used to indicate the origins of chromophores. FT-ICR mass spectra showed that CHO and CHON were the most abundant components of WSOC, but S-containing compounds appeared in a higher abundance in CC aerosols and vehicle emissions than BB aerosols, while considerably fewer S-containing compounds largely with CHO and CHON were detected in MSOC. The unique formulas of different sources in the van Krevelen (VK) diagram presented different molecular distributions. To be specific, BB aerosols with largely CHO and CHON had a medium H ∕ C and low O ∕ C ratio, while CC aerosols and vehicle emissions largely with S-containing compounds had an opposite H ∕ C and O ∕ C ratio. Moreover, the light absorption capacity of WSOC and MSOC was positively associated with the unsaturation degree and molecular weight in the source aerosols. The above results are potentially applicable to further studies on the EEM-based or molecular-characteristic-based source apportionment of chromophores in atmospheric aerosols.

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Section: Link Of Molecular Compositions and Optical Propertiesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

et al. 2020

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“…EEM analysis enables the probing of the chemical structure of DOM because of its ability to distinguish among different classes of organic matter (Wu et al, 2003). Generally, BrC absorption is related to the chromophores within it and is susceptible to change with variations in chemical properties, e.g., oxidation level (Mo et al, 2018), degree of unsaturation (Jiang et al, 2020), molecular weight (Tang et al, 2020b;Di Lorenzo et al, 2017), functional groups (Chen et al, 2017b), molecular composition, etc (Song et al, 2019;Lin et al, 2018 (Huo et al, 2018). As a linear relationship between organic matter concentration and fluorescence intensity can be assumed for very dilute samples due to the IFE (Murphy et al, 2013), we have corrected our fluorescence data for IFE using absorbance to enable "clean " correlation analysis (as shown in Fig.…”

Section: Chromophores Responsible For Brc Light Absorptionmentioning

confidence: 99%

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

Jiao¹,

Wang²,

Zhong³

et al. 2021

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Abstract. Chromophores represent an important portion of light-absorbing species, i.e. brown carbon. Yet knowledge on 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 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 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, while these inferences exhibited a refutation with primary biomass burning and coal combustion results. A multiple linear regression analysis revealed that larger chromophores that were oxygen-rich and highly aromatic with high molecular weights, were the key contributors of light absorption, preferably at longer emission wavelength (λmax > 500 nm). Positive matrix factorization analysis further suggested that up to 60 % of these responsible chromophores originated from biomass burning emissions.

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“…The urban regions are mainly affected by anthropogenic emissions. Therefore, urban BrC may contain (Srinivas and Sarin, 2013;Bosch et al, 2014;Zhang et al, 2017b), rural sites (Hecobian et al, 2010;Kirillova et al, 2014a;Zhu et al, 2018;Xie et al, 2019) and urban sites (Kirillova et al, 2014b;Yan et al, 2015;Chen et al, 2018;Huang et al, 2018;Park et al, 2018). a large amount of aromatic chromophores with a high conjugation degree, which absorb light at a longer wavelength and have lower AAE values (Lambe et al, 2013;Wang et al, 2018).…”

Section: Source Apportionment Of Brcmentioning

confidence: 99%

Characterization of the light-absorbing properties, chromophore composition and sources of brown carbon aerosol in Xi'an, northwestern China

et al. 2020

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Abstract. The impact of brown carbon aerosol (BrC) on the Earth's radiative forcing balance has been widely recognized but remains uncertain, mainly because the relationships among BrC sources, chromophores and optical properties of aerosol are poorly understood. In this work, the light absorption properties and chromophore composition of BrC were investigated for samples collected in Xi'an, northwestern China, from 2015 to 2016. Both absorption Ångström exponent (AAE) and mass absorption efficiency (MAE) show distinct seasonal differences, which could be attributed to the differences in sources and chromophore composition of BrC. Three groups of light-absorbing organics were found to be important BrC chromophores, including compounds that have multiple absorption peaks at wavelengths > 350 nm (12 polycyclic aromatic hydrocarbons and their derivatives) and compounds that have a single absorption peak at wavelengths < 350 nm (10 nitrophenols and nitrosalicylic acids and 3 methoxyphenols). These measured BrC chromophores show distinct seasonal differences and contribute on average about 1.1 % and 3.3 % of light absorption of methanol-soluble BrC at 365 nm in summer and winter, respectively, about 7 and 5 times higher than the corresponding carbon mass fractions in total organic carbon. The sources of BrC were resolved by positive matrix factorization (PMF) using these chromophores instead of commonly used non-light-absorbing organic markers as model inputs. Our results show that vehicular emissions and secondary formation are major sources of BrC (∼ 70 %) in spring, coal combustion and vehicular emissions are major sources (∼ 70 %) in fall, biomass burning and coal combustion become major sources (∼ 80 %) in winter, and secondary BrC dominates (∼ 60 %) in summer.

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Molecular Characterization of Water- and Methanol-Soluble Organic Compounds Emitted from Residential Coal Combustion Using Ultrahigh-Resolution Electrospray Ionization Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Cited by 89 publications

References 77 publications

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis

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

Characterization of the light-absorbing properties, chromophore composition and sources of brown carbon aerosol in Xi'an, northwestern China

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