Abundance and Light Absorption Properties of Brown Carbon Emitted from Residential Coal Combustion in China

Li, Meiju; Fan, Xingjun; Zhu, Mengbo; Zou, Chunlin; Song, Jianzhong; Wei, Siye; Jia, Wanglu; Peng, Ping’an

doi:10.1021/acs.est.8b05630

Cited by 114 publications

(82 citation statements)

References 60 publications

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“…2). The measured emission factors in this study fall within the range of previous straw burning experiments (4.7-12.9, 1.2-8.9 and 0.17-1.2 g kg −1 for PM 2.5 , OC and EC, respectively) (Akagi et al, 2011;Hays et al, 2005;Li et al, 2007). The estimated EFs from crop residue burning were generally lower than wood or forest burning emissions (Akagi et al, 2011;Aurell and Gullett, 2013;Jen et al, 2019).…”

Section: Emission Factors Of Carbonaceous Aerosolssupporting

confidence: 81%

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Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiency

Wang

et al. 2020

Atmos. Chem. Phys.

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Abstract. Biomass burning is one of the major sources of carbonaceous aerosols, which affects air quality, the radiation budget and human health. Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood compared with wood burning emissions. In this study, lab-controlled straw (wheat and corn) burning experiments were designed to investigate the emission factors and light absorption properties of different biomass burning organic aerosol (BBOA) fractions, including water-soluble organic carbon (WSOC), humic-like substances (HULIS) and water-insoluble organic carbon (WISOC). The influences of biofuel moisture content and combustion efficiency on emissions are comprehensively discussed. The emission factors of PM2.5, organic carbon (OC) and elemental carbon (EC) were 9.3±3.4, 4.6±1.9 and 0.21±0.07 g kg−1 for corn burning and 8.7±5.0, 3.9±2.8 and 0.22±0.05 g kg−1 for wheat burning, generally lower than wood or forest burning emissions. Though the mass contribution of WISOC to OC (32 %–43 %) was lower than WSOC, the light absorption contribution of WISOC (57 %–84 % at 300–400 nm) surpassed WSOC due to the higher mass absorption efficiency (MAE) of WISOC. The results suggested that BBOA light absorption would be largely underestimated if only the water-soluble fractions were considered. However, the light absorption of WSOC in the near-UV range, occupying 39 %–43 % of the total extracted OC absorption at 300 nm, cannot be negligible due to the sharper increase of absorption towards shorter wavelengths compared with WISOC. HULIS were the major light absorption contributors to WSOC, due to the higher MAE of HULIS than other high-polarity WSOC components. The emission levels and light absorption of BBOA were largely influenced by the burning conditions, indicated by modified combustion efficiency (MCE) calculated by measured CO and CO2 in this study. The emission factors of PM2.5, OC, WSOC, HULIS and organic acids were enhanced under lower MCE conditions or during higher moisture straw burning experiments. Light absorption coefficients of BBOA at 365 nm were also higher under lower MCE conditions, which was mainly due to the elevated mass emission factors. Our results suggested that the influence of varied combustion efficiency on particle emissions could surpass the differences caused by different types of biofuels. Thus, the burning efficiency or conditions should be taken into consideration when estimating the influence of biomass burning. In addition, we observed that the ratios of K+/OC and Cl-/OC increased under higher MCE conditions due to the enhancement of potassium and chlorine released under higher fire temperatures during flaming combustion. This indicates that the potassium ion, as a commonly used biomass burning tracer, may lead to estimation uncertainty if the burning conditions are not considered.

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Section: Emission Factors Of Carbonaceous Aerosolssupporting

confidence: 81%

“…Organic matter (OM), calculated by multiplying OC by 1.3 (Li et al, 2007), was the dominant component of straw burning aerosols, which accounted for ∼ 64 % and ∼ 55 % of the PM 2.5 emitted from corn and wheat burning, respectively (Fig. 2).…”

Section: Emission Factors Of Carbonaceous Aerosolsmentioning

confidence: 99%

Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiency

Wang

et al. 2020

Atmos. Chem. Phys.

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“…In addition, results showed that compounds observed in CC aerosols had lower H / C and O / C ratios than those in BB aerosols and vehicle emissions, indicating a higher unsaturated degree and lower oxidation level. There were compounds outside the specified regions, which had a high H / C ratio (≥ 2.2) and DBE of 0, corresponding to saturated oxygenated species, and there could be some long-chain polyalcohols (Lin et al, 2012a).…”

Section: Molecular Composition Detected By Ft-icr Msmentioning

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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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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“…Moreover, the higher MAE365 in biomass burning and bituminous coal combustion represented a stronger absorbing ability in the case of the MSOC fraction, which reflected greater variation in the chemical composition than in the WSOC fraction. The MAE365 of biomass burning and coal combustion in the WSOC fraction was also higher than that of ambient aerosol and biomass and coal combustion experiments in a laboratory sampling system (Chen et al, 2018;Zhu et al, 2018;Yan et al, 2015;Li et al, 2018;Park and Yu, 2016) ( Figure S4).…”

Section: Emission Characteristics and Optical Properties Of Extractsmentioning

confidence: 90%

“…Purified water was used as a baseline correction before measure. Mass absorption efficiency (MAE, m 2 g -1 C) can be obtained as following equation (Li et al, 2018):…”

Section: Uv−vis Absorption Spectra and Eem Fluorescence Spectramentioning

confidence: 99%

Molecular compositions and optical properties of dissolved brown carbon in smoke particles illuminated by excitation-emission matrix spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis

Tang

et al. 2019

Preprint

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<p><strong>Abstract.</strong> We investigated the fluorescence and chemical-structural characteristics of dissolved brown carbon (BrC) in smoke particulates emitted from the combustion of biomass and fossil fuels (coal and vehicle exhaust) by excitation-emission matrix (EEM) spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) coupled with electrospray ionization (ESI). Six components were resolved by parallel factor analysis (PARAFAC) of the water-soluble and methanol-soluble organic carbon (MSOC) fractions, respectively. These fluorescent components varied among sources. Combined with FT-ICR MS ion groups, we found that the fluorescent components agreed well with the functional groups, particularly with nitrogen (N)- and sulfur (S)-containing groups. Among the six PARAFAC components (P1&#8211;6) retrieved from the water-soluble organic carbon (WSOC) fraction, except for the P3 component, the other components exhibited different values among the three types of emission sources tested. Vehicle exhaust was characterized by high P1 and P6 components, which are mainly associated with aromatic organosulfate compounds, and a high P5 component, mainly associated with sulfonates; coal combustion was characterized by a high P4 component, which is associated with nitrooxy-organosulfate (nitrooxy-OS) compounds; and biomass burning was characterized by the P2 component. Similar results were observed in the case of the MSOC fraction. This study reveals the source contribution and possible structures of previously unclear excitation-emission matrix (EEM) fluorescent components in combustion-derived aerosols. These are the first findings of this type and are potentially applicable to further studies on EEM-based source apportionment of dissolved BrC in aerosols.</p>

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Abundance and Light Absorption Properties of Brown Carbon Emitted from Residential Coal Combustion in China

Cited by 114 publications

References 60 publications

Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiency

Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiency

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 smoke particles illuminated by excitation-emission matrix spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis

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