Evolution of Organic Aerosol From Wood Smoke Influenced by Burning Phase and Solar Radiation

Liu, Siyuan; Liu, Dantong; Hu, Dawei; Kong, Shaofei; Wu, Yangzhou; Cheng, Yi; Qiu, Hao; Zheng, Shurui; Yan, Qishe; Zheng, Huang; Kang, Hanqing; Zhang, Jiale; Zhao, Delong; Liu, Quan; Sheng, Jian; Ye, Jianhuai; He, Hao; Ding, Deping

doi:10.1029/2021jd034534

Cited by 12 publications

(8 citation statements)

References 102 publications

(165 reference statements)

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“…Ammonium nitrate particles were used to calibrate the ionization efficiency (IE) in AMS following the standard protocol. The HR-ToF-AMS was operated with a collection efficiency (CE) of 0.5 and 1 min sampling time resolution. Elemental ratios (O/C, H/C) of organics were performed using the updated improved-ambient (IA) method as proposed by Canagaratna et al Organic ions were classified as hydrocarbons (C x H y + ) and fragments containing different numbers of oxygen (C x H y O 1 + , C x H y O 2 + , C x H y O 3 + ) and containing nitrogen are classified as containing (C x H y O z N p + ) or without oxygen (C x H y N p + ) and defined as N-fragments.…”

Section: Methodsmentioning

confidence: 99%

“…The HR-ToF-AMS was operated with a collection efficiency (CE) of 0.5 and 1 min sampling time resolution. Elemental ratios (O/C, H/C) of organics were performed using the updated improved-ambient (IA) method as proposed by Canagaratna et al Organic ions were classified as hydrocarbons (C x H y + ) and fragments containing different numbers of oxygen (C x H y O 1 + , C x H y O 2 + , C x H y O 3 + ) and containing nitrogen are classified as containing (C x H y O z N p + ) or without oxygen (C x H y N p + ) and defined as N-fragments. We aim to broadly (but not quantitively) identify the contribution of nitrogen-containing OA (NOCs) from the bulk OA, hereby using several N-containing ions including CN + , CNO + , CH 3 NO + , C 3 H 4 N + , C 3 H 5 N + , C 2 H 2 NO + , C 3 H 6 N + , C 2 H 3 NO + , C 3 H 7 N + , C 3 H 8 N + , C 2 H 5 NO + , and C 2 H 6 NO + ( f CxHyNp+CxHyNpOz ) as the main fragments in determining the fraction of NOCs.…”

Section: Methodsmentioning

confidence: 99%

“…) and containing nitrogen are classified as containing (C x H y O z N p + ) or without oxygen (C x H y N p + ) 55 and defined as N-fragments. We aim to broadly (but not quantitively) identify the contribution of nitrogencontaining OA (NOCs) from the bulk OA, hereby using several N-containing ions including CN + , CNO + , CH 3 NO + , and C main fragments 57 in determining the fraction of NOCs.…”

Section: Instrumentation For Aerosol Characterizationmentioning

confidence: 99%

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Connecting the Light Absorption of Atmospheric Organic Aerosols with Oxidation State and Polarity

Jiang

Liu

et al. 2022

Environ. Sci. Technol.

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The light-absorbing organic aerosol (OA) constitutes an important fraction of absorbing components, counteracting major cooling effect of aerosols to climate. The mechanisms in linking the complex and changeable chemistry of OA with its absorbing properties remain to be elucidated. Here, by using solvent extraction, ambient OA from an urban environment was fractionated according to polarity, which was further nebulized and online characterized with compositions and absorbing properties. Water extracted high-polar compounds with a significantly higher oxygen to carbon ratio (O/C) than methanol extracts. A transition O/C of about 0.6 was found, below and above which the enhancement and reduction of OA absorptivity were observed with increasing O/C, occurring on the less polar and high polar compounds, respectively. In particular, the co-increase of nitrogen and oxygen elements suggests the important role of nitrogen-containing functional groups in enhancing the absorptivity of the less polar compounds (e.g., forming nitrogen-containing aromatics), while further oxidation (O/C > 0.6) on high-polar compounds likely led to fragmentation and bleaching chromophores. The results here may reconcile the previous observations about darkening or whitening chromophores of brown carbon, and the parametrization of O/C has the potential to link the changing chemistry of OA with its polarity and absorbing properties.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Instrumentation For Aerosol Characterizationmentioning

confidence: 99%

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Connecting the Light Absorption of Atmospheric Organic Aerosols with Oxidation State and Polarity

Jiang

Liu

et al. 2022

Environ. Sci. Technol.

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“…The vertical transport of aerosol and gases in the planetary boundary layer (PBL) from the surface to the lower free troposphere (FT) importantly determines the influence of anthropogenic emissions to the upper level of the atmosphere; for example, aerosols in the upper level of the PBL may have more important feedback effects in influencing the boundary layer dynamics (Li et al, 2017). The aerosol could be upward transported from surface to upper level through daytime convective mixing in the PBL (Garratt, 1994).…”

Section: Introductionmentioning

confidence: 99%

Reduced volatility of aerosols from surface emissions to the top of the planetary boundary layer

Liu

et al. 2021

Atmos. Chem. Phys.

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Abstract. Aerosols from surface emission can be transported upwards through convective mixing in the planetary boundary layer (PBL), which subsequently interact with clouds, serving as important sources to nucleate droplets or ice particles. However, the evolution of aerosol composition during this vertical transport has yet to be explicitly understood. In this study, simultaneous measurements of detailed aerosol compositions were conducted at two sites, namely urban Beijing (50 m above sea level – a.s.l.) and Haituo mountain (1344 m a.s.l.) during wintertime, representing the anthropogenically polluted surface environment and the top of the PBL, respectively. The pollutants from surface emissions were observed to reach the mountain site on daily basis through daytime PBL convective mixing. From the surface to the top of PBL, we found efficient transport or formation of lower-volatility species (black carbon, sulfate, and low-volatile organic aerosol, OA); however, a notable reduction in semivolatile substances, such as the fractions of nitrate and semivolatile OA reduced by 74 % and 76 %, respectively, during the upward transport. This implies that the mass loss of these semivolatile species was driven by the evaporation process, which repartitioned the condensed semivolatile substances to the gas phase when aerosols were transported and exposed to a cleaner environment. In combination with the oxidation processes, these led to an enhanced oxidation state of OA at the top of the PBL compared to surface environment, with an increase of oxygen to carbon atomic ratio by 0.2. Such a reduction in aerosol volatility during vertical transport may be important in modifying its viscosity, nucleation activity, and atmospheric lifetime.

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“…Smoldering emissions were rich in carbonaceous peaks. The flaming phase generally produced organic aerosols of higher light absorptivity, while the light scattering particles dominated in the smoldering phase. , It suggested that the particles emitted under different burning conditions should be treated separately in climate modeling . Representative particles versus total single particles are given in Figure S3.…”

Section: Resultsmentioning

confidence: 99%

Impact of Dilution Ratio and Burning Conditions on the Number Size Distribution and Size-Dependent Mixing State of Primary Particles from Domestic Solid Fuel Burning

Zheng

Kong

Yan

et al. 2022

Environ. Sci. Technol. Lett.

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Dilution ratios (DRs) and burning conditions obviously affect particle number size distributions (PNSD), chemical compositions, and mixing states. These impacts for domestic solid fuel burning were investigated. For honeycomb briquettes, total particle number emission factors (EFPN) under DR150 for flaming and smoldering were (7.1 ± 0.8) × 1015 and (19.6 ± 5.9) × 1016 particles kg–1, respectively. Smoldering and flaming conditions promoted different emissions of organic species, mineral species, trace metals, and soot particles, impacting the following homogeneous nucleation or condensation and collision, which could explain their diversities in PNSD. The EFPN would be overestimated under DR150 and underestimated under DR100. Single particles were classified into carbonaceous particles, K–rich particles, Na–K particles, metal particles, and other particles. For coal burning, metal-containing particles dominated (9.5%–88.7%) the particles in the size range of 0.5–1.5 μm, with 3.7%–90.3% of them containing iron (Fe). Here, 93.1% of Fe particles were already internally mixed with sulfate, and high DR150 would promote their mixing. For crop residue and wood flaming, the mixed elemental and organic carbon (ECOC) particles dominated (87.1%–95.2%), with 74.7% and 45.1% of them containing levoglucosan. The PNSDs and mixing states of chemical species are helpful to update the initial settings of corresponding modeling studies.

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Evolution of Organic Aerosol From Wood Smoke Influenced by Burning Phase and Solar Radiation

Abstract: Biomass burning emissions are the most important contributors to the global carbonaceous aerosols in the atmosphere, leading to important climate and human health impacts (

Cited by 12 publications

References 102 publications

Connecting the Light Absorption of Atmospheric Organic Aerosols with Oxidation State and Polarity

Connecting the Light Absorption of Atmospheric Organic Aerosols with Oxidation State and Polarity

Reduced volatility of aerosols from surface emissions to the top of the planetary boundary layer

Impact of Dilution Ratio and Burning Conditions on the Number Size Distribution and Size-Dependent Mixing State of Primary Particles from Domestic Solid Fuel Burning

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