Hygroscopicity of polycatechol and polyguaiacol secondary organic aerosol in sub- and supersaturated water vapor environments

Malek, Kotiba A.; Gohil, Kanishk; Al‐Abadleh, Hind A.; Asa-Awuku, Akua

doi:10.1039/d1ea00063b

Cited by 14 publications

(16 citation statements)

References 55 publications

(147 reference statements)

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“…κ-Köhler theory describes the water uptake of a wide range of organic aerosol components, including secondary organic aerosol, so it is expected to apply to secondary BrC, as well. In fact, κ-Köhler theory has recently been applied to polycatechol aerosol generated by iron-catalyzed reactions, broadly similar to the oligomeric products of OH-initiated oxidation . It is noted that there are systems, like 4-nitrocatechol internally mixed with ammonium sulfate, for which hygroscopic growth may not precisely follow κ-Köhler theory.…”

Section: Resultsmentioning

confidence: 99%

“…24 The κ value reported here for secondary BrC from catechol is slightly less than a recently reported measurement for polycatechol aerosol generated by iron-catalyzed reactions, 0.13 ± 0.05. 90 H-TMDA studies have also probed surrogates of primary biomass burning organic aerosol. 38,93,94 There is no systematic trend with the degree of functionalization of the precursor; i.e., κ was about the same for phenol (least functionalized) and pyrogallol (most functionalized), while it was only slightly less for catechol.…”

Section: ■ Introductionmentioning

confidence: 99%

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Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Betz

Calvert

Al-Mashala

et al. 2022

ACS Earth Space Chem.

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To understand the impact of light-absorbing organic aerosol, also called brown carbon (BrC), it is necessary to determine the extent to which the direct effect through aerosol− radiation interactions and the indirect effect through aerosol−cloud interactions change during its atmospheric residence time. Toward addressing this need, the light absorption and water uptake of secondary BrC aerosol produced from phenolic compounds, abundant biomass burning emissions, were measured. Phenol, catechol, and pyrogallol were selected to form a homologous series, varying in the number of hydroxyl substituents, and they were exposed to aqueous hydroxyl radical in a photoreactor, leading to the formation of secondary BrC. The absorptivity of the BrC was monitored by UV−vis spectroscopy; the hygroscopicity was determined using a hygroscopic tandem differential mobility analyzer. The absorptivity of the secondary BrC increased within 8 h of photo-oxidation and then began decreasing. After 24 h of photooxidation, at an atmospherically relevant OH exposure of 2.2 × 10 −10 mol s L −1 , the hygroscopicity parameters for BrC from phenol, catechol, and pyrogallol were similar, i.e., 0.13 ± 0.02, 0.10 ± 0.02, and 0.13 ± 0.02, respectively, so BrC from phenolic compounds exhibits similar water uptake regardless of the functionalization of the precursor. After 36 and 48 h of continued photo-oxidation, during which the product mixture exhibited further whitening, the hygroscopicity parameter of secondary BrC from catechol did not change. These observations suggest that the changes in absorptivity (related to the direct effect) of secondary BrC produced from phenolic precursors are greater than the changes in hygroscopicity (related to the indirect effect) upon atmospheric aging.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Betz

Calvert

Al-Mashala

et al. 2022

ACS Earth Space Chem.

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“…Hygroscopic growth and CCN activation of complex organic systems have been modeled by a few different approaches. ,,,,,− Some models explicitly consider all chemical species by employing functional group contribution methods. − , This approach is advantageous especially when the chemical composition of OM is completely measurable or predictable. ,, For instance, Hodas et al employed the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model for explaining the experimentally obtained CCN activity for mixtures of polyethylene glycol and ammonium sulfate. Malek et al accounted for hygroscopicity and CCN activity of polycatechol and polyguaiacol particles using adsorption isotherm theories. Nakao considered the relationships between elemental composition, volatility, molecular weight, and CCN activity for explaining empirically observed relationships between cloud nucleation ability and chemical composition of OM.…”

Section: Introductionmentioning

confidence: 99%

“…15,18,39 For instance, Hodas et al 41 employed the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model for explaining the experimentally obtained CCN activity for mixtures of polyethylene glycol and ammonium sulfate. Malek et al 42 accounted for hygroscopicity and CCN activity of polycatechol and polyguaiacol particles using adsorption isotherm theories. Nakao 43 considered the relationships between elemental composition, volatility, molecular weight, and CCN activity for explaining empirically observed relationships between cloud nucleation ability and chemical composition of OM.…”

Section: ■ Introductionmentioning

confidence: 99%

Water Solubility Distribution of Organic Matter Accounts for the Discrepancy in Hygroscopicity among Sub- and Supersaturated Humidity Regimes

Lee

Deng

Zhou

et al. 2022

Environ. Sci. Technol.

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Water uptake properties of organic matter (OM) are critical for aerosol direct and indirect effects. OM contains various chemical species that have a wide range of water solubility. However, the role of water solubility on water uptake by OM has poorly been investigated. We experimentally retrieved water solubility distributions of water-soluble OM (WSOM) from combustion of mosquito coil and tropical peat using the 1-octanol–water partitioning method. In addition, hygroscopic growth and cloud condensation nuclei (CCN) activity of solubility-segregated WSOM were measured. The dominant fraction of WSOM from mosquito coil smoldering was highly soluble (water solubility (S) > 10–2 g cm–3), while that from peat combustion contained ∼40% of less-soluble species (S < 10–3 g cm–3). The difference in water solubility distributions induced changes in the roles of less water-soluble fractions (S < 10–3 g cm–3) on CCN activity. Namely, the less water-soluble fraction from mosquito coil combustion fully dissolved at the point of critical supersaturation, while that for tropical peat smoldering was limited by water solubility. The present result suggests that water solubility distributions of OM, rather than its bulk chemical property, need to be quantified for understanding the water uptake process.

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“…The high growth factors measured for o AP + Fe(III), p AP + Fe(III) can be attributed to the presence of high-density hydrophilic functional groups in their polymeric structures. Previous literature has ascribed the high hygroscopicity measured for insoluble polymers due to the presence of hydroxyl groups in their structures 78 . In addition, The high surface area of their polymeric structures is conductive for water condensation which can drive droplet growth as reported by Gohil et al 79 .…”

Section: Resultsmentioning

confidence: 99%

Reactivity of aminophenols in forming nitrogen-containing brown carbon from iron-catalyzed reactions

et al. 2022

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Nitrogen-containing organic carbon (NOC) in atmospheric particles is an important class of brown carbon (BrC). Redox active NOC like aminophenols received little attention in their ability to form BrC. Here we show that iron can catalyze dark oxidative oligomerization of o- and p-aminophenols under simulated aerosol and cloud conditions (pH 1–7, and ionic strength 0.01–1 M). Homogeneous aqueous phase reactions were conducted using soluble Fe(III), where particle growth/agglomeration were monitored using dynamic light scattering. Mass yield experiments of insoluble soot-like dark brown to black particles were as high as 40%. Hygroscopicity growth factors (κ) of these insoluble products under sub- and super-saturated conditions ranged from 0.4–0.6, higher than that of levoglucosan, a prominent proxy for biomass burning organic aerosol (BBOA). Soluble products analyzed using chromatography and mass spectrometry revealed the formation of ring coupling products of o- and p-aminophenols and their primary oxidation products. Heterogeneous reactions of aminophenol were also conducted using Arizona Test Dust (AZTD) under simulated aging conditions, and showed clear changes to optical properties, morphology, mixing state, and chemical composition. These results highlight the important role of iron redox chemistry in BrC formation under atmospherically relevant conditions.

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Hygroscopicity of polycatechol and polyguaiacol secondary organic aerosol in sub- and supersaturated water vapor environments

Abstract: Polycatechol and polyguaiacol are light-absorbing and water-insoluble compounds that are produced from biomass burning emissions. The aerosol can act as seeds for cloud droplet formation.

Cited by 14 publications

References 55 publications

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Hygroscopicity of Secondary Brown Carbon Aerosol from Aqueous Photo-Oxidation of Phenolic Precursors

Water Solubility Distribution of Organic Matter Accounts for the Discrepancy in Hygroscopicity among Sub- and Supersaturated Humidity Regimes

Reactivity of aminophenols in forming nitrogen-containing brown carbon from iron-catalyzed reactions

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