Water uptake of humic and fulvic acid: measurements and modelling using single parameter Köhler theory

Hatch, C. D.; Gierlus, Kelly M.; Zahardis, James; Schuttlefield, Jennifer; Grassian, Vicki H.

doi:10.1071/en09083

Cited by 19 publications

(12 citation statements)

References 53 publications

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“…Multiple studies have sought to elucidate the hygroscopic properties of OA, as well as the influence of organic aerosol components on the hygroscopic behavior and phase transitions of inorganic salts. Much of this work has focused on single-and multicomponent aerosols comprised of carboxylic, dicarboxylic, and humic acids (e.g., Prenni et al, 2001;Choi and Chan, 2002a;Brooks et al, 2004;Chan et al, 2006;Moore and Raymond, 2008;Hatch et al, 2009;Pope et al, 2010;Lei et al, 2014), as well as mixtures of organic acids with inorganic salts (e.g., Cruz and Pandis, 2000;Choi and Chan, 2002b;Prenni et al, 2003;Wise et al, 2003;Brooks et al, 2004;Svenningsson et al, 2006;Sjogren et al, 2007;Gao et al, 2008). Recent studies have explored water uptake by sugars, higher molecular weight organics, and polymers (Gysel et al, 2004;Mochida and Kawamura, 2004;Tong et al, 2011;Zobrist et al, 2011;Lei et al, 2014;Xu et al, 2014).…”

Section: N Hodas Et Al: Influence Of Particle-phase State On the Hymentioning

confidence: 99%

Influence of particle-phase state on the hygroscopic behavior of mixed organic–inorganic aerosols

et al. 2015

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Abstract. Recent work has demonstrated that organic and mixed organic-inorganic particles can exhibit multiple phase states depending on their chemical composition and on ambient conditions such as relative humidity (RH). To explore the extent to which water uptake varies with particlephase behavior, hygroscopic growth factors (HGFs) of nine laboratory-generated, organic and organic-inorganic aerosol systems with physical states ranging from well-mixed liquids to phase-separated particles to viscous liquids or semi-solids were measured with the Differential Aerosol Sizing and Hygroscopicity Spectrometer Probe at RH values ranging from 40 to 90 %. Water-uptake measurements were accompanied by HGF and RH-dependent thermodynamic equilibrium calculations using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model. In addition, AIOMFAC-predicted growth curves are compared to several simplified HGF modeling approaches: (1) representing particles as ideal, well-mixed liquids; (2) forcing a single phase but accounting for non-ideal interactions through activity coefficient calculations; and (3) a Zdanovskii-Stokes-Robinson-like calculation in which complete separation of the inorganic and organic components is assumed at all RH values, with water uptake treated separately in each of the individual phases. We observed variability in the characteristics of measured hygroscopic growth curves across aerosol systems with differing phase behaviors, with growth curves approaching smoother, more continuous water uptake with decreasing prevalence of liquidliquid phase separation and increasing oxygen : carbon ratios of the organic aerosol components. We also observed indirect evidence for the dehydration-induced formation of highly viscous semi-solid phases and for kinetic limitations to the crystallization of ammonium sulfate at low RH for sucrosecontaining particles. AIOMFAC-predicted growth curves are generally in good agreement with the HGF measurements. The performances of the simplified modeling approaches, however, differ for particles with differing phase states. This suggests that no single simplified modeling approach can be used to capture the water-uptake behavior for the diversity of particle-phase behavior expected in the atmosphere. Errors in HGFs calculated with the simplified models are of sufficient magnitude to produce substantial errors in estimates of particle optical and radiative properties, particularly for the assumption that water uptake is driven by absorptive equilibrium partitioning with ideal particle-phase mixing.

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Section: N Hodas Et Al: Influence Of Particle-phase State On the Hymentioning

confidence: 99%

Influence of particle-phase state on the hygroscopic behavior of mixed organic–inorganic aerosols

et al. 2015

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“…The hygroscopic growth of humic acid sodium salts has been investigated by several previous laboratory studies (Badger et al, 2006;Gysel et al, 2004;Hatch et al, 2009). Gysel et al (2004) observed that humic acid sodium salts deliquesce at RH between 60-75 %.…”

Section: Humic Acid Sodium Saltsmentioning

confidence: 99%

Hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their influence on the water uptake of ammonium sulfate

Nowak

Poulain

et al. 2011

Atmos. Chem. Phys.

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Abstract. The hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their effects on ammonium sulfate were investigated using a hygroscopicity tandem differential mobility analyzer (H-TDMA). No hygroscopic growth is observed for disodium oxalate, while ammonium oxalate shows slight growth (growth factor = 1.05 at 90 %). The growth factors at 90 % RH for sodium acetate, disodium malonate, disodium succinate, disodium tartrate, diammonium tartrate, sodium pyruvate, disodium maleate, and humic acid sodium salt are 1.79, 1.78, 1.69, 1.54, 1.29, 1.70, 1.78, and 1.19, respectively. The hygroscopic growth of mixtures of organic salts with ammonium sulfate, which are prepared as surrogates of atmospheric aerosols, was determined. A clear shift in deliquescence relative humidity to lower RH with increasing organic mass fraction was observed for these mixtures. Above 80 % RH, the contribution to water uptake by the organic salts was close to that of ammonium sulfate for the majority of investigated compounds. The observed hygroscopic growth of the mixed particles at RH above the deliquescence relative humidity of ammonium sulfate agreed well with that predicted using the ZdanovskiiStokes-Robinson (ZSR) mixing rule. Mixtures of ammonium sulfate with organic salts are more hygroscopic than mixtures with organic acids, indicating that neutralization by gas-phase ammonia and/or association with cations of dicarbonxylic acids may enhance the hygroscopicity of the atmospheric particles.

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“…m Chan and Chan [2003]; EDB measurements at 22.5°C-23.8°C. n Hatch et al [2009]; TDMA measurements at 20°C. o Dinar et al [2007]; TDMA measurements at 21°C-23°C; G f at 95% was extrapolated.…”

Section: Category III Solutesmentioning

confidence: 99%

Hygroscopic growth of common organic aerosol solutes, including humic substances, as derived from water activity measurements

et al. 2011

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[1] Studies have shown that organic matter often constitutes up to 50% by mass of tropospheric aerosols. These organics may considerably affect the water uptake properties of these aerosols, impacting Earth's climate and atmosphere. However, considerable uncertainties still exist about hygroscopic properties of organic carbon (OC) in particles. In this study, we have assembled an apparatus to measure equilibrium water vapor pressure over bulk solutions. We used these results to calculate the hygroscopic growth curve and deliquescence relative humidity (DRH) of representative compounds in three OC categories: saccharides, mono/dicarboxylic acids, and HULIS (Humic-Like Substances). To our knowledge, this is the first study to examine the hygroscopic growth of HULIS by means of a bulk method on representative compounds such as fulvic and humic acids. We also explored the temperature effect on hygroscopic growth within the 0°C-30°C temperature range and found no effect. The DRH and hygroscopic growth obtained were in excellent agreement with published tandem differential mobility analyzer (TDMA), electrodynamic balance, and bulk data for sodium chloride, ammonium sulfate, d-glucose, levoglucosan, succinic acid, and glutaric acid. However, we found a hygroscopic growth factor of 1.0 at a relative humidity of 90% for phthalic, oxalic, humic, and two fulvic acids; these results disagree with various TDMA studies. The TDMA is used widely to study water uptake of organic particles but can be affected by particle microstructural arrangements before the DRH and by the inability to fully dry particles. Thus, in the future it will be important to confirm TDMA data for nondeliquescent organic particles with alternate methods.Citation: Zamora, I. R., A. Tabazadeh, D. M. Golden, and M. Z. Jacobson (2011), Hygroscopic growth of common organic aerosol solutes, including humic substances, as derived from water activity measurements,

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Water uptake of humic and fulvic acid: measurements and modelling using single parameter Köhler theory

Cited by 19 publications

References 53 publications

Influence of particle-phase state on the hygroscopic behavior of mixed organic–inorganic aerosols

Influence of particle-phase state on the hygroscopic behavior of mixed organic–inorganic aerosols

Hygroscopic behavior of atmospherically relevant water-soluble carboxylic salts and their influence on the water uptake of ammonium sulfate

Hygroscopic growth of common organic aerosol solutes, including humic substances, as derived from water activity measurements

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