Can COSMOTherm Predict a Salting in Effect?

Toivola, Martta; Prisle, Nønne L.; Elm, Jonas; Waxman, E.; Volkamer, Rainer; Kurtén, Theo

doi:10.1021/acs.jpca.7b04847

Cited by 20 publications

(19 citation statements)

References 28 publications

(131 reference statements)

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“…Changes in the relative ratios of unhydrated and hydrated forms would be expected due to changes in the molecular interactions (water-methylglyoxal, water-water) when ions co-exist in the solution. Such phenomena have been reported in previous experimental (Waxman et al, 2015) and computational (Toivola et al, 2017) studies, which have shown decrease of the cosolubility of methylglyoxal in aqueous solutions with addition of NaCl and Na 2 SO 4 (salting out effect). Here we observe a small change in the relative intensities between the peaks A and B in pure methylglyoxal solution compared to solution spiked with Na 2 SO 4 , but the shape of the background also changed in the spectrum and thus these changes remain inconclusive.…”

Section: Feature At 290 Evsupporting

confidence: 80%

Aqueous phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy

Michailoudi¹,

Lin²,

Yuzawa³

et al. 2020

Preprint

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Abstract. Glyoxal (CHOCHO) and methylglyoxal (CH3C(O)CHO) are well-known components of atmospheric particles and their properties can impact atmospheric chemistry and cloud formation. To get information on their hydration states in aqueous solutions and how they are affected by addition of inorganic salts (sodium chloride (NaCl) and sodium sulfate (Na2SO4)), we applied carbon and oxygen K-edge X-ray absorption spectroscopy (XAS) in transmission mode. The recorded C K-edge spectra show that glyoxal is completely hydrated in the dilute aqueous solutions, in line with previous studies. For methylglyoxal, we identified, supported by quantum chemical calculations, not only C-H, C=O and C-OH bonds, but also fingerprints of C-OH(CH2) and C=C bonds. This implies the presence of both mono- and dihydrated forms of methylglyoxal, as well as products of aldol condensation, and enol tautomers of the monohydrates. The addition of salts was found to introduce only very minor changes to absorption energies and relative intensities of the observed absorption features, indicating that the organic-inorganic interactions at the studied concentrations are not strong enough to affect the spectra in this work. The identified structures of glyoxal and methylglyoxal in aqueous environment support the uptake of these compounds to the aerosol phase in the presence of water and their contribution on secondary organic aerosol formation.

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Section: Feature At 290 Evsupporting

confidence: 80%

Aqueous phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy

Michailoudi¹,

Lin²,

Yuzawa³

et al. 2020

Preprint

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“…For NAFA concentrations between 0.1 and 1 g L À1 , surface tension for a given NAFA concentration tends to decrease with increasing NaCl concentration due to salting out of NAFA by NaCl. [31][32][33][34][35][36][37][38] This trend is however not uniform over the whole composition range. In particular for surface tensions at t ¼ 0 s, a trough appears in the tting surface, possibly due to the sensitivity of the t to data points.…”

Section: Modelingmentioning

confidence: 88%

Effects of surface tension time-evolution for CCN activation of a complex organic surfactant

Lin

Kristensen

Calderón

et al. 2020

Environ. Sci.: Processes Impacts

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“…When the nonideality is due to interactions with inorganic compounds, which can be highly concentrated in ambient aerosol particles, the effect is called a "salting-in" (γ < 1) or "salting-out" (γ > 1) interaction, depending on whether the interaction favors or disfavors, respectively, the presence of the compound in the phase in question. The effect of salting in or salting out on chemical systems with atmospheric relevance has been assessed with both experimental and theoretical approaches (Toivola et al, 2017;Wang et al, 2014;Waxman et al, 2015;Yu et al, 2011).…”

Section: Introductionmentioning

confidence: 99%

Single-particle experiments measuring humidity and inorganic salt effects on gas-particle partitioning of butenedial

et al. 2019

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Abstract. An improved understanding of the fate and properties of atmospheric aerosol particles requires a detailed process-level understanding of fundamental factors influencing the aerosol, including partitioning of aerosol components between the gas and particle phases. Laboratory experiments with levitated particles provide a way to study fundamental aerosol processes over timescales relevant to the multiday lifetime of atmospheric aerosol particles, in a controlled environment in which various characteristics relevant to atmospheric aerosol can be prepared (e.g., high surface-to-volume ratio, highly concentrated or supersaturated solutions, changes to relative humidity). In this study, the four-carbon unsaturated compound butenedial, a dialdehyde produced by oxidation of aromatic compounds that undergoes hydration in the presence of water, was used as a model organic aerosol component to investigate different factors affecting gas–particle partitioning, including the role of lower-volatility “reservoir” species such as hydrates, timescales involved in equilibration between higher- and lower-volatility forms, and the effect of inorganic salts. The experimental approach was to use a laboratory system coupling particle levitation in an electrodynamic balance (EDB) with particle composition measurement via mass spectrometry (MS). In particular, by fitting measured evaporation rates to a kinetic model, the effective vapor pressure was determined for butenedial and compared under different experimental conditions, including as a function of ambient relative humidity and the presence of high concentrations of inorganic salts. Even under dry (RH<5 %) conditions, the evaporation rate of butenedial is orders of magnitude lower than what would be expected if butenedial existed purely as a dialdehyde in the particle, implying an equilibrium strongly favoring hydrated forms and the strong preference of certain dialdehyde compounds to remain in a hydrated form even under lower water content conditions. Butenedial exhibits a salting-out effect in the presence of sodium chloride and sodium sulfate, in contrast to glyoxal. The outcomes of these experiments are also helpful in guiding the design of future EDB-MS experiments.

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Can COSMOTherm Predict a Salting in Effect?

Cited by 20 publications

References 28 publications

Aqueous phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy

Aqueous phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy

Effects of surface tension time-evolution for CCN activation of a complex organic surfactant

Single-particle experiments measuring humidity and inorganic salt effects on gas-particle partitioning of butenedial

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