A1 Journal article (refereed), original research

Heterogeneous Nucleation of Butanol on NaCl: A Computational Study of Temperature, Humidity, Seed Charge, and Seed Size Effects


Open Access hybrid publication

LUT Authors / Editors

Publication Details
Authors: Toropainen Antti, Kangasluoma Juha, Kurtén Theo, Vehkamäki Hanna, Keshavarz Fatemeh, Kubečka Jakub
Publisher: American Chemical Society
Publication year: 2021
Language: English
Related journal or series: Journal of Physical Chemistry A
Volume number: 125
Issue number: 14
Start page: 3025
End page: 3036
Number of pages: 12
ISSN: 1089-5639
eISSN: 1520-5215
JUFO level of this publication: 1
Open Access: Open Access hybrid publication

Abstract

Using a combination of quantum chemistry and cluster size distribution dynamics, we study the heterogeneous nucleation of n-butanol and water onto sodium chloride (NaCl)10 seeds at different butanol saturation ratios and relative humidities. We also investigate how the heterogeneous nucleation of butanol is affected by the seed size through comparing (NaCl)5, (NaCl)10, and (NaCl)25 seeds and by seed electrical charge through comparing (Na10Cl9)+, (NaCl)10, and (Na9Cl10)− seeds. Butanol is a common working fluid for condensation particle counters used in atmospheric aerosol studies, and NaCl seeds are frequently used for calibration purposes and as model systems, for example, sea spray aerosol. In general, our simulations reproduce the experimentally observed trends for the NaCl–BuOH–H2O system, such as the increase of nucleation rate with relative humidity and with temperature (at constant supersaturation of butanol). Our results also provide molecular-level insights into the vapor–seed interactions driving the first steps of the heterogeneous nucleation process. The main purpose of this work is to show that theoretical studies can provide molecular understanding of initial steps of heterogeneous nucleation and that it is possible to find cost-effective yet accurate-enough combinations of methods for configurational sampling and energy evaluation to successfully model heterogeneous nucleation of multicomponent systems. In the future, we anticipate that such simulations can also be extended to chemically more complex seeds.


Last updated on 2021-12-05 at 07:51

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