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Disordering effect of the ammonium cation accounts for anomalous enhancement of heterogeneous ice nucleation
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Whale, Thomas F. (2022) Disordering effect of the ammonium cation accounts for anomalous enhancement of heterogeneous ice nucleation. The Journal of Chemical Physics . doi:10.1063/5.0084635 ISSN 0021-9606.
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Official URL: http://dx.doi.org/10.1063/5.0084635
Abstract
Heterogeneous nucleation of ice from supercooled water is the process responsible for triggering nearly all ice formation in the natural environment. Understanding of heterogeneous ice nucleation is particularly key for understanding the formation of ice in clouds, which impacts weather and climate. While many effective ice nucleators are known the mechanisms of their actions remain poorly understood. Some inorganic nucleators have been found to nucleate ice at warmer temperatures in dilute ammonium solution than in pure water. This is surprising, analogous to salty water melting at a warmer temperature than pure water. Here, the magnitude of this effect is rationalized as being due to thermodynamically favorable ammonium-induced disordering of the hydrogen bond network of ice critical clusters formed on inorganic ice nucleators. Theoretical calculations are shown to be consistent with new experimental measurements aimed at finding the maximum magnitude of the effect. The implication of this study is that the ice-nucleating sites and surfaces of many inorganic ice nucleators are either polar or charged and therefore tend to induce formation of hydrogen ordered ice clusters. This work corroborates various literature reports indicating that some inorganic ice nucleators are most effective when nominally neutral and implies a commonality in mechanism between a wide range of inorganic ice nucleators.
Item Type: | Journal Article | |||||||||
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Subjects: | Q Science > QD Chemistry | |||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | |||||||||
Library of Congress Subject Headings (LCSH): | Nucleation, Ice, Solution (Chemistry) | |||||||||
Journal or Publication Title: | The Journal of Chemical Physics | |||||||||
Publisher: | American Institute of Physics | |||||||||
ISSN: | 0021-9606 | |||||||||
Official Date: | 28 March 2022 | |||||||||
Dates: |
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DOI: | 10.1063/5.0084635 | |||||||||
Status: | Peer Reviewed | |||||||||
Publication Status: | Published | |||||||||
Reuse Statement (publisher, data, author rights): | This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Thomas F Whale, "Disordering effect of the ammonium cation accounts for anomalous enhancement of heterogeneous ice nucleation", J. Chem. Phys. (2022); and may be found at https://doi.org/10.1063/5.0084635 | |||||||||
Access rights to Published version: | Open Access (Creative Commons) | |||||||||
Date of first compliant deposit: | 7 April 2022 | |||||||||
Date of first compliant Open Access: | 8 April 2022 | |||||||||
RIOXX Funder/Project Grant: |
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