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Ice nucleation in aqueous solutions of short- and long-chain poly(vinyl alcohol) studied with a droplet microfluidics setup
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Eickhoff, Lukas, Keßler, Mira, Stubbs, Christopher D., Derksen, Jakob, Viefhues, Martina, Anselmetti, Dario, Gibson, Matthew I., Hoge, Berthold and Koop, Thomas (2023) Ice nucleation in aqueous solutions of short- and long-chain poly(vinyl alcohol) studied with a droplet microfluidics setup. The Journal of Chemical Physics, 158 (15). 154504. doi:10.1063/5.0136192 ISSN 0021-9606.
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Official URL: http://dx.doi.org/10.1063/5.0136192
Abstract
Poly(vinyl alcohol) (PVA) has ice binding and ice nucleating properties. Here, we explore the dependence of the molecular size of PVA on its ice nucleation activity. For this purpose, we studied ice nucleation in aqueous solutions of PVA samples with molar masses ranging from 370 to 145 000 g mol−1, with a particular focus on oligomer samples with low molar mass. The experiments employed a novel microfluidic setup that is a follow-up on the previous WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) design by Reicher et al. The modified setup introduced and characterized here, termed nanoliter Bielefeld Ice Nucleation ARraY (nanoBINARY), uses droplet microfluidics with droplets (96 ± 4) µm in diameter and a fluorinated continuous oil phase and surfactant. A comparison of homogeneous and heterogeneous ice nucleation data obtained with nanoBINARY to those obtained with WISDOM shows very good agreement, underpinning its ability to study low-temperature ice nucleators as well as homogeneous ice nucleation due to the low background of impurities. The experiments on aqueous PVA solutions revealed that the ice nucleation activity of shorter PVA chains strongly decreases with a decrease in molar mass. While the cumulative number of ice nucleating sites per mass nm of polymers with different molar masses is the same, it becomes smaller for oligomers and completely vanishes for dimer and monomer representatives such as 1,3-butanediol, propan-2-ol, and ethanol, most likely because these molecules become too small to effectively stabilize the critical ice embryo. Overall, our results are consistent with PVA polymers and oligomers acting as heterogeneous 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, Polyvinyl alcohol, Ice, Microfluidics | |||||||||
Journal or Publication Title: | The Journal of Chemical Physics | |||||||||
Publisher: | American Institute of Physics | |||||||||
ISSN: | 0021-9606 | |||||||||
Official Date: | 17 April 2023 | |||||||||
Dates: |
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Volume: | 158 | |||||||||
Number: | 15 | |||||||||
Article Number: | 154504 | |||||||||
DOI: | 10.1063/5.0136192 | |||||||||
Status: | Peer Reviewed | |||||||||
Publication Status: | Published | |||||||||
Re-use Statement: | 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 The Journal of Chemical Physics, 158 (15). 154504. and may be found at http://dx.doi.org/10.1063/5.0136192 | |||||||||
Access rights to Published version: | Free Access (unspecified licence, 'bronze OA') | |||||||||
Date of first compliant deposit: | 20 April 2023 | |||||||||
Date of first compliant Open Access: | 17 April 2024 | |||||||||
RIOXX Funder/Project Grant: |
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