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.
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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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21 April 2023
Research Article|
April 17 2023
Ice nucleation in aqueous solutions of short- and long-chain poly(vinyl alcohol) studied with a droplet microfluidics setup
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Nucleation: Current Understanding Approaching 150 Years After Gibbs
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Lukas Eickhoff
;
Lukas Eickhoff
(Conceptualization, Formal analysis, Investigation, Methodology, Project administration, Validation, Visualization, Writing – original draft, Writing – review & editing)
1
Faculty of Chemistry, Bielefeld University
, 33615 Bielefeld, Germany
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Mira Keßler
;
Mira Keßler
(Investigation, Methodology, Resources, Visualization, Writing – review & editing)
1
Faculty of Chemistry, Bielefeld University
, 33615 Bielefeld, Germany
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Christopher Stubbs
;
Christopher Stubbs
(Investigation, Resources)
2
Department of Chemistry, University of Warwick
, Coventry CV4 7AL, United Kingdom
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Jakob Derksen;
Jakob Derksen
a)
(Investigation, Resources, Writing – review & editing)
3
Faculty of Physics, Bielefeld University
, 33615 Bielefeld, Germany
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Martina Viefhues
;
Martina Viefhues
(Methodology, Resources, Supervision, Writing – review & editing)
3
Faculty of Physics, Bielefeld University
, 33615 Bielefeld, Germany
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Dario Anselmetti
;
Dario Anselmetti
(Funding acquisition, Methodology, Project administration, Resources, Supervision, Writing – review & editing)
3
Faculty of Physics, Bielefeld University
, 33615 Bielefeld, Germany
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Matthew I. Gibson
;
Matthew I. Gibson
(Funding acquisition, Methodology, Project administration, Resources, Supervision, Writing – review & editing)
2
Department of Chemistry, University of Warwick
, Coventry CV4 7AL, United Kingdom
4
Division of Biomedical Sciences, Warwick Medical School, University of Warwick
, Coventry CV4 7AL, United Kingdom
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Berthold Hoge
;
Berthold Hoge
(Funding acquisition, Methodology, Project administration, Resources, Supervision)
1
Faculty of Chemistry, Bielefeld University
, 33615 Bielefeld, Germany
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Thomas Koop
Thomas Koop
b)
(Conceptualization, Funding acquisition, Methodology, Project administration, Supervision, Writing – original draft, Writing – review & editing)
1
Faculty of Chemistry, Bielefeld University
, 33615 Bielefeld, Germany
b)Author to whom correspondence should be addressed: [email protected]
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b)Author to whom correspondence should be addressed: [email protected]
a)
Now at: School of Life Sciences, University of Siegen, 57076 Siegen, Germany.
J. Chem. Phys. 158, 154504 (2023)
Article history
Received:
November 24 2022
Accepted:
February 22 2023
Citation
Lukas Eickhoff, Mira Keßler, Christopher Stubbs, Jakob Derksen, Martina Viefhues, Dario Anselmetti, Matthew I. Gibson, Berthold Hoge, Thomas Koop; Ice nucleation in aqueous solutions of short- and long-chain poly(vinyl alcohol) studied with a droplet microfluidics setup. J. Chem. Phys. 21 April 2023; 158 (15): 154504. https://doi.org/10.1063/5.0136192
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