Glass transition of aqueous solutions involving annealing-induced ice recrystallization resolves liquid-liquid transition puzzle of water

Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions based on annealing-induced upshift of glass-liquid transition temperature, . Here we report a universal water-content, , dependence of for aqueo...

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Published inScientific reports Vol. 5; no. 1; p. 15714
Main Authors Zhao, Li-Shan, Cao, Ze-Xian, Wang, Qiang
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 27.10.2015
Nature Publishing Group
Subjects
140/133
639/638/440/94
639/766/119/1002
Humanities and Social Sciences
multidisciplinary
Science
Online AccessGet full text
ISSN2045-2322
2045-2322
DOI10.1038/srep15714

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Abstract Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions based on annealing-induced upshift of glass-liquid transition temperature, . Here we report a universal water-content, , dependence of for aqueous solutions. Solutions with vitrify/devitrify at a constant temperature, , referring to freeze-concentrated phase with left behind ice crystallization. Those solutions with totally vitrify at under conventional cooling/heating process though, of the samples annealed at temperatures   to effectively evoke ice recrystallization is stabilized at . Experiments on aqueous glycerol and 1,2,4-butanetriol solutions in literature were repeated and the same samples subject to other annealing treatments equally reproduce the result. The upshift of by annealing is attributable to freeze-concentrated phase of solutions instead of ‘liquid II phase of water’. Our work also provides a reliable method to determine hydration formula and to scrutinize solute-solvent interaction in solution.
AbstractList Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions based on annealing-induced upshift of glass-liquid transition temperature, T(g) . Here we report a universal water-content, X(aqu) , dependence of T(g) for aqueous solutions. Solutions with X(aqu)>X(cr)(aqu)vitrify/devitrify at a constant temperature, ~T(g) , referring to freeze-concentrated phase with X(aqu)left behind ice crystallization. Those solutions with X(aqu)<X(aqu)<X(cr)(aqu) totally vitrify at Tg<Tg under conventional cooling/heating process though, Tg of the samples annealed at temperatures   to effectively evoke ice recrystallization is stabilized at . Experiments on aqueous glycerol and 1,2,4-butanetriol solutions in literature were repeated, and the same samples subject to other annealing treatments equally reproduce the result. The upshift of T(g) by annealing is attributable to freeze-concentrated phase of solutions instead of 'liquid II phase of water'. Our work also provides a reliable method to determine hydration formula and to scrutinize solute-solvent interaction in solution.
Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions based on annealing-induced upshift of glass-liquid transition temperature, "Equation missing" . Here we report a universal water-content, "Equation missing" , dependence of "Equation missing" for aqueous solutions. Solutions with "Equation missing" vitrify/devitrify at a constant temperature, "Equation missing" , referring to freeze-concentrated phase with "Equation missing" left behind ice crystallization. Those solutions with "Equation missing" totally vitrify at "Equation missing" under conventional cooling/heating process though, "Equation missing" of the samples annealed at temperatures  "Equation missing" to effectively evoke ice recrystallization is stabilized at "Equation missing" . Experiments on aqueous glycerol and 1,2,4-butanetriol solutions in literature were repeated and the same samples subject to other annealing treatments equally reproduce the result. The upshift of "Equation missing" by annealing is attributable to freeze-concentrated phase of solutions instead of ‘liquid II phase of water’. Our work also provides a reliable method to determine hydration formula and to scrutinize solute-solvent interaction in solution.
Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions based on annealing-induced upshift of glass-liquid transition temperature, . Here we report a universal water-content, , dependence of for aqueous solutions. Solutions with vitrify/devitrify at a constant temperature, , referring to freeze-concentrated phase with left behind ice crystallization. Those solutions with totally vitrify at under conventional cooling/heating process though, of the samples annealed at temperatures   to effectively evoke ice recrystallization is stabilized at . Experiments on aqueous glycerol and 1,2,4-butanetriol solutions in literature were repeated and the same samples subject to other annealing treatments equally reproduce the result. The upshift of by annealing is attributable to freeze-concentrated phase of solutions instead of ‘liquid II phase of water’. Our work also provides a reliable method to determine hydration formula and to scrutinize solute-solvent interaction in solution.
ArticleNumber 15714
Author Zhao, Li-Shan
Wang, Qiang
Cao, Ze-Xian
Author_xml – sequence: 1
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  surname: Zhao
  fullname: Zhao, Li-Shan
  organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Department of Physics, University of Science and Technology Beijing
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  givenname: Ze-Xian
  surname: Cao
  fullname: Cao, Ze-Xian
  organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
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  givenname: Qiang
  surname: Wang
  fullname: Wang, Qiang
  organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences
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Snippet Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions...
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Title Glass transition of aqueous solutions involving annealing-induced ice recrystallization resolves liquid-liquid transition puzzle of water
URI https://link.springer.com/article/10.1038/srep15714
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