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Title: The puzzling first-order phase transition in water–glycerol mixtures

Over the last decade, discussions on a possible liquid-liquid transition (LLT) have strongly intensified. The LLT proposed by several authors focused mostly on explaining the anomalous properties of water in a deeply supercooled state. However, there have been no direct experimental observations yet of LLT in bulk water in the so-called 'no man's land', where water exists only in the crystalline states. Recently, a novel experimental strategy to detect LLT in water has been employed using water-glycerol (W-G) mixtures, because glycerol can generate a strong hindrance for water crystallization. As a result, the observed first-order phase transition at a concentration of glycerol around c(g) approximate to 20 mol% was ascribed to the LLT. Here we show unambiguously that the first order phase transition in W-G mixtures is caused by the ice formation. We provide additional dielectric measurements, applying specific annealing temperature protocols in order to reinforce this conclusion. We also provide an explanation, why such a phase transition occurs only in the narrow glycerol concentration range. These results clearly demonstrate the danger of analysis of phase-separating liquids to gain better insights into water dynamics. These liquids have complex phase behavior that is affected by temperature, phase stability and segregation, viscositymore » and nucleation, and finally by crystallization, that might lead to significant misinterpretations.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4]
  1. Hebrew Univ. of Jerusalem (Israel). Dept. of Applied Physics; Kazan Federal Univ., Kazan (Russia)
  2. (Gutina), Anna [Hebrew Univ. of Jerusalem (Israel). Dept. of Applied Physics
  3. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry and Joint Inst. for Neutron Sciences; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  4. Hebrew Univ. of Jerusalem (Israel). Dept. of Applied Physics
Publication Date:
OSTI Identifier:
1319195
Grant/Contract Number:
AC05-00OR22725; CHE-1213444
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 17; Journal Issue: 27; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE; Kazan Federal University, Russia; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY