Experimental evidence of co-existence of equilibrium and nonequilibrium in two-glass-transition miscible mixtures
Literature Information
Xiao Jin, Yuxing Guo, Wenkang Tu, Shidong Feng, Yingdan Liu, Thomas Blochowicz, Li-Min Wang
Two glass-transitions have been observed in some miscible molecular mixtures with notable differences in geometry or chemistry of constituents. The explanation of the phenomena has been puzzling with diverse structural models. Here, we present detailed studies on two glass-transition mixtures composed of tripropyl phosphate (TPP) and polystyrene (PS) by using calorimetric and dielectric measurements. We found that ageing between the two transitions always generates endothermic peaks at temperatures ∼4 K higher than the ageing temperatures and, subsequent thermal cycles around the peaks can remove the ageing effect and restore the systems, confirming the co-existence of nonequilibrium and equilibrium states in the regions. We also found that the broad glass transition thermogram is associated with highly stretched relaxation dynamics. The results allow us to draw a conclusion of continuous mobility gradient spanning the two TPP–PS glass-transitions, rather than complete phase separation.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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