Regulating polystyrene glass transition temperature by varying the hydration levels of aromatic ring/Li+ interaction
Literature Information
Sze Yuet Chin, Yunpeng Lu, Weishuai Di, Kai Ye, Zihan Li, Chenlu He, Chun Tang
Polymer properties can be altered via lithium ion doping, whereby adsorbed Li+ binds with H2O within the polymer chain. However, direct spectroscopic evidence of the tightness of Li+/H2O binding in the solid state is limited, and the impact of Li+ on polymer sidechain packing is rarely reported. Here, we investigate a polystyrene/H2O/LiCl system using solid-state NMR, from which we determined a dipolar coupling of 11.4 kHz between adsorbed Li+ and H2O protons. This coupling corroborates a model whereby Li+ interacts with the oxygen atom in H2O via charge affinity, which we believe is the main driving force of Li+ binding. We demonstrated the impact of hydrated Li+ on sidechain packing and dynamics in polystyrene using proton-detected solid-state NMR. Experimental data and density functional theory (DFT) simulations revealed that the addition of Li+ and the increase in the hydration levels of Li+, coupled with aromatic ring binding, change the energy barrier of sidechain packing and dynamics and, consequently, changes the glass transition temperature of polystyrene.
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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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