ArticleThe journal of physical chemistry letters2026
Free-Energy Profile of Li-Ion Insertion Reaction in Highly Concentrated Electrolytes: Impact of Destabilized Li-Ion on Electrode Reaction Thermodynamics.
Article in The journal of physical chemistry letters, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Understanding the Li-ion insertion reaction at graphite electrodes as a chemical reaction requires a thermodynamic perspective, namely elucidating the underlying free-energy profile. In this study, we quantitatively constructed the free-energy profile of the Li-ion insertion reaction in highly concentrated electrolytes by combining activation thermodynamics derived from electrochemical impedance measurements with experimentally determined solvation free energies of Li+. The resulting free-energy profile revealed that the activation free energy (ΔG⧧) remains nearly constant across different solvent systems, whereas the solvation free energy of Li+ (ΔGLi) varies significantly depending on solvent properties and dominates the thermodynamics of the electrode reaction. Furthermore, high-energy X-ray total scattering and molecular dynamics simulations showed that Li+ forms ion-aggregate structures with anions and solvent molecules, where short-range Li+-Li+ configurations give rise to electrostatic repulsion, leading to destabilization of Li+. These results establish a direct link between solution structure and electrode reaction thermodynamics, providing new insights into the role of Li+ solvation in highly concentrated electrolytes.
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