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Excellent fast-charging performance is a key requirement for lithium-ion batteries intended for automotive applications. Rational particle design for active materials within electrodes represents a strategic approach to minimize kinetic limitationsespecially for the anode, where the lithium intercalation rate affects the overall cell charging capacity at elevated current densities. Typically, for practical applications, natural graphite flakes are shaped into rounded particles via a mechanical spheroidization process. In this work, we show that both surface and bulk particle properties correlate strongly with the applied spheroidization conditions, and directly affect the electrochemical performance, particularly in terms of lithium-intercalation rate. We demonstrate that graphite particles with a surface rich in prismatic planes, structural defects, and oxygen-rich groups are favorable for fast lithium uptake. The influence of the graphite particle characteristics on the lithium intercalation rate plays a key role at the electrode and cell level, affecting the overall cell performance. We provide new insights into particle optimization during spheroidization as an effective strategy for developing fast-charging lithium-ion batteries.

Super‐concentrated electrolyte solutions are of increasing interest for safer and more stable lithium and post‐lithium batteries. The combination of 7Li and 17O (at natural abundance) nuclear magnetic resonance (NMR) and electrochemical characterization is proposed here as an effective approach to investigate the Li+ solvation structures and properties of electrolytes featuring tetraethylene glycol dimethyl ether (TEGDME) and lithium‐bis(trifluoromethane sulfonyl) imide (LiTFSI). Five different formulations from salt‐in‐solvent to solvent‐in‐salt with LiTFSI at different concentrations (0.1 m, 0.5 m, 2 m, 4 m, 5 m) are investigated. The NMR results, also supported by physico‐chemical characterizations such as thermal gravimetric analyses, differential scanning calorimetry, specific conductivity and viscosity, give information about the association of Li+ ions with anion and solvent molecules, allowing a deeper knowledge on the relationships among structure and functional properties of super‐concentrated solutions.