| Abstract Scope |
To enhance the high-rate capability of lithium-ion batteries (LIBs) while maintaining high energy density, dielectric nanointerfaces such as BaTiO₃ (BTO) have been integrated at the electrode–electrolyte interface. This promotes ultrafast charge transfer through the dielectric layer, as confirmed by experiments and DFT-MD simulations. During charging, solvated Li⁺ ions adsorb and desolvate at the dielectric surface before intercalating into the electrode via a triple-phase interface (TPI). BTO nanocubes (~25 nm), with high dispersibility due to oleic acid, significantly improve LiCoO₂ cathode performance. Pulsed-laser deposition (PLD) further enhances TPI density, yielding a 47% increase in 10C-rate capacity compared to sol-gel methods. In lithium-ion capacitors (LICs), BTO-activated carbon composites show a 35% capacity gain. Additionally, optimal charge transfer occurs when the average electronegativity of doped ZrO₂ is ~1.3, indicating that interfacial charge adsorption is governed by electrostatic balance. |