Surface‐Anchored Nanoparticles Enable Electrode ζ‐Potential Control: Modulating Electrolyte Solvation to Form Inorganic‐Rich CEI for High‐Voltage Lithium‐Ion Batteries

The electrolyte, as the medium for charge transport, is critical to the stable cycling of lithium-ion batteries. However, severe electrolyte decomposition hinders the widespread adoption of high-voltage cathodes. Enhancing electrolyte stability and constructing a robust cathode-electrolyte interface (CEI) are therefore essential. In this study, it demonstrates that anchoring metal oxide nanoparticles with positive ζ potentials (zeta potential) on the cathode surface effectively modulates the solvation environment of ions at the electrode-electrolyte interface. This modulation alters ion distribution at the interface, promoting the formation of a stable, inorganic-rich CEI. When applied to a conventional LiNi_0.5Mn_1.5O₄ (LNMO) high-voltage cathode, the surface-anchored nanoparticles (SAN) strategy suppresses parasitic side reactions, prevents Mn²⁺ dissolution, and improves cycling stability when paired with conventional carbonate electrolytes across wide electrochemical windows. This study presents a novel approach for designing the cathode-electrolyte interface, advancing the practical application of high-voltage lithium-ion batteries.