Topologically Robust New Silica Phase Decoupling Intrinsic Zero‐Strain Feature and High‐Capacity Li ⁺ Storage

ABSTRACT

Conventional silicon‐based anodes present high specific capacity but show huge volume expansion, whereas the zero‐strain anodes generally show low specific capacity, presenting the zero‐strain and capacity paradox. Here, inspired by the typical zero‐strain anodes (such as Li ₄ Ti ₅ O ₁₂ ) and the high specific capacity of silicon‐based anodes, we report a new topologically robust silica phase (TRS) that enables an intrinsic zero‐strain feature with high lithium‐ion storage performance by fundamentally decoupling capacity from volume expansion. TRS features rigid Si‐O bonds with large topological rings, providing sufficient internal space and mechanical robustness to accommodate numerous lithium‐ions and achieving an intrinsic zero‐strain feature simultaneously. Comprehensive in‐situ transmission electron microscope (TEM), in‐situ Raman and in‐situ X‐ray diffraction (XRD) confirm its zero‐strain nature, exhibiting constant phase and lattice parameters during (de)lithiation, and revealing reversible lithium‐ion solid‐solution storage. The TRS anode delivers a high reversible capacity and energy density, which are higher than those of typical reported zero‐strain and graphite anodes, and maintains exceptional cycling stability. This topological structural strategy provides a new paradigm for designing next‐generation anodes with zero‐strain and high lithium‐ion storage performance.