Stabilizing Solid Electrolyte Interphase on Liquid Metal via Dynamic Hydrogel‐Derived Carbon Framework Encapsulation

Abstract Eutectic gallium–indium liquid metal (EGaIn‐LM), with a considerable capacity and unique self‐healing properties derived from its intrinsic liquid nature, gains tremendous attention for lithium‐ion batteries (LIBs) anode. However, the fluidity of the LM can trigger continuous consumption of the electrolyte, and its liquid–solid transition during the lithiation/de‐lithiation process may result in the rupture of the solid electrolyte interface (SEI). Herein, LM is employed as an initiator to in situ assemble the 3D hydrogel for dynamically encapsulating itself; the LM nanoparticles can be homogeneously confined within the hydrogel‐derived carbon framework (HDC) after calcination. Such design effectively alleviates the volume expansion of LM and facilitates electron transportation, resulting in a superior rate capability and long‐term cyclability. Further, the “dual‐layer” SEI structure and its key components, including the robust LiF outer layer and corrosion‐resistant and ionic conductive LiGaO x inner layer are revealed, confirming the involvement of LM in the formation of SEI, as well as the important role of carbon framework in reducing interfacial side reactions and SEI decomposition. This work provides a distinct perspective for the formation, structural evolution, and composition of SEI at the liquid/solid interface, and demonstrates an effective strategy to construct a reliable matrix for stabilizing the SEI.