Domain-limited laminar lithium deposition behavior mediated by the design of hybrid anode for sulfide-based all-solid-state batteries

Dendrite growth and the deterioration of anode/electrolyte interface impede the development of all-solid-state Li metal batteries. Tremendous designs of anode have been proposed to tackle these challenges. Herein, considering the issues of solid/solid contact and Li depositing nature, we realize a domain-limited laminar Li deposition by designing a three-dimensional (3D) skeleton supporting hybrid anode with embedded lithiophilic seeds. Specifically, LiC6 particles connect into a skeleton to limit the volume of anode for its sufficient contact with Li6PS5Cl electrolyte. Assisted by extensively dispersed Li22Sn5 inside the hybrid anode, the electrochemical reaction area is expanded to the whole bulk, giving full play to the 3D design of anode. Besides, density functional theory (DFT) calculations confirm that Li22Sn5 functions as lithiophilic seeds to regulate the laminar Li deposition. Ultimately, the hybrid anode exhibits outstanding compatibility towards Li6PS5Cl electrolyte as confirmed by the long lifespan of symmetric cell for 400 h at 0.5 mA cm-2. And a capacity retention of 93.6% is achieved in the full cell with Li2ZrF6 coated LiNi0.9Co0.05Mn0.05O2 cathodes after 50 cycles at 0.1 C. This work paves the way for designing composite metal anode with dynamically stable interface and suppressed Li dendrites for all-solid-state batteries.