3D-printed honeycomb lithium-silicon alloy anodes for stabilized interface in sulfide all-solid-state batteries

Abstract

Solid-state batteries have emerged as a crucial development direction for next-generation energy storage technologies, owing to their high energy density, long cycle life, and excellent safety. However, the most challenging issue of interfacial contact/degradation in solid-state batteries remains unsolved. Herein, a novel Si-C interlocking honeycomb electrode is designed/realized via 3D printing technology. Achieves 98.9 % capacity retention over 2100 cycles at 1C. The honeycomb pore walls form a mortise-tenon structure with the electrolyte to maintain good interfacial contact, while the hard carbon layer isolates the electrolyte from the lithium-silicon interface, thereby stabilizing the growth of the solid electrolyte interphase (SEI) and achieving stress-electrochemical coupling regulation. Moreover, as the honeycomb channels form an interpenetrating structure with the solid electrolyte, a three-dimensional ion transport network is established, shortening the lithium-ion diffusion path, enhancing the interfacial contact between the electrode and solid electrolyte, reducing the risk of lithium dendrite formation, and improving the rate performance of all-solid-state batteries. This approach leverages structural design to enhance material performance, for the first time enabling the compatibility of 3D-printed structured silicon-based anodes with sulfide-based all-solid-state systems, thus providing a scalable solution for next-generation high-energy-density batteries.