Controllable Particle Packing via Scalable Layer-by-Layer Assembly of Anode Particles for Fast-Charging Lithium-Ion Batteries.

Particle packing in battery electrodes is pivotal to the fast-charging performance of lithium-ion batteries (LIBs). However, precise control of particle packing structure remains a major challenge in electrode fabrication, primarily owing to the absence of robust interfacial bonding between micron-scale particles. Herein, we propose a novel layer-by-layer single-layer particle assembly technique to fabricate electrodes with well-defined particle packing structures. Using this approach, we prepared a 12-meter-long graphite (Gr)/hard carbon (HC) hybrid anode featuring a body-centered cubic (BCC)-like structure, which maximizes intimate Gr/HC contact interfaces and facilitates solid-state Li+ transport. Coupled with LiFePO4 (LFP) cathodes, the as-fabricated anode exhibits a high-capacity retention of 80.7% after 1650 cycles at 4C. From an electrode design standpoint, this controllable particle-packing strategy paves the way for a universal framework for developing sustainable, long-cycling, and fast-charging electrodes, potentially applicable to many types of battery anodes and cathodes.