Direct Revival of Spent Graphite Via an Elastic Rippled Carbon Nanoskin for High‐Performance Anodes

ABSTRACT The green and sustainable recycling of spent graphite (SG) is crucial for the circular economy of lithium‐ion batteries (LIBs), yet remains notoriously challenging due to the severe structural degradation and unstable electrode/electrolyte interface. Traditional recycling methods, such as high‐temperature treatment and leaching‐calcination, are often energy‐intensive and environmentally destructive. Herein, a direct and rapid revival strategy with microwave is proposed, which accomplishes the conformal construction of an elastic rippled carbon nanoskin on the surface of SG. The carbon nanoskin effectively repairs the microcracks and defects, and its unique elastic rippled structure accommodates the cyclic volume variation upon lithiation/delithiation, which ensures the stable interface and excellent performance. The regenerated graphite delivers a high initial Coulombic efficiency of 87.57%, a reversible capacity of 370.32 mAh g −1 after 400 cycles at 0.5 C with a capacity retention of 99.86%, and an outstanding rate performance with a capacity of 257.28 mAh g −1 after 450 cycles at 2 C, which is superior to commercial graphite. It also exhibits a notable performance in LiCoO 2 and LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cells. This work reveals a novel mechanistic insight into graphite regeneration through interfacial mechanical protection, offering a scalable and efficient pathway for upcycling spent graphite into advanced anode products.