Regenerated Graphite Electrodes with Reconstructed Solid Electrolyte Interface and Enclosed Active Lithium Toward >100% Initial Coulombic Efficiency

Abstract Solid electrolyte interface (SEI) is arguably the most important concern in graphite anodes, which determines their achievable Coulombic efficiency (CE) and cycling stability. In spent graphite anodes, there are already‐formed (yet loose and/or broken) SEIs and some residual active lithium, which, if can be inherited in the regenerated electrodes, are highly desired to compensate for the lithium loss due to SEI formation. However, current graphite regenerated approaches easily destroy the thin SEIs and residue active lithium, making their reuse impossible. Herein, this work reports a fast‐heating strategy (e.g., 1900 K for ≈150 ms) to upcycle degraded graphite via instantly converting the loose original SEI layer (≈100 nm thick) to a compact and mostly inorganic one (≈10–30 nm thick with a 26X higher Young's Modulus) and still retaining the activity of residual lithium. Thanks to the robust SEI and enclosed active lithium, the regenerated graphite exhibited 104.7% initial CE for half‐cell and gifted the full cells with LiFePO 4 significantly improved initial CE (98.8% versus 83.2%) and energy density (309.4 versus 281.4 Wh kg −1 ), as compared with commercial graphite. The as‐proposed upcycling strategy turns the “waste” graphite into high‐value prelithiated ones, along with significant economic and environmental benefits.