Strong Oxidizing Molten Salts for Strengthening Structural Restoration Enabling Direct Regeneration of Spent Layered Cathode

Abstract As a mainstream technology for recycling spent lithium‐ion batteries, direct regeneration is rapidly developed due to its high efficiency and green characteristics. However, efficient reuse of spent LiNi x Co y Mn 1‐ x ‐ y O 2 cathode is still a significant challenge, as the rock salt/spinel phase on the surface hinders the Li replenishment and phase transformation to the layered structure. In this work, the fundamental understanding of the repair mechanism is confirmed that the oxidizing atmosphere is the crucial factor that can greatly improve the rate and degree of phase restoration. Particularly, a ternary‐component molten salt system (LiOH‐Li 2 CO 3 ‐LiNO 3 ) is proposed for direct regeneration of LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523), which can in situ generate the strong oxidizing intermediate of superoxide radicals. Additionally, it shows a liquid‐like reaction environment at a lower temperature to acceclerate the transport rate of superoxide‐ions. Therefore, the synergistic effect of LiOH‐Li 2 CO 3 ‐LiNO 3 system can strengthen the full restoration of rock salt/spinel phases and achieve the complete Li‐supplement. As anticipated, the regenerated NCM523 delivers a high cycling stability with a retention of 91.7% after 100 cycles, which is even competitive with the commercial NCM523. This strategy provides a facile approach for the complete recovery of layer structure cathode, demonstrating a unique perspective for the direct regeneration of spent lithium‐ion batteries.