Short‐Process Regeneration of Highly Stable Spherical LiCoO 2 Cathode Materials from Spent Lithium‐Ion Batteries through Carbonate Precipitation

High‐efficacy recycling of spent lithium cobalt oxide (LiCoO 2 ) batteries is one of the key tasks in realizing a global resource security strategy due to the rareness of lithium (Li) and cobalt (Co) resources. However, it is of great significance to develop the innovative recycle methods for spent LiCoO 2 , simultaneously realizing the efficient recovery of valuable elements and the regeneration of high‐performance LiCoO 2 . Herein, a novel strategy of regenerating LiCoO 2 cathode is proposed, which involves the preparation of micro‐spherical aluminum (Al)‐doped lithium‐lacked precursor (Li 2x Co 1−x−y Al 2/3y CO 3, remarked as “PLCAC”) via ammonium bicarbonate coprecipitation. The comprehensive conditions affecting particle growth kinetics, morphology and particle size the has been investigated in detail by physical characterizations and electrochemical measurements. And the optimized Al‐doped LiCoO 2 materials with high‐density sphericity (LiCo 1−z Al z O 2 , remarked as “LCAO”) shows a high initial specific capacity of 161 mAh g −1 at 0.1 C and excellent capacity retention of 99.5 % within 100 cycles at 1 C in the voltage range of 2.8 to 4.3 V. Our work provides valuable insights into the featured design of LiCoO 2 precursors and cathode materials from spent LiCoO 2 batteries, potentially guaranteeing the high‐efficacy recycling and utilization of strategic resources.