Precise regulation of layered-to-rock structure of spent Li-ion cathodes achieving ultrahigh lithium recovery rate

With the rapid development of electric vehicles and digital devices, the accumulated spent lithium-ion batteries (LIBs) cause severe anxiety about lithium resources and environmental safety. However, the low capture rate of Li⁺ and the high chemical consumption of the existing recovery methods lead to high Li loss, treatment costs and disposal fees. Herein, we propose a universal strategy of spent LIBs recovery via precise directional regulating structures (from layered to rock) to achieve ultrahigh lithium recovery rate with super-low chemical and energy consumption. Experimental characterization and theoretical calculations reveal the dissociation of structure, reorganization of Li–O bonds and phase transformation of the cathode materials in the limited-domain reduction process, realizing the complete recovery of Li⁺ without consuming acid leaching agent. This process realizes an extra-high Li separation index (19154) and extra-long cycle half-life (173 cycles) which are far superior to those of traditional methods (9–191 and 7 cycles). Besides, ecological and economic analysis shows that the consumptions of chemicals and energy are only 9 % and 9.7 % those of the existing literature, respectively, providing a bright pathway for industrializable lithium batteries recycling.