Highly efficient selective recovery of lithium from spent lithium-ion batteries by thermal reduction with cheap ammonia reagent.

The rapid development of new energy technology leads to explosive growth of lithium-ion batteries (LIBs) industry which greatly alleviates the problems of environmental pollution and energy shortage. However, how to realize resource circulation of critical metals including lithium (Li) and cobalt (Co) becomes the new problem of LIBs industry. This paper proposes an improved thermal reduction technology to efficiently recycle Li and Co from spent LIBs, where cheap urea is applied as the only additive to provide ammonia (NH3). By thermal reduction, LiCoO2 was thermally reduced into water-soluble lithium carbonate and water-insoluble cobalt metal Under the optimal conditions, 99.96% Li with nearly 100% selectivity was obtained by water leaching. More importantly, the concept of "oxygen elements removal (OER)" was proposed to explain the metal extraction from spent LIBs, which could help to describe the reaction mechanism as O-cage digestion mechanism. Furthermore, metal extraction from spent LIBs was re-understood as "seeking an applicable reductant", which provided a fresh perspective for understanding Li selective recovery. These concepts and findings can provide some inspiration for metal recovery from spent LIBs.