Lithium is a rare metal because of geographical scarcity and technical barrier. Recycling lithium resource from spent lithium ion batteries (LIBs) is significant for lithium deficiency and environmental protection. A novel approach for recycling lithium element as LiCO from spent LIBs is proposed. First, the electrode materials preobtained by mechanical separation are pyrolyzed under enclosed vacuum condition. During this process the Li is released as LiCO from the crystal structure of lithium transition metal oxides due to the collapse of the oxygen framework. An optimal Li recovery rate of 81.90% is achieved at 973 K for 30 min with a solid-to-liquid ratio of 25 g L, and the purity rate of LiCO is 99.7%. The collapsed mechanism is then presented to explain the release of lithium element during the vacuum pyrolysis. Three types of spent LIBs including LiMnO, LiCoO, and LiCoMnNiO are processed to prove the validity of in situ recycling LiCO from spent LIBs under enclosed vacuum condition. Finally, an economic assessment is taken to prove that this recycling process is positive.

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Spent lithium ion battery (LIB) recovery is becoming quite urgent for environmental protection and social needs due to the rapid progress in LIB industries. However, recycling technologies cannot keep up with the exaltation of the LIB market. Technological improvement of processing spent batteries is necessary for industrial application. In this paper, spent LIB recovery processes are classified into three steps for discussion: gathering electrode materials, separating metal elements, and recycling separated metals. Detailed discussion and analysis are conducted in every step to provide beneficial advice for environmental protection and technology improvement of spent LIB recovery. Besides, the practical industrial recycling processes are introduced according to their advantages and disadvantages. And some recommendations are provided for existing problems. Based on current recycling technologies, the challenges for spent LIB recovery are summarized and discussed from technological and environmental perspectives. Furthermore, great effort should be made to promote the development of spent LIB recovery in future research as follows: (1) gathering high-purity electrode materials by mechanical pretreatment; (2) green metals leaching from electrode materials; (3) targeted extraction of metals from electrode materials.

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