With the rise of the new energy vehicle industry represented by Tesla and BYD, the need for lithium-ion batteries (LIBs) grows rapidly. However, owing to the limited service life of LIBs, the large-scale retirement tide of LIBs has come. The recycling of spent LIBs has become an inevitable trend of resource recovery, environmental protection, and social demand. The low added value recovery of previous LIBs mostly used traditional metal extraction, which caused environmental damage and had high cost. Beyond metal extraction, the upcycling of spent LIBs came into being. In this work, we have outlined and particularly focus on sustainable upcycling technologies of toxic electrolyte, cathode, and anode from spent LIBs. For electrolyte, whether electrolyte extraction or decomposition, restoring the original electrolyte components or decomposing them into low-carbon energy conversion is the goal of electrolyte upcycling. Direct regeneration and preparation of advanced materials are the best strategies for cathodic upcycling with the advantages of cost and energy consumption, but challenges remain in industrial practice. The regeneration of advanced graphite-based materials and battery-grade graphite shows us the prospect of regeneration of anode. Furthermore, the challenges and future development of spent LIBs upcycling are summarized and discussed from technological and environmental perspectives.
Keywords: Advanced upcycling; Cathode; Direct regeneration; Electrolyte; Graphite; Spent lithium-ion batteries; Sustainability evaluation.