Owing to the increasing pressure on the ecological effect of solid waste disposal and developing the need for disposal of the corresponding hazardous metals, recovery of spent lithium ion batteries (LIBs) has gain worldwide attention in recent years. Much work has been done in this regard in the past few decades, and several new, interesting, and unique methods have been developed to recycle the cathode, anode, and electrolyte. Therefore, time has come to summarize the highlights in this emerging area to facilitate young researchers. In this review, starting from the current market demand and commercial value of lithium ion batteries, we have summarized the most recent progress in the direction of recycling the cathode and anode materials and electrolyte. At the beginning, an overview of the recycling techniques is presented to grasp understanding of the topic. Later, laboratory and industrial investigations and implementation are reviewed with emphasis on anode (graphite) and electrolyte recovery. Life cycle assessment of end-of-life LIB recycling, limitations, and future efforts have also mentioned to focus on improving the efficiency of metal extraction and separation with the sustainable and systematic recycling of spent lithium ion batteries.
With the rapid growth of retired lithium-ion batteries (LIBs), the recycling of electrode materials has become a hot topic in research. Considering the economic factors, the recovery of cathode electrodes has always been the focus of research. Until now, the recovery of anode electrode materials has gained much attention due to their large proportion in batteries. This research focuses on the recovery and regeneration of anode graphite. Based on the existing form of lithium in anode graphite carbon powder, environmentally friendly citric acid is selected as the extraction reagent to extract lithium and regenerate spent graphite. Through orthogonal experiments and conditional experiments, the optimal conditions for extracting the lithium element from the spent LIB anodes were a temperature of 90 °C, S/L ratio of 1:50 g mL–1, C AC of 0.2 mol L–1, and time of 50 min, and the leaching rate of lithium ions can reach 97.58%. The electrochemical performance tests showed that the regenerated graphite anode material after the extraction of lithium had a high discharge capacity of 330 mA h g–1 after 80 cycles at 0.5 C, and the Coulombic efficiency is maintained above 99%. By comparing the regenerated graphite and the pretreated spent graphite, the regenerated leached graphite has obviously excellent electrochemical performance, and its properties can be comparable to those of artificial graphite. This experimental result provides a theoretical basis for the subsequent recycling of anode electrode graphite.
Considering the shortage and toxicity of raw materials, recycling cathode materials from spent lithium-ion batteries is currently the most promising measure to realize the green sustainability of cathode materials. Presently, most hydrometallurgical recovery methods and some cathode material synthesis methods are based on the use of acidic solutions. This study addresses the dissolution−chelation mechanism and limitations of the LiNi 1/3 Mn 1/3 Co 1/3 O 2 cathode materials in acidic solution, aiming at highlighting the interface reaction mechanism. In this work, malonic acid and hydrogen peroxide were used as the leaching system to conduct efficient green leaching of spent ternary cathode materials. The effects of different reaction parameters on the recovery efficiency of various valuable metal ions were studied by orthogonal and single-factor condition experiments. The results show that under the optimal conditions the leaching efficiency of the lithium ion is 95%, and the leaching efficiencies of Ni, Co, and Mn all reached over 98%. The dissolution mechanism was studied at the macro-and microscales based on the material characterization technology, kinetic studies, and the theoretical calculations of the binding energy of the possible product. Kinetic studies found that the dissolution−chelation process is controlled by chemical reactions or a chemical and diffusion reaction, and calculation results of the activation energy and binding energy show that lithium ions are leached preferentially over other metal ions. In addition, this recovery technology can be effectively used to recycle other spent rechargeable battery materials and may also lay a theoretical foundation for further study on the regeneration and resynthesis of materials.
Dendrite formation severely compromises further development of zinc ion batteries. Increasing the nucleation overpotential plays a crucial role in achieving uniform deposition of metal ions. However, this strategy has not yet attracted enough attention from researchers to our knowledge. Here, we propose that thermodynamic nucleation overpotential of Zn deposition can be boosted through complexing agent and select sodium L-tartrate (Na-L) as example. Theoretical and experimental characterization reveals L-tartrate anion can partially replace H2O in the solvation sheath of Zn2+, increasing de-solvation energy. Concurrently, the Na+ could absorb on the surface of Zn anode preferentially to inhibit the deposition of Zn2+ aggregation. In consequence, the overpotential of Zn deposition could increase from 32.2 to 45.1 mV with the help of Na-L. The Zn-Zn cell could achieve a Zn utilization rate of 80% at areal capacity of 20 mAh cm−2. Zn-LiMn2O4 full cell with Na-L additive delivers improved stability than that with blank electrolyte. This study also provides insight into the regulation of nucleation overpotential to achieve homogeneous Zn deposition.
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