Fast Determination of Lithium Content in Spent Cathodes for Direct Battery Recycling

Abstract

Determination of the lithium ion content in cathode materials, which is currently performed by coupled plasma-mass spectrometry (ICP-MS), involves tedious procedures and error-prone preparation. This work introduces a new methodology to quickly determine the lithium content in spent cathode materials (LiNi x Mn y Co z O 2 , x+y+z=1, NMC) using a thermalgravimetric analysis, which bypasses the use of ICP-MS and significantly reduces the cost and time required for determining the lithium content. Based on this new method, a new approach is developed to identify spent cathode materials suitable for direct relithiation recycling. Finally, these new methods have been applied to investigate the effectiveness of direct electrochemical-relithiation on recycling the spent cathodes, and provide insights for future development of direct battery materials recycling.

The Role of Cycle Life on the Environmental Impact of Li6.4La3Zr1.4Ta0.6O12 based Solid‐State Batteries

“…These materials must be recycled to avoid the generation of hazardous waste, reduce environmental pollution, ensure the availability of lithium sources into the future, and reduce raw material costs. [ 73,74 ] Comparatively, the SSB structure using the LLZTO returns to a reliance on critical REEs, specifically lanthanum. Although the LLZTO is not the only available SSB structure, alternatives such sulphide based systems (Li 4 SnS 4 ‐Li 3 ‐SbS 4 ) [ 75 ] and lithium niobate cathodes with Li 10 GeP 2 S 12 solid electrolytes [ 76 ] also rely on critical materials such as antimony and germanium.…”

Progress in the sustainable recycling of spent lithium‐ion batteries

“…The determination of the Li content is generally carried out by using inductively coupled plasma (ICP) technologies, of which the procedure is quite tedious. Ban and colleagues developed a new methodology to quickly determine the lithium content in spent cathode materials via a thermal gravimetric analysis, facilitating the direct relithiation recycling with a large time and cost save 54 . The similar methods using ionothermal lithiation or a ternary eutectic repair have also been developed recently.…”

Enabling Intelligent Recovery of Critical Materials from Li-Ion Battery through Direct Recycling Process with Internet-of-Things

“…Hydrogen peroxide (H2O2) was added to accelerate the leaching reaction with less acid utilized [54,55]. Organic acids which are more environ- Direct recycling (green line in Figure 2) is to recover, recondition and reintroduce the EOL cathode or anode materials into the supply chain for manufacturing with minimum processing [11,46,63,64]. In theory, everything inside LIBs can be recycled through the direct recycling process including the electrolyte, separator, aluminum, and graphite [63].…”

“…Cathode and anode materials are separated out for their respective regeneration processes. As the main reason for the degradation of the cathode material is the loss of lithium ions, the direct recycling process often uses re-lithiation to restore the electrochemical performance of the cathode [ 64 ]. Direct recycling is found to be the most energy-efficient and cost-effective option among all three types of recycling technologies [ 65 ].…”

“…Prior studies used a machine learning-based prediction model to investigate the optimal ratio of raw material solutions using a combination of X-ray diffraction (XRD) patterns and the experimentally derived characteristics [ 104 ], which provide a helpful use case of a machine learning algorithm in the physical synthesis process. Beyond solid-state sintering, re-lithiation can also be achieved through more complicated methods, such as hydrothermal [ 105 ], electrochemical [ 64 , 106 ], and chemical processes [ 107 ]. The benefits of integrating IoT in direct recycling increase once the methods/processes become more complicated (e.g., involving more steps or more parameters to be monitored) as real-data processing and analysis become more essential tools for process optimization.…”