Interfacial Metal-Solvent Chelation for Direct Regeneration of LiFePO Cathode Black Mass.

Direct regeneration of spent lithium-ion batteries presents a promising approach to effectively reuse valuable resources and benefit the environment. Unlike controlled laboratory conditions that commonly facilitate impurity purification and minimize structural damage, the LiFePO cathode black mass faces significant interfacial challenges, including structure deterioration, cathode-electrolyte interphase residues, and damage from storage procedures, which hinder lithium replenishment and structure regeneration. Here, a metal-solvent chelation reaction using a lithium acetylacetonate solution is introduced to address these challenges under ambient conditions.

Pathway decisions for reuse and recycling of retired lithium-ion batteries considering economic and environmental functions.

Reuse and recycling of retired electric vehicle (EV) batteries offer a sustainable waste management approach but face decision-making challenges. Based on the process-based life cycle assessment method, we present a strategy to optimize pathways of retired battery treatments economically and environmentally. The strategy is applied to various reuse scenarios with capacity configurations, including energy storage systems, communication base stations, and low-speed vehicles.

Closed-Loop Direct Upcycling of Spent Ni-Rich Layered Cathodes into High-Voltage Cathode Materials.

Facing the resource and environmental pressures brought by the retiring wave of lithium-ion batteries (LIBs), direct recycling methods are considered to be the next generation's solution. However, the contradiction between limited battery life and the demand for rapidly iterating technology forces the direct recovery paradigm to shift toward "direct upcycling." Herein, a closed-loop direct upcycling strategy that converts waste current collector debris into dopants is proposed, and a highly inclusive eutectic molten salt system is utilized to repair structural defects in degraded polycrystalline LiNiCoMnO cathodes while achieving single-crystallization transformation and introducing Al/Cu dual-doping.

Sustainable upcycling of mixed spent cathodes to a high-voltage polyanionic cathode material.

Sustainable battery recycling is essential for achieving resource conservation and alleviating environmental issues. Many open/closed-loop strategies for critical metal recycling or direct recovery aim at a single component, and the reuse of mixed cathode materials is a significant challenge. To address this barrier, here we propose an upcycling strategy for spent LiFePO and Mn-rich cathodes by structural design and transition metal replacement, for which uses a green deep eutectic solvent to regenerate a high-voltage polyanionic cathode material.

Fast Li Replenishment Channels-Assisted Recycling of Degraded Layered Cathodes with Enhanced Cycling Performance and Thermal Stability.

The direct recycling of cathode materials in lithium-ion batteries is important for environmental protection and resource conservation. The key regeneration processes are composition replenishment and atom rearrangement, both of which depend on the migration and diffusion of atoms. However, for the direct recycling of degraded LiNiCoMnO (D-NCM523) cathode, the irreversible phase transitions that accumulate during the long-term cycles block the Li diffusion channels with a high diffusion energy barrier, making it difficult to fully repair the layered structure and resulting in rapid capacity decay.

Toward Direct Regeneration of Spent Lithium-Ion Batteries: A Next-Generation Recycling Method.

The popularity of portable electronic devices and electric vehicles has led to the drastically increasing consumption of lithium-ion batteries recently, raising concerns about the disposal and recycling of spent lithium-ion batteries. However, the recycling rate of lithium-ion batteries worldwide at present is extremely low. Many factors limit the promotion of the battery recycling rate: outdated recycling technology is the most critical one.

Subtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material.

Adding extra raw materials for direct recycling or upcycling is prospective for battery recycling, but overlooks subtracting specific components beforehand can facilitate the recycling to a self-sufficient mode of sustainable production. Here, a subtractive transformation strategy of degraded LiNiCoMnO and LiMnO to a 5 V-class disordered spinel LiNiMnO-like cathode material is proposed. Equal amounts of Co and Ni from degraded materials are selectively extracted, and the remaining transition metals are directly converted into NiCoMn(CO) precursor for preparing cathode material with in-situ Co doping.

Collaborative and privacy-preserving retired battery sorting for profitable direct recycling via federated machine learning.

Unsorted retired batteries with varied cathode materials hinder the adoption of direct recycling due to their cathode-specific nature. The surge in retired batteries necessitates precise sorting for effective direct recycling, but challenges arise from varying operational histories, diverse manufacturers, and data privacy concerns of recycling collaborators (data owners). Here we show, from a unique dataset of 130 lithium-ion batteries spanning 5 cathode materials and 7 manufacturers, a federated machine learning approach can classify these retired batteries without relying on past operational data, safeguarding the data privacy of recycling collaborators.

A Multifunctional Amino Acid Enables Direct Recycling of Spent LiFePO Cathode Material.

Lithium iron phosphate (LiFePO , LFP) batteries are extensively used in electric vehicles and energy storage due to their good cycling stability and safety. However, the finite service life of lithium-ion batteries leads to significant amounts of retired LFP batteries, urgently required to be recycled by environmentally friendly and effective methods. Here, a direct regeneration strategy using natural and low-cost L-threonine as a multifunctional reductant is proposed.

Toward Sustainable All Solid-State Li-Metal Batteries: Perspectives on Battery Technology and Recycling Processes.

Lithium (Li)-based batteries are gradually evolving from the liquid to the solid state in terms of safety and energy density, where all solid-state Li-metal batteries (ASSLMBs) are considered the most promising candidates. This is demonstrated by the Bluecar electric vehicle produced by the Bolloré Group, which is utilized in car-sharing services in several cities worldwide. Despite impressive progress in the development of ASSLMBs, their avenues for recycling them remain underexplored, and combined with the current explosion of spent Li-ion batteries, they should attract widespread interest from academia and industry.

Topotactic Transformation of Surface Structure Enabling Direct Regeneration of Spent Lithium-Ion Battery Cathodes.

Recycling spent lithium-ion batteries (LIBs) has become an urgent task to address the issues of resource shortage and potential environmental pollution. However, direct recycling of the spent LiNiCoMnO (NCM523) cathode is challenging because the strong electrostatic repulsion from a transition metal octahedron in the lithium layer provided by the rock salt/spinel phase that is formed on the surface of the cycled cathode severely disrupts Li transport, which restrains lithium replenishment during regeneration, resulting in the regenerated cathode with inferior capacity and cycling performance. Here, we propose the topotactic transformation of the stable rock salt/spinel phase into NiCoMn(OH) and then back to the NCM523 cathode.

Ultrahigh-Voltage LiCoO at 4.7 V by Interface Stabilization and Band Structure Modification.

Lithium cobalt oxide (LCO) is widely used in Li-ion batteries due to its high volumetric energy density, which is generally charged to 4.3 V. Lifting the cut-off voltage of LCO from 4.

Direct regeneration of degraded lithium-ion battery cathodes with a multifunctional organic lithium salt.

The recycling of spent lithium-ion batteries is an effective approach to alleviating environmental concerns and promoting resource conservation. LiFePO batteries have been widely used in electric vehicles and energy storage stations. Currently, lithium loss, resulting in formation of Fe(III) phase, is mainly responsible for the capacity fade of LiFePO cathode.

Long-Life Regenerated LiFePO from Spent Cathode by Elevating the d-Band Center of Fe.

A large amount of spent LiFePO (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li diffusion.

Adaptable Eutectic Salt for the Direct Recycling of Highly Degraded Layer Cathodes.

Recycling spent lithium-ion batteries (LIBs) is promising for resource reuse and environmental conservation but suffers from complex processing and loss of embedded value of spent LIBs in conventional metallurgy-based recycling routes. Herein, we selected a eutectic LiI-LiOH salt with the lowest eutectic point among binary eutectic lithium salt systems to provide a Li-rich molten environment, not only offering excess lithium but benefiting ion diffusion compared with that in the solid environment. Hence, the highly degraded LiNiCoMnO in spent LIBs which suffers high Li-deficiency and serious structural defects with harmful phase transitions is directly regenerated.

Suppressed Lattice Oxygen Release via Ni/Mn Doping from Spent LiNiMnCoO toward High-Energy Layered-Oxide Cathodes.

LiCoO has suffered from poor stability under high voltage as a result of insufficient Co-O bonding that causes lattice oxygen release and lattice distortions. Herein, we fabricated a high-voltage LiCoO at 4.6 V by doping with Ni/Mn atoms, which are obtained from spent LiNiMnCoO cathode materials.