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With the rising demand for lithium-ion batteries (LIBs), it is crucial to develop recycling methods that minimize environmental impacts and ensure resource sustainability. The focus of this short review is on the electrochemical techniques used in LIB recycling, particularly electrochemical leaching and electrodeposition. Our summary covers the latest research, highlighting the principles, progress, and challenges tied to these methods. By examining the current state of electrochemical recovery, this review intends to provide guidance for future advancements and enhance LIB recycling efficiency. [ABSTRACT FROM AUTHOR]

Lithium‐ion battery cathode materials suffer from bulk and interfacial degradation issues, which negatively affect their electrochemical performance. Oxide coatings can mitigate some of these problems and improve electrochemical performance. However, current coating strategies have low throughput, are expensive, and have limited applicability. In this article, we describe a low‐cost and scalable strategy for applying oxide coatings on cathode materials. We report synergistic effects of these oxide coatings on the performance of aqueously processed cathodes in cells. The SiO2 coating strategy developed herein improved mechanical, chemical, and electrochemical performance of aqueously processed Ni‐, Mn‐ and Co‐based cathodes. This strategy can be used on a variety of cathodes to improve the performance of aqueously processed Li‐ion cells. [ABSTRACT FROM AUTHOR]

The emergence and dominance of lithium-ion batteries in expanding markets such as consumer electronics, electric vehicles, and renewable energy storage are driving enormous interests and investments in the battery sector. The explosively growing demand is generating a huge number of spent lithium-ion batteries, thereby urging the development of cost-effective and environmentally sustainable recycling technologies to manage end-of-life batteries. Currently, the recycling of end-of-life batteries is still in its infancy, with many fundamental and technological hurdles to overcome. Here, the authors provide an overview of the current state of battery recycling by outlining and evaluating the incentives, key issues, and recycling strategies. The authors highlight a direct recycling strategy through discussion of its benefits, processes, and challenges. Perspectives on the future energy and environmental science of this important field is also discussed with respect to a new concept introduced as the Battery Identity Global Passport (BIGP). [ABSTRACT FROM AUTHOR]

Separation of electrode materials from their current collectors is an enabling step toward recovering critical materials from spent lithium‐ion batteries. In the presented research, a highly efficient, cost‐effective, and environmentally sustainable separation process was developed for that purpose. Ethylene glycol, a vital commodity chemical as an antifreeze and polymer precursor, is used to delaminate electrode materials at low temperatures in seconds without altering the crystalline structure and morphology of active electrode materials. The recovered current collectors were intact without any corrosion. The authors also found that the solvent could be continuously reused, leading to the development of a closed‐loop ecosystem and lithium‐ion battery circular economy. The ultrafast delamination was driven by the competitive inhibition of binding through the weakening of hydrogen bonding. The ethylene glycol‐based separation is a sustainable electrode recovery process that paves the way for battery recycling. [ABSTRACT FROM AUTHOR]

The growing global trend toward mobile electrification is primarily driven by the rising popularity of electric vehicles, leading to an unprecedented surge in demand for lithium-ion batteries. As a result, the importance of battery recycling has become increasingly apparent. Battery recycling aims to recover valuable materials from both spent batteries and battery manufacturing scraps. By recycling these resources, the reliance on raw material extraction is reduced, which benefits resource conservation and minimizes the need for new mining operations. While significant attention has been given to the recycling of spent batteries, less emphasis has been placed on the recycling and recovery of battery scraps. However, it is important to recognize that many gigafactories are still taking steps to improve their manufacturing processes, and end-of-life batteries take approximately 10 years to become suitable for recycling, the manufacturing scraps will serve as the primary sources for recycling in this decade. This review delves into the progress in recycling technologies associated with battery manufacturing scraps, shedding light on the challenges, opportunities, and evolving perspectives surrounding battery manufacturing scrap recycling. We aim to contribute to the knowledge base of battery manufacturing scrap recycling and promote a more comprehensive understanding of the subject. • Definitions of spent batteries and battery manufacturing scraps specified. • Comprehensive evaluation of battery manufacturing scraps for battery recycling. • In-depth analysis of the generation of battery manufacturing scraps. • Critical review of the present research on battery manufacturing scrap recycling. • Outlook on the challenges and perspectives for battery manufacturing scrap recycling. [ABSTRACT FROM AUTHOR]

To recycle high-value lithium-ion battery components, it is imperative to efficiently separate electrode materials from current collector foils and to separate cathodes from anodes. This study investigates the delamination behaviors of cathodes and anodes from their respective current collectors in aqueous media. Whereas anode films can easily detach from copper foils in water, the delamination of cathode films does not exhibit the same behavior in water; instead, the cation exchange reaction results in lithium leaching and aluminum corrosion in the presence of water. A buffer solution with surfactant additives has been designed to prevent aluminum corrosion and to improve solution wetting behavior, thereby facilitating cathode delamination. The delamination difference enables the sequential recovery of electrode materials and metal foils at different separation stages, simplifying the traditionally intricate processes within a one-pot recovery system. The recovered materials retain their crystal structure and morphology, and there are no signs of aluminum corrosion or residues on the metal foils. The sequential separation technique achieves nearly 100% separation efficiency for electrode materials from metal foils and over 98% separation efficiency for cathode and anode materials. • Complete anode-copper separation: achieved 100% delamination efficiency. • Buffer and surfactant prevent aluminum corrosion and enhance cathode delamination. • One-pot recovery: streamlined electrode/metal and anode/cathode separation process. • Material integrity retained: Crystal structure preserved; no corrosion observed. • Sustainable recycling: aqueous method for high-efficiency component reclamation. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries (LIBs) have revolutionized portable electronics and electric vehicles (EVs), but the growing accumulation of end-of-life (EOL) batteries poses environmental challenges. Recycling high-value cathodes from EOL LIBs can minimize waste and reduce the need for mining critical minerals. This study focuses on the direct recycling of Ni-rich cathodes, particularly lithium-manganese-cobalt-oxide (NMC) 622 in a "reciprocal ternary molten salts (RTMS)" system. The ionothermal relithiation in the RTMS system successfully restores the layered structure, lithium content, and electrochemical performance of the NMC 622 cathode, comparable to the pristine material. The cost analysis reveals that cathode regeneration through ionothermal relithiation is more economical than virgin production or conventional recycling methods. • A "reciprocal ternary molten salts" (RTMS) system for direct battery recycling. • Directly recycling of spent Ni-rich cathodes by topotactic reactions in RTMS. • A low cost and highly efficient direct recycling process for spent Li-ion batteries. [ABSTRACT FROM AUTHOR]

Improving the fast charging performance of lithium ion batteries (LIBs) has the promise to increase the widespread adoption of electric vehicles (EVs). Electrolyte development plays an important role in enabling fast charging. In this study, fast charging performance of LIBs is studied with different electrolytes of 1.2 M LiPF 6 in Ethylene Carbonate (EC)/Ethyl Methyl Carbonate (EMC)/co-solvents at 30/50/20 wt%. The co-solvents are methyl acetate (MA), ethyl acetate (EA), ethyl formate (EF), dimethyl carbonate (DMC) and EMC. Long term cycling performance under fast charging shows different capacity retention behaviors for different co-solvents. The structural changes in the electrode material are studied by X-ray absorption spectroscopy (XAS) and X-ray diffraction (XRD). The molarity changes in electrolyte is investigated by inductively coupled plasma-optical emission spectroscopy (ICP-OES). The electrode/electrolyte interfaces before and after fast charging are analyzed by X-ray photoemission spectroscopy (XPS). The characterization results are in good agreement with the long-term cycling performance. DMC shows the highest fast-charging capability among the five studied co-solvents due to its increased conductivity, improved electrode/electrolyte interface and stable electrode structural integrity. [ABSTRACT FROM AUTHOR]

Enabling aqueous processing for lithium-ion battery cathodes is essential as solvents like N-methyl-2-pyrrolidone (NMP) are expensive, hazardous, and being phased out of usage around the world. Using water as a solvent can reduce electrode manufacturing cost and environmental impact, but it presents unique challenges for cathodes such as Li and transition metal dissolution from the active material and current collector corrosion. In this study, the suitability of aqueous processing for five cathode active materials is evaluated: LiCoO 2 (LCO), LiFePO 4 (LFP), LiMn 2 O 4 (LMO), LiNi 0.80 Co 0.15 Al 0.05 O 2 (NCA), and LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC532). After three days of water exposure, NCA and NMC532 exhibit significantly greater pH values (11.5–12.5) than the Ni-free materials (9.0–10.5), though all pH values suggest corrosion of the Al substrate would occur. Surface compositions change to various extent while little change is observed in the crystal structures. The transition metal dissolution in water and electrolyte is relatively low for all materials, though the Li dissolution in water is high for NCA (~0.1 mg mL−1). Electrochemical testing in half coin cells reveals that high-molecular weight polyacrylic acid addition is able to modify the pH and provide adequate binding to the current collector to permit aqueous processing of NCA. • Corrosion of Al current collector is predicted for all five active materials tested. • Interactions between active materials and water are limited to the surface. • Compared to Li, transition metal dissolution is benign. • pH needed to be modified to fabricate aqueous-processed NCA cathode. • Aqueous processing of NCA is achievable through addition of high-MW PAA. [ABSTRACT FROM AUTHOR]

Scalable and sustainable production of high voltage cathodes is required to meet the increasing demands for Li-ion batteries. Additionally, the anticipated scarcity of critical materials like cobalt necessitates demonstration of Co-free alternatives that can match the performance metrics of conventional cathodes. Herein, a hydrothermal synthesis route for production of a new class of high-capacity, cobalt-free cathode material, LiNi 0.9 Mn 0.05 Al 0.05 O 2 (NMA9055) for next-generation Li-ion batteries is reported. The synthesized cathode material shows high crystallinity and purity with monodispersed spherical morphology. Extensive electrochemical, structural, and post-mortem characterization of this novel NMA material is carried out. NMA-Li half cells show an initial discharge capacity of 200 mAh/g with a 96% capacity retention over 100 cycles when cycled between 3.0 and 4.4 V. On the other hand, NMA full cells with Li 4 Ti 5 O 12 (LTO) electrodes as the anode, show an initial discharge capacity of 186 mAh/g with 81% capacity retention over 200 cycles. Post-mortem structural and morphological characterization show that the NMA morphology and crystal structure do not degrade significantly over 200 charge/discharge cycles. This new class of cobalt free cathode material containing nickel, manganese and aluminum synthesized by an ammonia-free synthesis route is expected to provide a facile solution towards sustainable cathode production. • Hydrothermal method to synthesize LiNi 0.9 Mn 0.05 Al 0.05 O 2 (NMA) cobalt-free cathode. • High crystallinity and spherical morphology achieved by ammonia-free process. • NMA half cells show 200 mAh g−1 capacity with 96% capacity over 100 cycles. • NMA-LTO full cells shows capacity of 186 mAh g−1 with 81% retention over 200 cycles. • Extensive in-situ and ex-situ characterization performed to study the material. [ABSTRACT FROM AUTHOR]

Recently, rapid fluctuations in cobalt prices have created a worsening supply chain constraint that has become a serious cause of concern amidst global battery manufacturers. To address this challenge, here we report a new class of cobalt-free, nickel-rich layered cathode material termed the NFA class with general formula LiNi x Fe y Al z O 2 (x + y + z = 1). Using co-precipitation reaction in a continuous stirred tank reactor, we synthesized NFA(OH) 2 precursors with the constituent Ni, Fe and Al elements successfully incorporated. The obtained LiNFAO 2 cathode was characterized using X-Ray diffraction, Mössbauer spectroscopy and scanning electron microscopy. Electrochemical behavior was assessed using cyclic voltammetry, galvanostatic charge/discharge, electrochemical impedance spectroscopy and galvanostatic intermittent titration technique at various states of lithiation/delithiation. Electrochemical performance evaluations revealed that our cobalt-free material delivers high capacity of 190 mAh/g at 0.1C. Rate and cycling performance evaluations also indicated good rate capability and cycling stability with 88% capacity retention after 100 cycles at C/3. Using NFA cathodes, we also fabricated a 0.5Ah (C/3) cobalt-free Li-ion battery which demonstrated reasonable cycling stability with ~72% capacity retained after 200 cycles. Overall, our work demonstrates the immense potential of the cobalt-free NFA class cathodes as viable candidates towards development of next generation cost effective lithium ion batteries. Image 1 • Introducing a new class of cobalt-free, nickel-rich layered cathode (LiNi x Fe y Al z O 2). • Our cobalt-free cathode powders were synthesized using co-precipitation process. • Our cobalt-free cathodes delivered high capacities ~190 mAh/g at 0.1C. • We also fabricated a 0.5 Ah (C/3) cobalt-free Li-ion battery pouch cell. • The cobalt-free battery delivered good capacities and cycling performance. [ABSTRACT FROM AUTHOR]