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Given the rising lithium-ion battery retirement trend, there is a pressing need for a sustainable, cost-effective, versatile, and industrially viable positive active powder reprocessing method. The current treatment methods require significant amounts of acids, reducing agents, and other additives, resulting in increased treatment expenses and detrimental environmental consequences. This paper proposes a synergistic redox strategy, based on thermodynamic calculations of potential self-promoting reactions in mixed LFP/NCM systems, for the recovery of spent LFP and NCM batteries without the need for additional agents in a milder acidic atmosphere. In this cooperative redox strategy, the spontaneous extraction and oxidation of Fe2+ to Fe3+ took place within the acidic solution atmosphere encapsulating LFP. Simultaneously, NCM underwent further reduction, yielding Ni2+ and Fe2+, thereby enabling the proficient dissolution and segregation of lithium and transition metal ions. The leaching rate of lithium, nickel, cobalt and manganese was close to 100% when the reaction was carried out at 20 °C for 40 min. The final raw material was reprepared into a battery with a capacity of 168.8 mA h g−1 at 1C, and the cycle retention rate was 76.78% after 300 cycles. Regenerating FPO into LFP cathode material achieves closed-loop recycling of all elements and generates 12% higher profits compared to separate processes. Our method proposes a zero-additive battery recycling process and successfully explains the intrinsic redox process. [ABSTRACT FROM AUTHOR]

With the increasing use and the consequent retirement of lithium-ion batteries (LIBs), there has been an upsurge in spent LIBs, posing significant challenges to energy, resources, and the environment, which has led to the necessity to recycle spent LIBs. For the recovery of valuable components in cathode materials, traditional hydrometallurgical and pyrometallurgical methods are not conducive to the sustainable development of the environment, making it crucial to explore lithium-ion battery (LIB) recovery technologies beyond traditional methods. This paper focuses on introducing intensification technologies that are beyond the traditional methods, including external field intensification technologies (in the fields of acoustics, optics, electricity, and magnetism), novel solvent-based intensification technologies, direct recovery technologies, and potential development technologies. From the perspective of process intensification, the process flow, principle, effect, and scope of application of various recovery technologies are systematically summarized. Furthermore, the advantages of these advanced recovery methods and the current challenges faced by them are discussed to propose the potential research direction of the recovery technology of lithium-ion battery cathode materials, which is of significant importance for the sustainable development of the global new energy industry, the maintenance of ecological balance, and the circular utilization of mineral resources, such as lithium, nickel, and cobalt. [ABSTRACT FROM AUTHOR]

A facile mechanical mixing‐calcination method was employed to coat lithium metaborate onto LiNi0.88Co0.06Mn0.03Al0.03O2 cathode. Physical characterizations revealed that the coating layer was uniformly spread on the surface of the material particles, and did not alter the structure and morphology. Electrochemical measurements indicated that the surface‐modified cathode showed significantly improved cycling stability, both under room‐temperature and high‐temperature (50 °C). The coated sample delivered an initial discharge capacity of 211.0 mAh g−1 at 0.1 C, and a capacity retention of 87.5 % after 300 cycles at 1 C rate under room‐temperature. Meanwhile, it could maintain 97.2 % of initial capacity after 120 cycles at 1 C under 50 °C, which was much higher than the value of the pristine sample (only 37.2 %). The lithium‐ion diffusion kinetics was analyzed by electrochemical impedance spectroscopy. The coated material exhibits lower surface resistance and charge‐transfer resistance, as well as faster lithium‐ion diffusion than the pristine one. The materials were also characterized after cycling. The surface‐modified sample possessed more stable surficial and structural stability. [ABSTRACT FROM AUTHOR]

High nickel content in LiNixCoyMnzO2 (NCM, x ≥ 0.8, x + y + z = 1) layered cathode material allows high specific energy density in lithium-ion batteries (LIBs). However, Ni-rich NCM cathodes suffer from performance degradation, mechanical and structural instability upon prolonged cell cycling. Although the use of single-crystal Ni-rich NCM can mitigate these drawbacks, the ion-diffusion in large single-crystal particles hamper its rate capability. Herein, we report a strategy to construct an in situ Li1.4Y0.4Ti1.6(PO4)3 (LYTP) ion/electron conductive network which interconnects single-crystal LiNi0.88Co0.09Mn0.03O2 (SC-NCM88) particles. The LYTP network facilitates the lithium-ion transport between SC-NCM88 particles, mitigates mechanical instability and prevents detrimental crystalline phase transformation. When used in combination with a Li metal anode, the LYTP-containing SC-NCM88-based cathode enables a coin cell capacity of 130 mAh g−1 after 500 cycles at 5 C rate in the 2.75-4.4 V range at 25 °C. Tests in Li-ion pouch cell configuration (i.e., graphite used as negative electrode active material) demonstrate capacity retention of 85% after 1000 cycles at 0.5 C in the 2.75-4.4 V range at 25 °C for the LYTP-containing SC-NCM88-based positive electrode. Single-crystal Ni-rich cathodes suffer from side reactions with the electrolyte and slow Li-ion transport during high-voltage cycling. Herein, a Li1.4Y0.4Ti1.6(PO4)3 coating is applied to facilitate the Li-ion transport and improve the cycling life of the cell. [ABSTRACT FROM AUTHOR]

Abstract The nanosized LiMnPO 4 ·Li 3 V 2 (PO 4) 3 /carbon/graphene (LMP·LVP/C/G) composite is synthesized via a sol-gel method combined with freeze-drying. It is revealed that the composite is consisted of monoclinic Li 3 V 2 (PO 4) 3 and orthorhombic olivine-type LiMnPO 4 , which are homogeneously distributed in this mixture. While the LMP·LVP nanoparticles are intimately wrapped by a thin carbon layer. Particularly, the graphene nanosheets are closely coating on the LMP·LVP/C particles and constructing a highly conductively network, which exert significantly influence on the particle morphology with nanosize and rate capability with excellent performance for LMP·LVP/C/G composite. Due to the smaller polarization and higher Li+ diffusion induced by this hierarchical structure, the LMP · LVP/C/G composite delivers 116.3 mAh g−1 at ultrahigh rate of 10C, and ultrolong cycling life with capacity retention of 85.2% after 500 cycles. The synergistical effect between LMP·LVP and dual carbon wrapping with well-designed hierarchical structure provides an effective strategy to improve Li+ intercalation performance for cathode materials. Graphical abstract Image 1 Highlights • LMP·LVP/C/G composite is synthesized by a facile and scalable method. • Mutual doped LMP·LVP nanoparticles are coated by carbon and embedded in rGO nanosheets. • LMP·LVP/C/G composite delivers small polarization and high conductivity. • LMP·LVP/C/G composite presents ultrahigh rate capability and long cycling stability. [ABSTRACT FROM AUTHOR]

[Display omitted] • Ni-rich cathode material coated with a dual conductive layer is designed and synthesized. • The dual coating layer was composed of V 2 O 5 particles anchored on rGO sheets. • V 2 O 5 could facilitate the diffusion of Li+ and reduce surface lithium residuals. • rGO could facilitate the transfer of electrons. • The designed cathode material exhibited excellent electrochemical performances. Nickel-rich material has the advantages of high energy density and low cost, so it is an attractive cathode material. However, the defects such as fast capacity drop and low capacity at high rates hinder its commercial application. Herein, to solve the problems and obtain nickel-rich material with high performance, a novel dual conductive layer is designed and coated on the surface of LiNi 0.84 Co 0.11 Mn 0.05 O 2 material. The uniform hybrid coating layer is composed of vanadium pentoxide (V 2 O 5) and reduced graphene oxide (rGO). The V 2 O 5 could facilitate the Li+ intercalation/deintercalation process of the nickel-rich cathode material and stabilize its layered structure after reacting with surface lithium residuals, and the rGO with excellent electronic conductivity is helpful to facilitate the transfer of electrons. Therefore, the V 2 O 5 /rGO hybrid coating layer not only prevents the surface against corrosion by electrolyte, but also improves the electronic and ionic conductivity of the material. The results showed that the cycling and rate performances of the designed material are more superior than those of the pristine material. The designed material performed an outstanding capacity of 145.7 mAh g−1 at 10 C, and the capacity retention was 90.43% at 1 C after 100 cycles, which is much higher than the pristine material. This work provides an effective strategy for improving the electrochemical performances of nickel-rich cathode materials. [ABSTRACT FROM AUTHOR]

The treatment of spent lithium-ion batteries has become an urgent issue along with the explosive growth of consumption. Traditional metallurgical technologies can recover lithium and other valuable elements in LiFePO 4 , yet existing various disadvantages to be solved, such as long acid leaching process and harsh reaction conditions. Herein, a delicate method of recycling waste LiFePO 4 via a "feed three birds with one scone" strategy is developed and regenerated as the advanced cathode material. Particularly, it effectively separates the three materials, aluminum foil, lithium-contain compound and high-purity FePO 4 , via one-step oxidation leaching reaction at room temperature. The leaching rate of Li exceeds 98% by adding ammonium persulfate, which is facilitated to obtain transformed lithium carbonate and high-purity precursor FePO 4. The reaction mechanism of oxidation leaching process is analyzed through kinetic and thermodynamic analyses, which believe that the leaching reaction of oxidation is controlled by an ion diffusion. Meanwhile, the recycled Li 2 CO 3 and FePO 4 are utilized as raw materials to synthesize LiFePO 4 cathode, making the utmost advantages of waste LiFePO 4 electrode. As anticipated, the regenerated LiFePO 4 displays excellent rate capability (discharge capacity of 135.5 mAh g−1 at 1C) and cyclic properties (capacity retention of 98.0% after 400 cycles). This green and effective method can efficiently recycle waste LiFePO 4 electrodes and inspire the regeneration of electrode materials from spent lithium-ion batteries. [Display omitted] ● It is an effective strategy to recycle waste lithium-ion battery and resynthesize LiFePO 4 cathode. ● FePO 4 , lithium-contain compound and aluminum foil are simultaneously separated by one step. ● The leaching efficiency of lithium is up to 98.1% at normal temperatures and pressures. [ABSTRACT FROM AUTHOR]

The porous spherical LiFePO 4 ·LiMnPO 4 ·Li 3 V 2 (PO 4) 3 @C@rGO (Sample-G) composites are prepared via a spray drying process. The results show that the composites consist of orthorhombic olivine-type LiFe 0.5 Mn 0.5 PO 4 and monoclinic Li 3 V 2 (PO 4) 3 , which are evenly distributed. In particular, nanoparticles are embedded in graphene nanosheets, which are interconnected and stacked to form a porous sphere structure with an interior three-dimensional conductive network, resulting in the huge improvement on electrochemical performance and structural stability. Due to the increased Li+ diffusion coefficient, the composite possesses 98.6 and 82.9 mAh g−1 with capacities retention of 81.6% and 71.8% at 10 and 20C after 1000 cycles, respectively. The mutual cross-doping effect between LFP·LMP·LVP and a porous sphere structure with a 3D conductive network inside provides a practical method for improving the cycling and rate performance. [ABSTRACT FROM AUTHOR]

In order to enhance the electrochemical properties of nickel-rich LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode material, lithium-ion conductor shell was coated on the surface of the material through a facile wet chemical route. The morphologies, structures and chemical compositions of the samples were characterized by scanning electron microscope, transmission electron microscope, X-ray diffraction, energy dispersive spectrometer and X-ray photoelectron spectroscopy. The result shows that the particle surface was uniformly coated by a very thin LaPO 4 layer. Electrochemical measurements proved that the LaPO 4 -coated sample exhibited excellent cycling performance. The capacity retention of LaPO 4 -coated sample was 91.2% at 1 C after 100 cycles, which was higher compared with that of the pristine sample (76.4%). Moreover, the rate performance of the coated sample was greatly enhanced especially at 2, 5 and 10 C rate. The LaPO 4 -coated sample showed smaller charge transfer resistance and higher diffusion coefficient of lithium ions compared with those of the pristine sample. [ABSTRACT FROM AUTHOR]

As lithium metal resource supply and demand stabilize and prices decrease, the efficient recovery of valuable metals other than lithium from spent lithium-ion batteries is receiving increasing attention. Currently, challenges remain in the selective lithium recovery efficiency and the high cost of regenerating valuable metal slag after lithium extraction, particularly for spent ternary cathode materials. To address these challenges, this study introduces a closed-loop recovery process for spent ternary cathode materials, employing sulfur-assisted roasting to achieve efficient lithium extraction and high-value direct regeneration of ternary leaching residues. At moderate temperatures (500 ℃), LiNi x Co y Mn 1−x-y O 2 (NCM) materials undergo a directional transformation of lithium to Li 2 SO 4 in synergy with sulfur and oxygen, achieving a lithium leaching extraction rate of 98.91 %. Additionally, the relatively mild reaction conditions preserve the secondary spherical morphology and uniform distribution of NiCoMn-based oxide residue without introducing adverse impurities, ensuring the successful regeneration of high-value NCM cathode materials (R-NCM). The R-NCM material exhibits good discharge capacity (144.3 mA·h/g at 1 C) and relatively stable cycling performance, with a capacity retention rate of 80 % after 150 cycles. This work provides a viable pathway for the efficient and environmental-friendly pyrometallurgical closed-loop recovery of spent lithium-ion batteries. [Display omitted] • Introduction of a novel closed-loop recovery strategy utilizing sulfur-assisted roasting. • Demonstration of elemental sulfur's efficacy as a potent Li+ extractant, substantially mitigating impurity generation. • The gentle lithium extraction conditions minimize structural damage to the material. • Direct regeneration of high-value cathode materials from metal slag. [ABSTRACT FROM AUTHOR]

[Display omitted] • The enhancement effect of B-doping on electrochemical property is unraveled. • It delivers significantly improved cycling stability even under harsh testing conditions. • It exhibits outstanding high-rate long-cycling stability for pouch-type full cell. • This work provides an insight into the development for single-crystalline NCM cathode. Ni-rich layered oxides are considered as promising cathode materials for Li-ion batteries (LIBs) due to their satisfying theoretical specific capacity and reasonable cost. However, poor cycling stability caused by structural collapse and interfacial instability of the Ni-rich cathode material limits the further applications of commercialization. Herein, a series of B-doped single-crystal LiNi 0.83 Co 0.05 Mn 0.12 O 2 (NCM) are designed and fabricated, aiming to improve the structural stability and enlarge the Li+-ions diffusion paths simultaneously. It reveals that B-doping at TM layers will facilitate the formation of stronger B-O covalent bonds and expand the layered distance, significantly enhancing the thermodynamics and kinetic of NCM electrode. With the synergistic effect of single-crystalline architecture and appropriate B-doping, it can effectively alleviate the occurrence of internal strain with structural degradation and boost the intrinsic rate capability synchronously. As anticipated, the 0.6 mol % B-doped NCM electrode exhibits enhanced rate property and superior cycle stability, even at the harsh condition of high-temperature and elevated cut-off voltage. Remarkably, when tested in pouch-type full-cell, it maintains high reversible capacity with superior capacity retention of 91.35% over 500 cycles with only 0.0173% decay per cycle. This research illustrates the feasibility of B-doping and single-crystalline architecture to improve the electrochemical performance, which is beneficial to understand the enhancement effect and provides the design strategy for the commercialization progress of Ni-rich cathode materials. [ABSTRACT FROM AUTHOR]

Al 2 O 3 and AlPO 4 single-coated and double-coated LiNi 0.5 Co 0.2 Mn 0.3 O 2 materials have been synthesized by a wet-coating method in this paper. XRD, XPS, SEM, TEM, DSC as well as electrochemical methods are employed to investigate the structure, surface properties, thermal stability as well as electrochemical properties. The obtained layers are homogenously coated on the particles and the coating thickness is around 20–30 nm, the surface compositions are analyzed by XPS in detail as well. Comparing with those single-coated or uncoated samples, the double-coated one exhibits more superior thermal stability as well as electrochemical properties. The possible reason is mainly due to the dense and uniform coating layer as well as the formation of Li 3 PO 4 and LiAlO 2 on the cathode surface. Based on these results, it seems that Al 2 O 3 and AlPO 4 double-coating is an efficient strategy in improving the properties of LiNi 0.5 Co 0.2 Mn 0.3 O 2 materials, which can be also applied to other Ni-rich layered materials. [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel PDDA/GO dual-layer coating strategy to effectively improve the performance of NCM811 is proposed in this paper. • NCM811 particles can be well-encapsulated in the resultant dual-layer by a simple electrostatic adsorption method. • The PDDA/GO coating depresses the LiF component, enables a homogeneous organic-enriched CEI film with fast Li diffusion and effective corrosion protection on cathodes. • NCM811-PDDA/GO cathodes exhibit a 77% capacity retention after 500 cycles at the current density of 50 mA g−1, against 28% for pristine NCM811. Cathode-electrolyte interphases (CEIs) are determinative to the electrochemical performance of lithium-ion batteries, especially those with Ni-rich cathodes. Herein, we employed the simple electrostatic adsorption (SEA) method to generate a homogenous polydimethyldiallyl ammonium chloride/ graphene oxide (PDDA/GO) dual-layer coating on the surface of a model single-crystalline Ni-rich cathode, LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), and thus modified the CEIs in both compositions and microstructures. The PDDA/GO coating depresses the LiF component, enables a homogeneous organic-enriched CEI film with fast Li diffusion and effective corrosion protection on cathodes. Together with the mechanical confinement on cathodes, these characters of modified CEIs benefit the electrochemical stability effectively. For instance, NCM811-PDDA/GO cathodes exhibit a 77% capacity retention after 500 cycles at the current density of 50 mA g−1, against 28% for pristine NCM811. This study provides new insights in correlating the coating and CEIs, which effectively guide the development of Ni-rich cathodes for high performance. Such a simple strategy to form a homogeneous coating can also be extended into other electrode materials easily. [ABSTRACT FROM AUTHOR]

• W-doped Ni-rich layered cathode material is synthesized from W-doped precursor. • A small amount of W dopant enables ultra-fasting charging. • W-doped cathode shows improved stability in fast charge–discharge cycling. • W-doped cathode displays improved structure stability during charge–discharge. W-doped Ni-rich LiNi 0.879 Co 0.088 Mn 0.030 W 0.003 O 2 cathode material for lithium-ion batteries (LIBs) is synthesized from a bulk W-doped Ni 0.879 Co 0.088 Mn 0.03 W 0.003 (OH) 2 precursor. Comparative study between the W-doped cathode and its undoped counterpart LiNi 0.88 Co 0.09 Mn 0.03 O 2 is implemented. X-ray diffraction indicates that the W-doping shows no obvious influence on the crystallographic structure. Scanning electron microscope measurements indicate that the W-doped material has coarsened primary particles. Electrochemical evaluations reveal that the electrochemical performance is significantly improved by a small amount of W-doping, especially for the rate capability. The W-doped cathode delivers an initial discharge capacity of 201.7 mAh g−1, which is slightly higher than that of the undoped one (197.5 mAh g−1). When tested at 20C, the W-doped sample still has a discharge capacity of about 140 mAh g−1, whereas the value of the undoped one is only 104 mAh g−1. Furthermore, cyclic voltammetry and electrochemical impedance spectra measurements suggest that the W-doping can stabilize the H2 → H3 phase transition, as well as suppress the impedance increase during cycling process. [ABSTRACT FROM AUTHOR]

[Display omitted] • A facile surface modification for Ni-rich layered cathode materials is proposed. • A NASICON-type Li 2 AlZr(PO 4) 3 is used as the coating layer. • Lithium residues on the surface of NCM material are removed by this modification. • The cycling stability and rate capability are significantly improved. Ni-rich layered oxides are considered as a promising commercial cathode material due to high energy density and low cost. However, the severe capacity degradation and poor rate capability caused by structural collapse during long cycles limit their practical application. Herein, a NASICON-structured Li 2 AlZr(PO 4) 3 is constructed on the surface of LiNi 0.92 Co 0.05 Mn 0.03 O 2 for stabilizing the layered structure. In addition, the construction process consumes the lithium residues on the surface of the material particles, thus reducing alkalinity of the material surface. Meanwhile, the electrochemical properties of the samples are studied. The capacity of the 1 wt% Li 2 AlZr(PO 4) 3 coated sample shows 144.2 mAh g−1 with a discharge middle voltage of 3.71 V after 400 cycles under the voltage range of 2.7–4.3 V. Further studies confirm that the uniform NASICON coating can effectively alleviate the structural degradation and intergranular cracks after long-term cycling. The research results illustrate the feasibility of the practical application of the modification strategy, which can be popularized in Ni-rich layered cathode materials. [ABSTRACT FROM AUTHOR]

• The effects of various cations doping on electrochemical performance in Ni-rich single-crystalline NCM cathode. • Nb-ion doping NCM sample decrease the cation mixing, remain structural stability. • Nb-NCM shows the outstanding cycling stability with a voltage range of 3.0–4.5 V at room (25 ℃) and high (45 ℃) temperature. Layer Ni-rich cathode material has been attracted much attention due to its high energy density. A critical challenge of Ni-rich LiNi 1−x-y Co x Mn y O 2 systems is the severe capacity fading and poor rate capability due to the structural degradation during lithium-ion battery (LIB) cycle process. In this study, we employ a fast screening methodology to determine the effects of doping single-crystalline LiNi 0.7 Co 0.1 Mn 0.2 O 2 with cations Nb5+, Sr2+, Y3+, and then focus on the effects of Nb-ion doping on the structural stabilization (Nb-NCM). Nb ions doping and single crystallization are applied for LiNi 0.7 Co 0.1 Mn 0.2 O 2 (Nb-NCM), which enhance the structural stability and upgrade the electrochemical performance. Impressively, the modified Nb-NCM material shows remarkably cycling at the rate of 1 C (3.0–4.5 V) with a capacity retention of 80.1% after 200 cycles. Even at high temperatures (45 ℃), the structure of Nb-NCM also remains stable, which has a capacity of 149.8 mA h g−1 at 1 C (3.0–4.5 V) after 100 cycles. Further studies reveal that the successful doping of Nb-ion effectively inhibits cation mixing degree and structural degradation, and increases the diffusion coefficient of lithium-ion, which is the key to obtain the excellent electrochemical performance for LIBs. The present work indicates that the method of Nb-ion doping single-crystalline particles is an effective strategy to improve the stability of layered structure of Ni-rich NCM cathode material, and it represents an improve advance in the development of outstanding performance lithium-ion batteries. [ABSTRACT FROM AUTHOR]