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All-solid-state lithium-ion batteries (ASSLBs) represent a promising breakthrough in battery technology owing to their high energy density and exceptional stability. When crafting cathode electrodes for ASSLBs, the solid electrolyte/cathode material interface is physically hindered by the specific morphology of carbon additive materials. In this paper, we examine the distribution of conductive additives within the electrode and its impact on the electrochemical performance of composites incorporating either nano-sized carbon black (CB) or micron-sized carbon nanofibers (CNF) into Ni-rich (LiNi0.8Co0.1Mn0.1O2) cathode material based composites. When nano-sized CB is employed as a conductive additive, it enhances the electrical conductivity of the composite by adopting a uniform distribution. However, its positioning between the solid electrolyte and cathode material leads to an increase in interfacial resistance during charge and discharge cycles, resulting in decreased electrochemical performance. In contrast, using micron-sized CNF as a conductive additive results in a reduction in the composite's electrical conductivity compared to CB. Nevertheless, due to the comparatively uninterrupted interfaces between the solid electrolyte and cathode materials, it exhibits superior electrochemical characteristics. Our findings are expected to aid the fabrication of electrochemical-enhanced cathode composite electrodes for ASSLBs. [ABSTRACT FROM AUTHOR]

[Display omitted] • Dispersion/aggregation of acetylene black determines settling time of cathode slurry. • Strength and recoverability of conductive network structure affect cathode properties. • Hydrostatic pressure change of slurry linked to cathode density/volume resistivity. Hypothesis: It is important to elucidate the effect of the particle dispersion/aggregation state of electrode slurries on resulting electrodes for the development of superior lithium-ion batteries. Many studies have been conducted to characterize cathode slurries for lithium-ion batteries; however, the particle dispersion state of cathode slurries remains unclear. This study investigates the rheological behavior and the packing ability of the cathode slurries for obtaining a denser electrode with lower electric resistance. Experiments: In addition to the conventional flow curve measurement, we measured the changes in the hydrostatic pressure of the slurries with time to evaluate their packing ability. The relationship between the properties of the cathode slurries and those of the as-cast cathodes was also investigated. Findings: It was found that a slurry in which acetylene black powder forms a network structure, with sufficient strength and the ability to rapidly recover after breaking, yields a cathode with comparatively high density and comparatively low volume resistivity. It was also found that the normalized settling time of a cathode slurry determined from its change in hydrostatic pressure over time correlates well with both the density and volume resistivity of a resulting as-cast cathode. [ABSTRACT FROM AUTHOR]

The multi-interactions between nanoparticles and micro-particles, as well as polymers are responsible for complex rheological behavior in electrode slurry, which has crucially influenced the quality and lifetime of lithium-ion batteries. To clarify the shear- and time-dependent rheological behavior of the multi-component slurry, the effect of various components on the yield stress, viscosity, and thixotropic time scales has been investigated by steady-state and transient step experiments. The results demonstrate that the amounts of added carbon black, polymeric binders, and active material play a significant role in the rheological properties. In the steady-state tests, the viscosity of the slurry increases with the increase of the carbon black, polymer, and active material content. However, the yield stress of the slurry only distinctly increases when the carbon black and polymer are increased, while it is virtually unaffected by large particles of the active material. In the transient tests, the destroyed timescale rises and the recovery timescale reduces as the carbon black, polymer, and active material content are increased. The quantitative relationship between various components and rheological behaviors will be useful for the preparation and coating process of slurry. [ABSTRACT FROM AUTHOR]

Many studies have been recently conducted on Ni-rich cathodes to increase cell capacity. The improvement of cell capacity is reaching its limit by increasing Ni content of a cathode material. In addition, increasing Ni content of a cathode material is unsafe due to gas evolution. Thus, research on Ni-rich cathode should proceed in parallel with the development of cell design, i.e., thickening electrode. However, during a calendering process, upper layer particles with low mechanical strength can be fractured, which is a problem with a thick electrode. To solve this issue, electrodes were designed using single crystalline lithium nickel cobalt manganese oxides (NCM) of high mechanical strength together with existing polycrystalline NCM in the present study. Four types of electrodes were tested to determine the best design for the electrode. Among them, double layer of upper layer with single crystalline and lower layer with polycrystalline (DB) completely prevented particle fracturing in the upper layer while maintaining sufficient tortuosity within the electrode. The reaction within the electrode was much more uniform than in other samples. As a result, DB had higher capacity of 34.6 mAh g−1 than the pristine after 40 cycles and a higher capacity of 50.5 mAh g−1 at 2C. • Particles on the upper layer of electrode can be fractured by the pressing force. • The carbon black and PVDF of the upper layer can be agglomerated. • The upper layer of the DB was entirely made of SC, there was no upper layer crack. • The DB enabled a uniform reaction within the electrode without upper layer crack. [ABSTRACT FROM AUTHOR]

Conductive additives, like carbon black or graphite, are essential components of lithium ion batteries due to the limited electrical conductivity of most electrode materials. However, there is still a lack of knowledge about the optimized distribution of these materials within the electrode. A dry mixing process is used in order to prepare a conductive coating by depositing carbon black on the surface of Li(Ni 1/3 Mn 1/3 Co 1/3 )O 2 (NMC) cathode particles. It is demonstrated that this – from a theoretically point of view – favorable distribution does not allow the preparation of working electrodes without taking into account the role of the binder. After adding an organic binder to the slurry, the polymer deposits on top of the carbon shell during drying and inhibits the conductive contact between the particles. This can be avoided by a fraction of distributed carbon particles which are associated with the binder phase providing conductive paths through the isolating organic material. It is shown that carbon black and graphite are principally fulfilling this task, but both materials are leading to varying processing behavior and electrode properties. [ABSTRACT FROM AUTHOR]

Metal chalcogenides undergoing alloying and conversion mechanism can give high capacity as anode for lithium-ion batteries. However, large volume change and phase segregation lead to poor cycle performance. In this study, we focus on Sb 2 Se 3 and develop methods to enhance its long-term stability and reversibility. In particular, we find that carbon encapsulation reduces volume change during lithiation/delithiation and facilitates the recombination process of Sb and Se even after long cycling. With an addition of 20 wt% acetylene black, the Sb 2 Se 3 /C nanocomposite material exhibits an excellent cycle performance with a charge capacity of 545 mAh g−1 at 250 mA g−1 after 1000 cycles, corresponding to a capacity retention of 99.3%. We also demonstrate a full cell with LiFePO 4 cathode and Sb 2 Se 3 /C anode that is capable of delivering a stable capacity of 340 mAh g−1 at 1 A g−1 (about 3 C rate) after 300 cycles. • Sb 2 Se 3 nanoparticles encapsulated with carbon matrix is synthesized via mechanical ball-milling. • Carbon matrix enhances the mechanical stability of the electrode and suppresses phase segregation. • Sb 2 Se 3 @20%AB delivers a stable capacity of 545 mAh g−1 over 1000 cycles. • Sb 2 Se 3 @20%AB/LiFeO 4 full cell shows good rate capability and cycle stability. [ABSTRACT FROM AUTHOR]

Li-ion batteries (LIBs) employ porous, composite-type electrodes, where few weight percentages of carbonaceous conducting agents and polymeric binders are required to bestow electrodes with electrical conductivity and mechanical robustness. However, the use of such inactive materials has limited enhancements of battery performance in terms of energy density and safety. In this study, we introduced graphene/polyvinylidene fluoride (Gr/PVdF) composites in Ni-rich oxide cathodes for LIBs, replacing conventional conducting agents, carbon black (CB) nanoparticles. By using Gr/PVdF suspensions, we fabricated highly dense LiNi0.85Co0.15Al0.05O2 (NCA) cathodes having a uniform distribution of conductive Gr sheets without CB nanoparticles, which was confirmed by scanning spreading resistance microscopy mode using atomic force microscopy. At a high content of 99 wt.% NCA, good cycling stability was shown with significantly improved areal capacity (Qareal) and volumetric capacity (Qvol), relative to the CB/PVdF-containing NCA electrode with a commercial-level of electrode parameters. The NCA electrodes using 1 wt.% Gr/PVdF (0.9:0.1) delivered a high Qareal of ~3.7 mAh cm−2 (~19% increment) and a high Qvol of ~774 mAh cm−3 (~18% increment) at a current rate of 0.2 C, as compared to the conventional NCA electrode. Our results suggest a viable strategy for superseding conventional conducting agents (CB) and improving the electrochemical performance of Ni-rich cathodes for advanced LIBs. [ABSTRACT FROM AUTHOR]

We report the preparation of thick ceramic electrodes of the olivine LiFePO 4 (LFP) with high mass loading. These electrodes are preparated by means of Powder Extrusion Moulding (PEM), which is a technology easily scalable and cheap. These LFP cathodes are additive-free (neither binder nor extra carbon black) with ~0.5 mm thickness, allowing to develop very high areal capacity (13.7 mA h cm−2). By means of a strict control of sintering process, the carbon coating of the commercial LFP powder remains and the decomposition of the active material is prevented. The optimized self-supported LFP cathode presents good cyclability over 20 cycles at C/10 with no capacity loss. The good electrochemical performance of these novel LFP thick electrodes and their non-flammability make them interesting candidates for both mobile and stationary applications. Image 1 • Thick ceramic electrodes of LiFePO4 with high areal capacities (13.7 mA h cm-2). • Self-supported LFP cathode with good cyclability at C/10. • New generation of high performances and sustainable ultra-thick electrodes. • Thick electrodes (~500 μm) prepared by an easily scalable manufacturing process. [ABSTRACT FROM AUTHOR]

Nickel–manganese–cobalt oxides, with LiNi0.33Mn0.33Co0.33O2 (NMC) as the most prominent compound, are state-of-the-art cathode materials for lithium-ion batteries in electric vehicles. The growing market for electro mobility has led to a growing global demand for Li, Co, Ni, and Mn, making spent lithium-ion batteries a valuable secondary resource. Going forward, energy- and resource-inefficient pyrometallurgical and hydrometallurgical recycling strategies must be avoided. We presented an approach to recover NMC particles from spent lithium-ion battery cathodes while preserving their chemical and morphological properties, with a minimal use of chemicals. The key task was the separation of the cathode coating layer consisting of NMC, an organic binder, and carbon black, from the Al substrate foil. This can be performed in water under strong agitation to support the slow detachment process. However, the contact of the NMC cathode with water leads to a release of Li+ ions and a fast increase in the pH. Unwanted side reactions may occur as the Al substrate foil starts to dissolve and Al(OH)3 precipitates on the NMC. These side reactions are avoided using pH-adjusted solutions with sufficiently high buffer capacities to separate the coating layer from the Al substrate, without precipitations and without degradation of the NMC particles. [ABSTRACT FROM AUTHOR]