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High production rates and the constant expansion of production capacities for lithium-ion batteries will lead to large quantities of production waste in the future. The desired achievement of a circular economy presupposes that such rejects could be recovered. This paper presents a two-staged process route that allows one to recover graphite and conductive carbon black from already coated negative electrode foils in a water-based and function-preserving manner, and it makes it directly usable as a particle suspension for coating new negative electrodes. In a first step, coating residues, which accumulate in production (as offcuts or rejects for example), are decoated in an aqueous ultrasonic bath. The ultrasonic bath also serves as a pre-thickener. As a result, high mass concentrations of active material can already be achieved in the water after the first process step. Water is then removed from the negative electrode suspension in a subsequent step by applying dynamic cross-flow filtration. With this unit operation, it is possible to concentrate the slurry residue to a solid content similar to that of the new electrode slurries used for coatings. An important criterion for the direct utilization of production waste is that the particle properties are affected as little as possible so that the suspension can be used directly for coating new films. This work presents the individual recycling process steps and their influence on the particle and slurry properties. The aim is to assess whether the recyclate is suitable for a coating of new negative electrodes and thus also for manufacturing batteries from 100% recycled material. [ABSTRACT FROM AUTHOR]

Thermal monitoring of lithium-ion batteries ensures their safe and optimal operation. To collect the most accurate temperature data of LIBs, previous studies used thermocouples in the cell and proved them to be technically viable. However, the cost and scale-up limitations of this method restricted its use in many applications, hindering its mass adoption. This work developed a low-cost and scalable screen-printed carbon black thermocouple to study its applicability for the thermal monitoring of LIB. Given the appropriate manufacturing parameters, it was found that thermal sensors may be printed on the electrodes, installed on a pouch cell, and once calibrated, operate with excellent sensitivity. However, to reliably use a printed carbon black thermocouple in operando of a pouch cell, its chemical resistance against electrolytes was found to require further development. [ABSTRACT FROM AUTHOR]

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]

The effects of electrochemical aging on the mechanical properties of electrodes in lithium-ion batteries are challenging to measure and are largely unknown. Mechanochemical degradation processes occur at different scales within an electrode and understanding the correlation between the degradation of mechanical properties, electrochemical aging, and morphological changes is crucial for mitigating battery performance degradation. This paper explores the evolution of mechanical and electrochemical properties at the layer level in a Ni-rich positive electrode during the initial stages of electrochemical cycling. The investigation involves complementary cross-section analyses aimed at unraveling the connection between observed changes on both macroscopic and microscopic scales. The macroscopic constitutive properties were assessed using a U-shaped bending test method that had been previously developed. The compressive modulus exhibited substantial dependency on both the porous structure and binder properties. It experienced a notable reduction with electrolyte wetting but demonstrated an increase with cycling and aging. During the initial stages of aging, electrochemical impedance spectra revealed increased local resistance near the particle–electrolyte interface. This is likely attributable to factors such as secondary particle grain separation and the redistribution of carbon black. The swelling of particles, compression of the binder phase, and enhanced particle contact were identified as probable factors adding to the elevation of the elastic modulus within the porous layer as a result of cycling. [ABSTRACT FROM AUTHOR]

Sodium iron phosphate-pyrophosphate, Na4Fe3(PO4)2P2O7 (NFPP) emerges as an excellent cathode material for sodium-ion batteries. Because of lower electronic conductivity, its electrochemical performance depends drastically on the synthesis method. Herein, we provide a simple and unified method for synthesis of composites between NFPP and reduced graphene oxide (rGO) and standard carbon black, designed as electrode materials for both sodium- and lithium-ion batteries. The carbon additives affect only the morphology and textural properties of the composites. The performance of composites in sodium and lithium cells is evaluated at elevated temperatures. It is found that NFPP/rGO outperforms NFPP/C in both Na and Li storage due to its hybrid mechanism of energy storage. In sodium half-cells, NFPP/rGO delivers a reversible capacity of 95 mAh/g at 20 °C and 115 mAh/g at 40 °C with a cycling stability of 95% and 88% at a rate of C/2. In lithium half-cells, the capacity reaches a value of 120 mAh/g at 20 and 40 °C, but the cycling stability becomes worse, especially at 40 °C. The electrochemical performance is discussed on the basis of ex situ XRD and microscopic studies. The good Na storage performance of NFPP/rGO at an elevated temperature represents a first step towards its commercialization. [ABSTRACT FROM AUTHOR]

In this study, multi-walled carbon nanotubes (MWCNTs) were modified by thermal fluorination to improve dispersibility between MWCNTs and Li4Ti5O12 (LTO) and were used as additives to compensate for the disadvantages of LTO anode materials with low electronic conductivity. The degree of fluorination of the MWCNTs was controlled by modifying the reaction time at constant fluorination temperature; the clear structure and surface functional group changes in the MWCNTs due to the degree of fluorination were determined. In addition, the homogeneous dispersion in the LTO was improved due to the strong electronegativity of fluorine. The F-MWCNT conductive additive was shown to exhibit an excellent electrochemical performance as an anode for lithium ion batteries (LIBs). In particular, the optimized LTO with added fluorinated MWCNTs not only exhibited a high specific capacity of 104.8 mAh g−1 at 15.0 C but also maintained a capacity of ~116.8 mAh g−1 at a high rate of 10.0 C, showing a capacity almost 1.4 times higher than that of LTO with the addition of pristine MWCNTs and an improvement in the electrical conductivity. These results can be ascribed to the fact that the semi-ionic C–F bond of the fluorinated MWCNTs reacts with the Li metal during the charge/discharge process to form LiF, and the fluorinated MWCNTs are converted into MWCNTs to increase the conductivity due to the bridge effect of the conductive additive, carbon black, with LTO. [ABSTRACT FROM AUTHOR]

The abundant use of lithium-ion batteries (LIBs) in a wide variety of electric devices and vehicles will generate a large number of depleted batteries, which contain several valuable metals, such as Li, Co, Mn, and Ni, present in the structure of the cathode material (LiMO2). The present work investigates the extraction of lithium, as lithium chloride, from spent LIBs by carbochlorination roasting. The starting samples consisted of a mixture of cathode and anode materials from different spent LIBs known as black mass. Calcium chloride was used as a chlorinating agent, and carbon black was used as a reducing agent. The black mass, calcium chloride, and carbon black were mixed in 50:20:30 w/w % proportions. Non-isothermal thermogravimetric tests up to 850 °C and isothermal tests at 350, 500, and 700 °C were carried out in an inert atmosphere. It was observed that the carbochlorination reaction starts at 500 °C. An extraction percentage of 99% was attained through carbochlorination at 700 °C. The characterization results indicate that CaCO3, Ni, and Co and, to a lesser extent, CoO, NiO, and MnO2 are present in the roasted sample after the processes of washing, filtering, and drying. [ABSTRACT FROM AUTHOR]

Silicon is a promising anode material that can increase the theoretical capacity of lithium-ion batteries (LIBs). However, the volume expansion of silicon remains a challenge. In this study, we employed a novel combination of conductive additives to effectively suppress the volume expansion of Si during charging/discharging cycles. Rather than carbon black (CB), which is commonly used in SiO anodes, we introduced single-walled carbon nanotubes (SWCNTs) as a conductive additive. Owing to their high aspect ratio, CNTs enable effective connection of SiO particles, leading to stable electrochemical operation to prevent volume expansion. In addition, we explored a combination of CB and SWCNTs, with results showing a synergetic effect compared to a single-component of SWCNTs, as small-sized CB particles can enhance the interface contact between the conductive additive and SiO particles, whereas SWCNTs have limited contact points. With this hybrid conductive additive, we achieved a stable operation of full-cell LIBs for more than 200 cycles, with a retention rate of 91.1%, whereas conventional CB showed a 74.0% specific capacity retention rate. [ABSTRACT FROM AUTHOR]

Water-based processing of electrodes is associated with an enhanced environmental footprint for lithium-ion battery (LIB) production in conjunction with reduced costs. This trend is accompanied by an increasing demand for electrode dispersion processing in inkjet printing. However, most of the dispersion components show a low inherent dispersibility with poor stability in aqueous formulations. This is particularly important when it comes to qualifying electrode dispersions for use in inkjet printing, since the effect of agglomeration and sedimentation effects must be effectively prevented. Therefore, additives are needed to improve the dispersive behavior. This paper analyzes the suitability of dispersants for organic electrode components, in particular graphite and carbon black. An empirical approach was devised on the basis of comprehensive theoretical considerations. Empirical investigations revealed that the utilization of polyvinylpyrrolidone (PVP) favored the enhanced stabilization of graphite nanoparticles. The addition of Triton X-100 (TX-100) resulted in an improved stabilization of carbon black. Based on these empirical studies, a methodology was derived, which supports the application of suitable dispersants in printable dispersions. [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]

Novel core-shell structure hard carbon/Si-carbon composites are prepared, and their electrochemical performances as an anode material for lithium-ion batteries are reported. Three different types of shell coating are applied using Si-carbon, Si-carbon black-carbon and Si-carbon black-carbon/graphite nanosheets. It appears that the use of n-Si/carbon black/carbon composite particles in place of n-Si for the shell coating is of great importance to achieve enhanced electrochemical performances from the core-shell composite samples, and additional wrapping with graphite nanosheets leads to a more stable cycle performance of the core-shell composites. [ABSTRACT FROM AUTHOR]

Recycling of lithium-ion batteries will become imperative in the future, but comprehensive and sustainable processes for this are still rather lacking. Direct recycling comprising separation of the black mass components as a key step is regarded as the most seminal approach. This paper contributes a novel approach for such separation, that is fractionation in a tubular centrifuge. An aqueous dispersion of cathode materials (lithium iron phosphate, also referred to as LFP, and carbon black) serves as exemplary feed to be fractionated, desirably resulting in a sediment of pure LFP. This paper provides a detailed study of the commonly time-dependent output of the tubular centrifuge and introduces an approach aiming to achieve constant output. Therefore, three different settings are assessed, constantly low, constantly high and an increase in rotational speed over time. Constant settings result in the predictable unsatisfactory time-variant output, whereas rotational speed increase proves to be able to maintain constant centrate properties. With further process development, the concept of fractionation in tubular centrifuges may mature into a promising separation technique for black mass in a direct recycling process chain. [ABSTRACT FROM AUTHOR]

Lots of lithium ion battery (LIB) products contain lithium metal oxide LiNi5Co2Mn3O2 (LNCM) as the positive electrode's active material. The stable surface of this oxide results in high resistivity in the battery. For this reason, conductive carbon-based materials, including acetylene black and carbon black, become necessary components in electrodes. Recently, carbon nano-tube (CNT) has appeared as a popular choice for the conductive carbon in LIB. However, a large quantity of the conductive carbon, which cannot provide capacity as the active material, will decrease the energy density of batteries. The ultra-high cost of CNT, compared to conventional carbon black, is also a problem. In this work, we are going to introduce long-length carbon nano-tube s(L-CNT) into electrodes in order to design a reduced-amount conductive carbon electrode. The whole experiment will be done in a 1Ah commercial type pouch LIB. By decreasing conductive carbon as well as increasing the active material in the positive electrode, the energy density of the LNCM-based 1Ah pouch type LIB, with only 0.16% of L-CNT inside the LNCM positive electrode, could reach 224 Wh/kg and 549 Wh/L, in weight and volume energy density, respectively. Further, this high energy density LIB with L-CNT offers stable cyclability, which may constitute valuable progress in portable devices and electric vehicle (EV) applications. [ABSTRACT FROM AUTHOR]

Low-molecular-weight carbonyl-containing compounds are considered beneficial energy storage materials in alkali metal-ion/alkaline earth metal-ion secondary batteries owing to the ease of their synthesis, low cost, rapid kinetics, and high theoretical energy density. This study aims to prepare a novel carbonyl compound containing a maleamic acid (MA) backbone as a material with carbon black to a new MA anode electrode for a lithium-ion battery. MA was subjected to attenuated total reflection-Fourier-transform infrared spectroscopy, and its morphology was assessed through scanning electron microscopy, followed by differential scanning calorimetry to determine its thermal stability. Thereafter, the electrochemical properties of MA were investigated in coin cells (2032-type) containing Li metal as a reference electrode. The MA anode electrode delivered a high reversible capacity of about 685 mAh g−1 in the first cycle and a higher rate capability than that of the pristine carbon black electrode. Energy bandgap analysis, electrochemical impedance, and X-ray photoelectron spectroscopy revealed that MA significantly reduces cell impedance by reforming its chemical structure into new nitrogen-based highly ionic diffusion compounds. This combination of a new MA anode electrode with MA and carbon black can increase the performance of the lithium-ion battery, and MA majorly outweighs transitional carbon black. [ABSTRACT FROM AUTHOR]

Silicon can be used in a variety of applications. Particularly, silicon particles are attracting increased attention as energy storage materials for lithium-ion batteries. However, silicon has a limited cycling performance owing to its peeling from the current collector and the volume expansion that occurs during alloying with lithium in the charging process. Significant contributors to this problem are the even distribution of silicon nanoparticles within the carbon matrix and their deep placement in the internal structure. In this study, we synthesized silicon nanoparticles and carbon materials via a bottom-up approach using a new method called plasma in solution. Silicon nanoparticles and the carbon matrix were synthesized in a structure similar to carbon black. It was confirmed that the silicon particles were evenly distributed in the carbon matrix. In addition, the evaluation of the electrochemical performance of the silicon–carbon matrix (Si–C) composite material showed that it exhibited stable cycling performance with high reversible capacity. [ABSTRACT FROM AUTHOR]

Waste soot generated from diesel engine of merchant ships has ≥ 2 µm agglomerates consisting of 30–50 nm spherical particles, whose morphology is identical to that of carbon black (CB) used in many industrial applications. In this study, we crystallized waste soot by heat treatment to transform it into a unique completely graphitic nano-onion structure, which is considerably different from that of commercial conductive CB. While commercial CB has a large specific surface area because of many surface micropores generated due to quenching by water-spraying in the production process, the heat-treated waste soot has a smooth micropore-free surface. Thus, the treated waste soot acquires the shape of CB but has a much smaller specific surface area. When the treated soot is used as a conductive material in lithium ion battery (LIB) half cells, the Coulombic efficiency of the entire anode is improved significantly owing to its low specific surface area; the electrochemical performance of the LIB is considerably enhanced compared to that of conventional conductive materials. Thus, polluting soot generated in marine propulsion can be transformed into a new class of CB with a unique structure by simple heat treatment; this soot can also be used as an inexpensive conductive material to enhance the LIB performance. [ABSTRACT FROM AUTHOR]

ReS2 nanosheets are grown on the surface of carbon black (CB) via an efficient hydrothermal method. We confirmed the ultra-thin ReS2 nanosheets with ≈1–4 layers on the surface of the CB (ReS2@CB) by using analytical techniques of field emission scanning electron microscopy (FESEM) and high-resolution transmission electron microscopy (HRTEM). The ReS2@CB nanocomposite showed high specific capacities of 760, 667, 600, 525, and 473 mAh/g at the current densities of 0.1 (0.23 C), 0.2 (0.46 C), 0.3 (0.7 C), 0.5 (1.15 C) and 1.0 A/g (2.3 C), respectively, in conjunction with its excellent cycling performance (432 mAh/g at 2.3 C; 91.4% capacity retention) after 100 cycles. Such LIB performance is greatly higher than pure CB and ReS2 powder samples. These results could be due to the following reasons: (1) the low-cost CB serves as a supporter enabling the formation of ≈1–4 layered nanosheets of ReS2, thus avoiding its agglomeration; (2) the CB enhances the electrical conductivity of the ReS2@CB nanocomposite; (3) the ultra-thin (1–4 layers) ReS2 nanosheets with imperfect structure can function as increasing the number of active sites for reaction of Li+ ions with electrolytes. The outstanding performance and unique structural characteristics of the ReS2@CB anodes make them promising candidates for the ever-increasing development of advanced LIBs. [ABSTRACT FROM AUTHOR]

A hindrance to the practical use of sodium-ion batteries is the lack of adequate anode materials. By utilizing the co-intercalation reaction, graphite, which is the most common anode material of lithium-ion batteries, was used for storing sodium ion. However, its performance, such as reversible capacity and coulombic efficiency, remains unsatisfactory for practical needs. Therefore, to overcome these drawbacks, a new carbon material was synthesized so that co-intercalation could occur efficiently. This carbon material has the same morphology as carbon black; that is, it has a wide pathway due to a turbostratic structure, and a short pathway due to small primary particles that allows the co-intercalation reaction to occur efficiently. Additionally, due to the numerous voids present in the inner amorphous structure, the sodium storage capacity was greatly increased. Furthermore, owing to the coarse co-intercalation reaction due to the surface pore structure, the formation of solid-electrolyte interphase was greatly suppressed and the first cycle coulombic efficiency reached 80%. This study shows that the carbon material alone can be used to design good electrode materials for sodium-ion batteries without the use of next-generation materials. [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]