Search Results (252)

Cathodic exfoliation of graphite has emerged as an attractive method to synthesize high-quality and lo- defect graphene. Here, it is demonstrated that the type of starting graphite material influences the properties of exfoliated graphene. Graphite foil, natural graphite, and graphite rods were examined in the exfoliation processes performed in 3.0 M KCl at −15 V. The use of a graphite foil facilitates the rapid cathodic exfoliation process in comparison with structurally more compact natural graphite and graphite rods. For the graphite foil, the cathodically exfoliated graphene exhibits a low defect density (I_D/I_G of 0.09, a C/O ratio of 35) with graphite exfoliation yield of 92.8%. In contrast, the exfoliated graphene from natural graphite exhibits an I_D/I_G of 0.15, a C/O ratio of 28, and a graphite exfoliation yield of 30.5%, whereas graphene from graphite rod exhibits an I_D/I_G of 0.86, a C/O ratio of 30, and a graphite exfoliation yield of 19.5%. The dense structure of natural graphite and graphite rods led to longer exfoliation times. Exfoliation of graphite rods produced few-layer graphene with the smallest sheet size, whereas natural graphite and graphite foil yielded multilayer graphene with larger sheets. This study demonstrates the feasibility of using aqueous-based cathodic exfoliation to produce graphene from various graphite sources, leading to variations in sheet thickness, size, defect density, and solvent dispersibility. Full article

Lithium-ion batteries (LiBs) are utilized in numerous applications due to advancements in technology, and the recovery of end-of-life (EoL) LiBs is imperative for environmental and economic reasons. Pyrometallurgical and hydrometallurgical methods have been used in the recovery of metals such as Li, Co, and Ni in the EoL LiBs. Hydrometallurgical methods, which have been demonstrated to exhibit higher recovery efficiency and reduced energy consumption, have garnered increased attention in recent research. Inorganic acids, including HCl, HNO₃, and H₂SO₄, as well as organic acids such as acetic acid and citric acid, are employed in the hydrometallurgical recovery of these metals. It is imperative to acknowledge the environmental hazards posed by these acids. Consequently, solvometallurgical processes, which involve the use of organic solvents with minimal or no water, are gaining increasing attention as alternative or complementary techniques to conventional hydrometallurgical processes. In the context of solvent systems that have been examined for a range of solvometallurgical methods, deep eutectic solvents (DESs) have garnered particular interest due to their low toxicity, biodegradable nature, tunable properties, and efficient metal recovery potential. In this study, the leaching process of black mass containing graphite, LCO, NMC, and LMO was carried out in a short time using the ternary DES system. The ternary DES system consists of choline chloride (ChCl), glycolic acid (GLY), and ascorbic acid (AA). As a result of the leaching process of cathode powders in the black mass without any pre-enrichment process, Li, Co, Ni, and Mn elements passed into solution with an efficiency of over 95% at 60 °C and within 1 h. Moreover, the kinetics of the leaching process was investigated, and Density Functional Theory (DFT) calculations were used to explain the leaching mechanism. Full article

Accurate prediction of the State of Health (SOH) of lithium-ion batteries is essential for ensuring their safe and reliable operation. However, traditional deep learning approaches often suffer from challenges such as overfitting, limited generalization capability, and suboptimal prediction accuracy. To address these issues, this paper proposes a novel framework that combines a Long Short-Term Memory (LSTM) network with a Physics-Informed Neural Network (PINN), referred to as LSTM-PINN, for high-precision SOH estimation. The proposed framework models battery degradation using state-space equations and extracts latent temporal features. These features are further integrated into a Deep Hidden Temporal Physical Module (DeepHTPM), which incorporates physical prior knowledge into the learning process. This integration significantly enhances the model’s ability to accurately capture the complex dynamics of battery degradation. The effectiveness of LSTM-PINN is validated using two publicly available datasets based on graphite cathode materials (NASA and CACLE). Extensive experimental results demonstrate the superior predictive performance of the proposed model, achieving Mean Absolute Errors (MAEs) of just 0.594% and 0.746% and Root Mean Square Errors (RMSEs) of 0.791% and 0.897% on the respective datasets. Our proposed LSTM-PINN framework enables accurate battery aging modeling, advancing lithium-ion battery SOH prediction for industrial applications. Full article

Electrochemical formation of ceria (mixed Ce₂O₃ and CeO₂) coatings on different types of screen-printed carbon electrodes (SPCEs) (based on graphite (C110), carbon nanotubes (CNT), single-walled carbon nanotubes (SWCNT), carbon nanofibers (CNF), and mesoporous carbon (MC)) were studied. Their potential applications as catalysts for various redox reactions and electrochemical sensors were investigated. The ceria oxide layers were electrodeposited on SPCEs at various current densities and deposition time. The morphology, structure, and chemical composition in the bulk of the ceria layers were studied by SEM and EDS methods. XRD was used to identify the formed phases. The concentration, chemical composition and chemical state of the elements on the surface of studied samples were characterized by XPS. It was established that the increase of the concentration of CeCl₃ in the solution and the cathode current density strongly affected the surface structure and concentration (relation between Ce³⁺ and Ce⁴⁺, respectively) in the formed ceria layers. At low concentration of CeCl₃ (0.1M) and low values of cathode current density (0.5 mA·cm⁻²), porous samples were obtained, while with their increase, the ceria coatings grew denser. Full article

Silicon oxide–graphite is a promising high-capacity anode material for next-generation lithium-ion batteries (LIBs). However, despite using a small fraction (≤5%) of Si, it suffers from a short cycle life owing to intrinsic swelling and particle pulverization during cycling, making practical application challenging. High-nickel (Ni ≥ 80%) oxide cathodes for high-energy-density LIBs and their operation beyond 4.2 V have been pursued, which requires the anodic stability of the electrolyte. Herein, we report a nonflammable multi-functional fluorinated ester–based liquid electrolyte that stabilizes the interfaces and suppresses the swelling of highly loaded 5 wt% SiO–graphite anode and LiNi_0.88Co_0.08Mn_0.04O₂ cathode simultaneously in a 3.5 mAh cm⁻² full cell, and improves cycle life and battery safety. Surface characterization results reveal that the interfacial stabilization of both the anode and cathode by a robust and uniform solid electrolyte interphase (SEI) layer, enriched with fluorinated ester-derived inorganics, enables 80% capacity retention of the full cell after 250 cycles, even under aggressive conditions of 4.35 V, 1 C and 45 °C. This new electrolyte formulation presents a new opportunity to advance SiO-based high-energy density LIBs for their long operation and safety. Full article

Separators are generally considered inert components in lithium-ion batteries. In the past, some electroactive polymers have been successfully applied in separator modifications for overcharge protection or as acid scavengers. This study highlights the first use of two “electroactive” carbazole polymers (copolymer 9-phenyl-9H-carbazole-phenyl [PCP] and poly(9-vinylcarbazole) [PVC]), which were each applied separately as coatings on the cathode-facing side of commercial Celgard 2325 separators, respectively, to enhance the cycling performance of 0.3Li₂MnO₃·0.7LiMn_0.5Ni_0.5O₂//graphite (LMR-NM//Gr) full cells through interphase engineering. The team observed an irreversible polymer oxidation process of the carbazole-functionalized polymers—occurring only during the first charge—for the modified separator cells, and the results were confirmed by dQ/dV analysis, cyclic voltammetry measurements, and nuclear magnetic resonance characterizations. During this oxidation, carbazole polymers participate in the process of interphase formation, contributing to the improved cycling performance of LMR-NM//Gr batteries. Particularly, oxidation takes place at voltages of ~4.0 and ~3.5 V when PCP and PVC are used as separator coatings, which is highly irreversible. Further postmortem examinations suggest that the improvements using these modified separators arise from the formation of higher-quality and more inorganic SEI, as well as the beneficial CEI enriched in LixPOyFz. These interphases effectively inhibit the crosstalk effect by reducing TM dissolution. Full article

The primary challenge associated with stainless steel in fuel cell operation is its susceptibility to corrosion, which leads to increased contact resistance and subsequent degradation of electrochemical performance. In general, the protective layers have been loaded onto the metal surface by widely used traditional techniques such as physical vapor deposition (PVD), or cathode arc ion plating. However, the above sputtering and evaporation ways require a high-vacuum condition, complicated experimental setups, higher costs, and an elevated temperature. Therefore, herein the achievement for uniform coatings over a large surface area has been realized by using a cost-effective strategy through a complete wet chemical process. The synergistic regulation of two conductive components and a plastic additive has been employed together with the entrapment of a surfactant to optimize the microstructure of the coating surface. The assembly of layered graphite and a polystyrene sphere could maintain both the high corrosion resistance feature and excellent electrical conductivity. In particular, the intrinsic vacant space in the above physical barriers has been filled with fine powders of indium tin oxide (ITO) due to its small size, and the interconnected conductive network with vertical/horizontal directions would be formed. All the key technical targets based on the U.S. Department of Energy (DOE) have been achieved under the simulated operating environments of a proton exchange membrane fuel cell. The corrosion current density has been measured as low as 0.52 μA/cm² (for the sample of graphite/mixed layer) over the applied potentials from −0.6 V to 1.2 V and its protective efficiency is evaluated to be 99.8%. The interfacial contact resistance between the sample and the carbon paper is much less than 10 mΩ·cm² (3.4 mΩ·cm²) under a contact pressure of 165 N/cm². The wettability has been investigated and its contact angle has been evolved from 48° (uncoated sample) to even 110°, providing superior hydrophobicity to prevent water penetration. Such an innovative approach opens up new possibilities for improving the durability and reducing the costs of carbon-based coatings. Full article

Sodium dual-ion batteries combine economic and environmental benefits by using carbon materials in both electrodes and sodium compounds in the electrolyte. Among other factors, their successful implementation for energy storage relies on optimization of the properties of the carbon electrode materials. To this end, carbon materials with a wide range of textural and structural properties were prepared by simply heat treating a single porous carbon in the absence or presence of a low-cost highly effective iron-based catalyst. These materials were investigated as anode or cathode in the sodium dual-ion batteries by prolonged galvanostatic cycling. The optimal textural and structural properties for carbon materials to achieve the best performance as electrodes in sodium dual-ion batteries were identified as having a high degree of graphitic structural order combined with minimal microporosity in the cathode and a non-graphitic structure with a layer spacing of around 0.37 nm and moderate microporosity in the anode. Full article

Iron phosphate (FePO₄·2H₂O) was synthesized via anodic oxidation using nickel–iron alloy composition simulates from laterite nickel ore as the anode and graphite electrodes as the cathode, with phosphoric acid serving as the electrolyte. A uniform experimental design was employed to systematically optimize the synthesis parameters including voltage, electrolyte concentration, electrolysis time, and degree of acidity or alkalinity (pH). The results indicate that the addition of cetyltrimethylammonium bromide (CTAB) surfactant effectively modulated the morphology of the anodic oxidation products. The optimized conditions were determined to be an electrolyte concentration of 1.2 mol/L, a voltage of 16 V, a pH of 1.6, an electrolysis time of 8 h, and a 3% CTAB addition. Under these conditions, the synthesized FePO₄·2H₂O exhibited enhanced performance as a lithium-ion battery precursor. Specifically, the corresponding LiFePO₄/C cathode delivered an initial discharge capacity of 157 mA h g⁻¹ at 0.2 C, retaining 99.36% capacity after 100 cycles. These findings provide valuable insights and theoretical foundations for the efficient preparation of iron phosphate precursors, highlighting the significant impact of optimized synthesis conditions on the electrochemical performance of lithium iron phosphate. Full article

Lithium-ion batteries (LIBs) are widely used in diverse applications, ranging from portable ones to stationary ones. The appropriate handling of the immense amount of spent batteries has, therefore, become significant. Whether recycled or repurposed for second-life applications, knowing their chemistry type can lead to higher efficiency. In this paper, we propose a novel machine learning-based approach for accurate chemistry identification of the electrode materials in LIBs based on their temperature dynamics under constant current cycling using gated recurrent unit (GRU) networks. Three different chemistry types, namely lithium nickel cobalt aluminium oxide cathode with silicon-doped graphite anode (NCA-GS), nickel cobalt aluminium oxide cathode with graphite anode (NCA-G), and lithium nickel manganese cobalt oxide cathode with graphite anode (NMC-G), were examined under four conditions, 0.2 C charge, 0.2 C discharge, 1 C charge, and 1 C discharge. Experimental results showed that the unique characteristics in the surface temperature measurement during the full charge or discharge of the different chemistry types can accurately carry out the classification task in both experimental setups, where the model is trained on data under different cycling conditions separately and jointly. Furthermore, experimental results show that the proposed approach for chemistry type identification based on temperature dynamics appears to be more universal than voltage characteristics. As the proposed approach has proven to be efficient in the chemistry identification of the electrode materials LIBs in most cases, we believe it can greatly benefit the recycling and second-life application of spent LIBs in real-life applications. Full article

Li/graphite fluoride (Li/CF_x) batteries display the highest energy densities among those of commercially available primary Li batteries but fail to satisfy the high-performance requirements of advanced applications. To address this drawback, two liquid organic dinitrates, namely, 1,4-butanediol dinitrate (BDE) and 2,2,3,3-tetrafluoro-1,4-butanediol dinitrate (TBD), were employed as high-energy energetic materials, and they were highly compatible with the electrolytes of Li/CF_x batteries. The use of Super P electrodes confirmed that the reduction reaction mechanisms of both nitrate ester-based compounds delivered considerable specific capacities, associated with discharge potentials matching that of the Li/CF_x battery. When considering the combined mass of the electrolyte and cathode as the active material, the overall energy densities of the Li/CF_x batteries increased by 25.3% (TBD) and 20.8% (BDE), reaching 1005.50 and 969.1 Wh/kg, respectively. The superior performance of TBD was due to the synergistic effects of the high electronegativities and levels of steric hindrance of the F atoms. Moreover, the nanocrystal LiF particles generated by TBD induced crack formation within the fluorinated graphite, increasing the lithium-ion accessible surface area and enhancing its utilization efficiency. These combined factors enhanced the reactivity of TBD and facilitated its involvement in electrochemical reactions, thus improving the capacity of the battery. The developed strategy enables the facile, cost-effective enhancement of the capacities of Li/CF_x batteries, paving the way for their practical use in energy-demanding devices. Full article

Aluminium is an attractive material for proton-exchange-membrane fuel cell bipolar plates as it has a much lower density than steel and is easier to form than both steel and graphite. This work focused on the development of amorphous carbon films deposited using closed-field unbalanced magnetron sputtering (CFUBMS) in order to improve the corrosion resistance of aluminium bipolar plates and to enhance fuel cell performance and durability. Chromium and tungsten adhesion layers were used for the coatings. It was possible to achieve good electrical conductivity and high electrochemical corrosion resistance up to 70 °C on polished Aluminium alloy 6082 by tuning the deposition parameters. Coatings with a tungsten adhesion layer showed better corrosion resistance than those with a chromium adhesion layer. In situ, accelerated stress testing of single cells was performed using uncoated and coated Al6082 bipolar plates. Both coatings resulted in improved fuel cell performance compared to uncoated aluminium when used on the cathode side of the fuel cell. Full article

As the global energy demand continues to rise, the utilization of lithium-ion capacitors (LICs), which combine the advantages of lithium-ion batteries (LIBs) and electrochemical capacitors (ECs), is also increasing. LICs offer high energy density, high power density, and a long life cycle. However, a prelithiation process is required for graphite-based anode materials. In LICs, the formation of the solid electrolyte interphase (SEI) layer inevitably causes an initial irreversible capacity loss, often resulting in the excessive consumption of lithium ions. Considering the limited lithium resources, prelithiation is essential to achieve a satisfactory electrochemical performance in LICs. Various anode prelithiation techniques have been reported to enhance the capacity of LIBs and LICs. Among these, the direct-contact prelithiation method involves physically contacting lithium metal with the electrode or active material. In this study, direct-contact prelithiation was performed on soft carbon-based anode materials, and LICs were fabricated using activated carbon-based cathode materials. The electrochemical properties of the fabricated LICs were evaluated to demonstrate the feasibility of applying the direct-contact prelithiation technique. Full article

Metal–organic frameworks (MOFs) are regarded as advanced supercapacitor materials owing to their high surface area, redox-active sites, and porosity. However, their insufficient charge carrier mobility remains a critical limitation for practical application. Integrating MOFs with conductive carbon substrates is an effective strategy to break through this limitation. However, conventional carbon materials often require complex preparation methods and pre-activation steps for use in MOF composites. Herein, multilayer graphene (MLG) mechanically exfoliated from expandable graphite is employed as a substrate, and a van der Waals force-assisted chemical deposition method is developed to directly anchor Ni-MOF onto its surface without requiring pre-activation treatment. To optimize the composite, Ni-MOFs with various mass loadings are synthesized on MLG surface. The morphological characteristics and energy storage performance of these composites are thoroughly characterized. Ni-MOF/MLG-0.30 (with a 70.8% Ni-MOF loading on MLG) features a porous stacking structure of well-crystalline Ni-MOF parallelogram nanosheets on MLG, exhibiting optimal electrochemical performance. The composite achieves 1071.4 F·g⁻¹ at 1 A·g⁻¹, and a capacitance retention of 64.9% at the elevated current density of 10 A·g⁻¹. Meanwhile, the composite maintains 63.2% of its initial capacitance after 5000 charge/discharge cycles at 4 A·g⁻¹. A hybrid supercapacitor is fabricated using Ni-MOF/MLG-0.30 cathode and activated carbon anode, delivering 27.9 Wh·kg⁻¹ energy density at 102.5 W·kg⁻¹ power output. Full article

This study investigates graphite separation from Lithium-Ion Battery (LIB) black mass (which is a mixture of anode and cathode materials) via froth flotation coupled with an open-loop recycling approach for the graphite (froth) product. Black mass samples originating from different LIB types were used to produce a carbon-poor and a carbon-enriched fractions. The optimization of the flotation parameters was carried out depending on the black mass chemistry, i.e., the number of flotation stages and the dosing of flotation agents. The carbon-enriched product (with a carbon content of 92 wt.%, corresponding to a recovery of 89%) was subsequently used as a secondary carbon source for refractory material (magnesia carbon brick). Analyses of brick chemistry, as well as thermo-mechanic properties in terms of density, porosity, cold crushing strength (CCS), hot modulus of rupture (HMOR—the maximum bending stress that can be applied to a material before it breaks), and thermal conductivity showed no negative influence on brick quality. It could be demonstrated that flotation graphite can principally be used as a secondary source for non-battery applications. This is a highly valuable example that contributes to a more complete closure of a battery’s life cycle in terms of circular economy. Full article