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Polyvinylidene fluoride (PVDF) binder removal is critical for the recovery of valuable metal materials during the treatment of spent lithium-ion batteries (LIBs). This study proposed a new PVDF removal method through subcritical methanol extraction. The optimal conditions and mechanism of the method for the liberation of cathode materials were explored, and the recovered cathode materials, aluminum foils (Al foils), and extracted binder were characterized. Experimental results on actual cathode sheets show that under the extraction temperature of 200 °C, after holding and stirring time for 10 min, the cathode materials were recovered in the form of powder with an exfoliation efficiency of 98.51 % from Al foil without any damage. The removal efficiency of PVDF reached 78.74 wt% while the crystal structure of LiMn 2 O 4 remained intact. Compared with the new binder, the recovered PVDF (R-PVDF) has a similar glass transition temperature and melting point but presents a more intricate surface morphology, lower crystallinity, and higher proportion α-phase crystallin. The results indicate that R-PVDF has the potential to be reused as a new binder in LIBs. This study aims to provide a new efficient and environmentally friendly solution for the recycling of spent LIBs., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier Ltd.)

In recent years, the demand for lithium-ion batteries (LIBs) has been increasing rapidly. Conventional recycling strategies (based on pyro- and hydrometallurgy) are damaging for the environment and more sustainable methods need to be developed. Bioleaching is a promising environmentally friendly approach that uses microorganisms to solubilize metals. However, a bioleaching-based technology has not yet been applied to recover valuable metals from waste LIBs on an industrial scale. A series of experiments was performed to improve metal recovery rates from an active cathode material (LiCoO 2 ; LCO). (i) Direct bioleaching of ≤0.5 % LCO with two prokaryotic acidophilic consortia achieved >80 % Co and 90 % Li extraction. Significantly lower metal recovery rates were obtained at 30 °C than at 45 °C. (ii) In contrast, during direct bioleaching of 3 % LCO with consortia adapted to elevated LCO levels, the 30 °C consortium performed significantly better than the 45 °C consortium, solubilizing 73 and 93 % of the Co and Li, respectively, during one-step bioleaching, and 83 and 99 % of the Co and Li, respectively, during a two-step process. (iii) The adapted 30°C consortium was used for indirect leaching in a low-waste closed-loop system (with 10 % LCO). The process involved generation of sulfuric acid in an acid-generating bioreactor (AGB), 2-3 week leaching of LCO with the biogenic acid (pH 0.9), selective precipitation of Co as hydroxide, and recirculation of the metal-free liquor back into the AGB. In total, 58.2 % Co and 100 % Li were solubilized in seven phases, and >99.9 % of the dissolved Co was recovered after each phase as a high-purity Co hydroxide. Additionally, Co nanoparticles were generated from the obtained Co-rich leachates, using Desulfovibrio alaskensis , and Co electrowinning was optimized as an alternative recovery technique, yielding high recovery rates (91.1 and 73.6% on carbon felt and roughened steel, respectively) from bioleachates that contained significantly lower Co concentrations than industrial hydrometallurgical liquors. The closed-loop system was highly dominated by the mixotrophic archaeon Ferroplasma and sulfur-oxidizing bacteria Acidithiobacillus caldus and Acidithiobacillus thiooxidans . The developed system achieved high metal recovery rates and provided high-purity solid products suitable for a battery supply chain, while minimizing waste production and the inhibitory effects of elevated concentrations of dissolved metals on the leaching prokaryotes. The system is suitable for scale-up applications and has the potential to be adapted to different battery chemistries.

Separator is an essential component of lithium-ion batteries (LIBs), which is placed between the electrodes to impede their electrical contact and provide the transport channels for lithium ions. Traditionally, the separator contributes the overall mass of LIBs, thereby reducing the gravimetric capacity of the devices. Herein, a dual-layer redox-active cellulose separator is designed and fabricated to enhance the electrochemical performances of LIBs by introducing NiS. The presented separator is composed of an insulating bacterial cellulose (BC) nanofiber layer and a conductive, and redox-active NiS@BC/carbon nanotubes layer. By using the NiS@BC separator, the discharge capacity of the LiFePO4//Li half battery is enhanced to 117 mAh g-1 at a current of 2C owing to the redox-activity of NiS. Moreover, the functional separator-electrode interface can facilitate the homogenous Li stripping/plating and depress the polarization upon the repeated stripping/plating process. Consequently, the battery containing the redox-active separator exhibits outstanding cycle stability and rate capability. The present study contributes a novel strategy for the developments of functional separators to improve the electrochemical properties of LIBs., Competing Interests: Declaration of competing interest The authors declare that they have no conflict of interest., (Copyright © 2024 Elsevier B.V. All rights reserved.)

H 2 Ti 12 O 25 holds great promise as a high-voltage anode material for advanced lithium-ion battery applications. To enhance its electrochemical performance, control of the crystal orientation and morphology is an effective way to cope with slow Li + -ion diffusion inside H 2 Ti 12 O 25 with severe anisotropy. In this report, Na 2 Ti 6 O 13 nanorods, prepared from Na 2 CO 3 and anatase TiO 2 in molten NaCl medium, were used as a precursor in the synthesis of long single-crystal H 2 Ti 12 O 25 nanorods with reactive facets. The as-prepared H 2 Ti 12 O 25 nanorods with a diameter of 100-200 nm showed higher charge (extraction) specific capacity and better rate performance than previously reported systems. The reversible capacity of H 2 Ti 12 O 25 was 219.8 mAh g -1 at 1C after 100 cycles, 172.1 mAh g -1 at 10C, and 144.4 mAh g -1 at 20C after 200 cycles; these values are higher than those of H 2 Ti 12 O 25 prepared by the conventional soft-chemical method. Moreover, the as-prepared H 2 Ti 12 O 25 nanorods exhibited superior cycle stability with more than 94 % retention of capacity with nearly 100 % coulombic efficiency after 100 cycles at 1C. On the basis of the above results, long single-crystal H 2 Ti 12 O 25 nanorods synthesized in molten NaCl with outstanding electrochemical characteristics hold a significant amount of promise for hybrid electric vehicles and energy-storage systems., (© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The electrochemical performance of lithium ion battery was enhanced by using biochar derived from Cladophora glomerata (C. glomerata) as widespread green macroalgae in most areas of the Iran's Caspian sea coast. By the utilization of the structure of the biochar, micro-/macro-ordered porous carbon with olive-shaped structure was successfully achieved through pyrolysis at 500 °C, which is the optimal temperature for biofuel production, and was activated with HCl. The biochar and HCl treatment biochar (HTB) were applied as anode electrode in lithium ion batteries. Then, electrochemical measurements were conducted on the electrodes via galvanostatic charge-discharge, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) analyses. The electrochemical results indicated a higher specific discharge capacity (700 mAh g -1 ) and good cycling stability for HTB at the current density of 0.1 A g -1 as compared to the biochar. The reason that HTB electrode works better than the biochar could be due to the higher surface area, formation functional groups, removal impurities, and formation some micropores after HCl treatment. The biochar derived from marine biomass and treatment process developed here could provide a promising path for the low-cost, renewable, and environmentally friendly electrode materials. Graphical abstract Algal-biochar into Li-ion Battery.

Rechargeable lithium-ion batteries with high energy and high power density are required in the application of electric vehicles and portable electronics. Herein, we introduce a type of spherical Li-rich cathode material, Li1.2Ni0.2Mn0.6O2, assembled from uniform nanocubes by a facile polyvinylpyrrolidone (PVP)-assisted hydrothermal method. The material with a hierarchical nano-/microstructure exhibits stable high-rate performance. Furthermore, the precipitant (i.e., urea) and the structure-directing agent (i.e., PVP) effectively activated the Li2 MnO3 components in the microscale material to achieve a high specific capacity of 298.5 mAh g(-1) in the first cycle. This Li-rich cathode material still delivered 243 mAh g(-1) at 0.1 C after 200 cycles and the capacity retentions at 0.5, 1, 2, and 5 C were 94.4, 78.7, 76.3, and 67.8% after 150 cycles, respectively. The results make this Li-rich nano-/microstructure a promising cathode material for long-life and high-performance lithium-ion batteries., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Hollow structures of transition-metal oxides, particularly mixed-metal oxides, could be promising for various applications such as lithium-ion batteries (LIBs). Compared to the synthesis of metal oxide hollow spheres by the template method, non-spherical metal oxide hollow hexagonal polyhedra have not been developed to date. Herein, we report the controlled hydrothermal synthesis of a new phase of Co3 V2 O8 ⋅n H2 O hollow hexagonal prismatic pencils (HHPPs), which is composed of uniform structural units. By varying the amount of NaOH in the presence of NH4 (+) and without any template or organic surfactant, the hexagonal prismatic pencils gradually transform from solid into hollow structures, with sizes varying from 5 to 20 μm. The structure of pencils can be preserved only in a limited range of the molar ratio of OH(-) /NH4 (+) . As a new anode material for LIBs, such hollow pencils exhibit impressive lithium storage properties with high capacity, good cycling stability, and superior rate capability., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

We demonstrate multiscale patterned electrodes that provide surface-area enhancement and strong adhesion between electrode materials and current collector. The combination of multiscale structured current collector and active materials (anodes and cathodes) enables us to make high-performance Li-ion batteries (LIBs). When LiFePO4 (LFP) cathode and Li4 Ti5 O12 (LTO) anode materials are combined with patterned current collectors, their electrochemical performances are significantly improved, including a high rate capability (LiFePO4 : 100 mAh g(-1) , Li4 Ti5 O12 : 60 mAh g(-1) at 100C rate) and highly stable cycling (LiFePO4 : capacity retention of 99.8% after 50 cycles at 10C rate). Moreover, we successfully fabricate full cell system consisting of patterned LFP cathode and patterned LTO anode, exhibiting high-power battery performances [capacity of approximately 70 mAh g(-1) during 1000 cycles at 10C rate (corresponding to charging/discharging time of 6 min)]. We extend this idea to Si anode that exhibits a large volume change during lithiation/delithiation process. The patterned Si electrodes show significantly enhanced electrochemical performances, including a high specific capacity (825 mAh g(-1) ) at high rate of 5C and a stable cycling retention (88% after 100 cycle at a 0.1C rate). This simple strategy can be extended to other cathode and anode materials for practical LIB applications., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The miniaturization of power sources aimed at integration into micro- and nano-electronic devices is a big challenge. To ensure the future development of fully autonomous on-board systems, electrodes based on self-supported 3D nanostructured metal oxides have become increasingly important, and their impact is particularly significant when considering the miniaturization of energy storage systems. This review describes recent advances in the development of self-supported 3D nanostructured metal oxides as electrodes for innovative power sources, particularly Li-ion batteries and electrochemical supercapacitors. Current strategies for the design and morphology control of self-supported electrodes fabricated using template, lithography, anodization and self-organized solution techniques are outlined along with different efforts to improve the storage capacity, rate capability, and cyclability., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

[Display omitted] Black phosphorus (BP) has been highly regarded as a favourable candidate for fast-charging anode applications owing to its high theoretical capacity and advantageous charge–discharge platform. However, BP faces challenges related to compromised electrochemical performance resulting from an unstable solid-electrolyte interface (SEI) and substantial volumetric expansion. This study proposes the engineering of an inorganic-dense SEI on the surface of BP-C through the strategic incorporation of lithium fluoride (LiF). The presence of LiF in the system preferentially promotes LiPF 6 adsorption from the electrolyte, facilitating the in-situ formation of a lithium-enriched inorganic SEI film on the BP-C particulate surfaces. This strategic formation effectively mitigates subsequent electrolytic decomposition, accommodates volumetric expansion, and substantially improves the rate capability and cycling stability of the system. Consequently, the BP-LiF-C electrode demonstrates high initial coulombic efficiency of 86.8 % and maintains a steady capacity of 926.1 mAh g−1 over 700 cycles at 2000 mA g−1. Moreover, when paired with a LiFePO 4 cathode, the full cell exhibits long cycling stability, retaining 98.6 % of its capacity after 500 cycles at 2000 mA g−1, and performs at high rate. Therefore, utilising LiF to modulate the interfacial architecture of BP-based electrode composites provide notable guidance to enhance energy storage systems. [ABSTRACT FROM AUTHOR]

The development of anode materials with high rate performance as well as favourable working durability is key for next-generation lithium-ion batteries (LIBs). Here, MgV3O8 is reported as an advanced anode material, using a facile and scalable solution combustion technology. The MgV3O8 anode shows a "near-zero" volume change (<10% over 1000 cycles). This can be explained by a solid-solution Li+ storage mechanism, leading to superior cycling stability. Consequently, the MgV3O8 electrode achieves a remarkable capacity of approximately 102.6 mA h g−1 at 2.0 A g−1, along with a low fading rate of 0.001% per cycle over 3000 cycles. [ABSTRACT FROM AUTHOR]

Silicon (Si) anodes have long been recognized to significantly improve the energy density and fast-charging capability of lithium-ion batteries (LIBs). However, the implementation of these anodes in commercial LIB cells has progressed incrementally due to the immense volume change of Si across its full state-of-charge (SOC) range. Here, we report an anode-tailored full-cell design (ATFD), which incorporates micrometer-sized silicon (µ-Si) alone, for operation over a limited, prespecified SOC range identified as 30-70%. This range allows homogeneous (de)lithiation throughout the electrode, accompanied by an acceptable level of volume change. The ATFD-based cell exhibits 21.3% higher gravimetric energy density than that of its graphite-based counterpart in a commercial 18650 cylindrical cell and 84.6% capacity retention after 500 cycles even at a fast-charging rate of 3 C. This study indicates that the partial, intermediate SOC operation of the µ-Si anode can markedly increase the energy density and boost the fast-charging capability of a LIB cell, a challenging task in traditional cell engineering. [ABSTRACT FROM AUTHOR]

A low-temperature electrolyte was constructed with LiPF6 as the lithium salt, LiDFOB+LiBF4+LiPO2F2 as the lithium salt additives, fluoroethylene carbonate (FEC) + vinylene carbonate (VC) +tris (trimethylsilyl) phosphae (TMSP) as the film-forming additives, and ethylene carbonate (EC) +dimethyl carbonate (DMC) +ethyl methyl carbonate (EMC) as the solvent, and was used to improve the low-temperature (-20 ℃) performance of NCM811(LiNi0.8Co0.1Mn0.1O2) lithium-ion battery. The properties of low-temperature electrolytes were studied by various analytical techniques, and the effects of lithium salts and film-forming additives on the electrochemical properties of lithium-ion batteries were studied. The results show that the low-temperature electrolyte has good cycling stability and lithium deposition performance. Lithium-ion batteries assembled from low-temperature electrolytes have excellent low-temperature electrochemical properties. The first discharge specific capacity is 171.5 mAh/g at-20 ℃ and 0.1 C, and the capacity retention rate is 96.33% for 120 cycles at 1 C. The SEM and TEM results of the electrodes before and after cycling show that the low-temperature electrolyte form a uniform and dense CEI film on the surface of the positive electrode, due to the action of lithium salt and film-forming additives, which restrain the cracking of the positive electrode material and prevent the electrolyte decomposition, effectively improving the cycling stability of lithium-ion batteries at low temperatures. [ABSTRACT FROM AUTHOR]

Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era. Different from traditional methods, this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning, which is used to rapidly and robustly predict polarization-free incremental capacity analysis (ICA) curves in minutes, and physical modeling, which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves. Only measured charging current and voltage signals are used. Results demonstrates that 11 points collected at any starting state-of-charge (SOC) in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error (RMSE) of 0.2774 Ah/V. Accordingly, battery status can be accurately elevated based on their degradation at both macro and electrode levels. Through transfer learning, such a method can also be adapted to different battery chemistries, indicating the enticing potential for wide applications. [ABSTRACT FROM AUTHOR]

The design of artificial solid eletroctrolyte interphase is an important task to minimize capacity losses in Li-ion batteries. Herein, TiO2 created through atomic layer deposition was used as an artificial SEI on Si nanoparticles. Such coating led to substantial improvement of cycling stability when evaluated with FEC-free electrolyte. [ABSTRACT FROM AUTHOR]

Tremendous efforts are made to enhance the energy density of lithium‐ion batteries, among which designing thick electrodes is a promising approach. Traditionally, kinetic effects are considered in constructing thick electrodes, such as decreasing the tortuosity to facilitate ion transport. This work innovatively investigates the coupling effect of kinetics and thermodynamics on electrode processes and conducts a competitive analysis between them by visualizing electrode processes. The results indicate that a sloping equilibrium potential curve facilitates the uniform utilization of electrodes, but severe kinetic constraints render the thermodynamic regulation ineffective. Thus, modifying the thermodynamic properties of the electrode to strengthen the regulatory effect is a promising approach. Kinetic constraints are the inherent factors limiting the capacity release of batteries. An in‐depth analysis reveals that ensuring the hybrid control of ions and electrons can significantly alleviate kinetic reaction heterogeneity. As a proof‐of‐concept, thick electrodes with vertical channels are constructed, enabling thermodynamics to regain dominance in the electrode process, ultimately achieving outstanding capacity retention of 63% at 4C. This work provides a more comprehensive perspective and represents a significant breakthrough in guiding electrode design to achieve a higher energy density. [ABSTRACT FROM AUTHOR]

Electrodes are vital for lithium‐ion battery performance. The primary method for large‐scale electrode production involves wet slurry casting methods, which encounter challenges related to solvent usage, energy consumption, and mechanical stability. Dry processed (DP) electrodes are a promising alternative but struggle with rate capability and mechanical properties. Here, an approach of incorporating 1 wt.% flour into DP electrodes (DP–1%F) through a binder fibrillation strategy is introduced, which enhances the mechanical strength, rate performance, and cycling stability of the electrodes. The cross‐linking of protein and starch in flour, along with the fibrillation of Polytetrafluoroethylene (PTFE), enable the DP–1%F electrode to exhibit robust mechanical properties and high flexibility. Additionally, the incorporation of flour makes the DP electrode primarily create large pores, reducing electrode tortuosity, thereby endowing the DP–1%F electrode with improved kinetic behavior. The robust mechanical properties and improved kinetic behavior suppress the development of irreversible phase transitions and intragranular/intergranular cracks. These characteristics led to the superior cycling stability of the DP–1%F electrodes with a capacity retention of 80.3% after 260 cycles at 2C and 4.5 V (LiNi0.8Co0.1Mn0.1O2). The findings offer valuable insights for the development of high‐power, long‐life DP electrodes, addressing key challenges in lithium‐ion batteries. [ABSTRACT FROM AUTHOR]

Mitigating the growth of dendritic lithium (Li) metal on silicon (Si) anodes has become a crucial task for the pursuit of long‐term cycling stability of high energy density Si‐based lithium‐ion batteries (LIBs) under fast charging or other specific conditions. While it is widely known that Li metal plating on Si‐based anodes may introduce inferior cycling stability and cause safety concerns, the evolution of the anode/material structure and electrochemical performance with Li metal plating remains largely unexplored. A comprehensive quantitative investigation of the hybrid Li storage mechanism, combining the Li alloying/dealloying mechanism and plating/stripping mechanism, has been conducted to explore the effect of Li plating on Si‐based anodes. The findings reveal that Li plating/stripping accounts for the decay of the overall Coulombic efficiency and cycling stability of the hybrid Li storage mechanism. Furthermore, alloying reactions occurring below 0 V encourage the formation of crystalline Li15Si4, which subsequently exacerbates voltage hysteresis. The performance decay is amplified as the ratio of Li plating/stripping capacity increases, or in other words, as the over‐lithiation level rises, thereby posing a threat to the battery's cycling stability. These results provide valuable insights into the design of advanced Si‐based electrodes for high energy density LIBs. [ABSTRACT FROM AUTHOR]

Flexible electrodes are highly desirable for next-generation wearable lithium-ion batteries. To achieve high-capacity flexible electrode materials, SnO2 with high theoretical capacity has been introduced into electrodes and shows promising capacity. However, the electrodes are still confronted with major challenges in terms of inferior rate capability and cycling stability, which are caused by large volume changes of SnO2 during the lithiation/delithiation process. Here, we adopt an adsorption assembly strategy to fabricate a flexible carbon fiber/SnO2@rGO electrode that effectively stabilizes the volume changes of SnO2 and enhances the charge transport kinetics in electrodes. The sandwich-like structure endows the electrode's high flexibility and succeeds in improving both rate capability and cycling stability. The flexible carbon fiber/SnO2@rGO electrode delivers a high capacity of 453 mAh g−1 at 50 mA g−1 and outstanding capacity retention of 88% after 1000 cycles at 2 A g−1. [ABSTRACT FROM AUTHOR]

Lithium plating may occur during charging, especially at high rates or overcharging conditions for lithium-ion batteries (LIBs), which would cause battery capacity degradation and even trigger thermal runaway. Thus, it is essential to detect lithium plating onset during the charging processes. Electrochemical impedance can reveal the dynamic electrode properties of the battery, which is promising for use in battery management systems for the online detection of lithium plating onset. In this article, the impedance at 1 Hz is measured during the over-discharge and fast discharge processes using lithium–graphite half-cells. For half-cells, the variation in graphite electrode potential vs. Li/Li+ during discharging is directly recorded. An equivalent circuit model is proposed and adopted to estimate the real lithium plating reaction overpotential, which is deemed the thermodynamic indicator of lithium plating and is used as validation for the detection of lithium plating onset. Through the auxiliary validation of the estimation of lithium plating overpotential and the shape of incremental capacity curves, the relationship between impedance changes at specific frequency and the lithium plating onset is revealed. The results lay a good foundation for proposing the online diagnostic method of lithium plating onset based on the in situ impedance. [ABSTRACT FROM AUTHOR]

COFs with multiple redox active sites were designed and synthesized, and then composite with CNTs. Finally, the LIBs anode material with high specific capacity and high cycle stability was obtained. [Display omitted] • Two β-ketoenamine-linked COFs with multiple active centers were prepared. • The synergistic effect of CNTs and COFs is utilized to improve the electrochemical performance of the battery. • The LIBs electrode material with high specific capacity and high cycle stability was obtained. • The mechanism of lithium storage in COFs and the cause of electrode activation were verified by ex-situ XPS method. It is essential to advance the development of lithium-ion batteries (LIBs) characterized by high specific capacity and extended cycle life. Covalent organic frameworks (COFs) have emerged as pivotal materials in achieving this objective due to their long-range ordered porous structures and ease of modification. In this work, we designed and synthesized two types of β-ketoenamine-linked COFs, namely TP-3J-COF and TP-3Q-COF, which incorporate multiple redox sites. These COFs were subsequently applied to the anode of LIBs, resulting in the successful fabrication of batteries that demonstrate both high specific capacity and prolonged cycle life. Furthermore, we prepared two composites by in situ growth of COFs on carbon nanotubes (CNTs). The synergistic interaction between the COFs and CNTs enabled the TP-3J-COF@CNT and TP-3Q-COF@CNT composites to achieve maximum specific capacities of 1020 mAh g−1 and 731 mAh g−1, respectively, along with cycle lives exceeding 1400 and 3000 cycles. This research underscores the efficacy of the strategy involving the construction of COFs with multiple redox-active units and their composite formation with CNTs as a robust approach for the development of high-performance LIBs. [ABSTRACT FROM AUTHOR]

Nickel-rich layered oxides are one of the most promising positive electrode active materials for high-energy Li-ion batteries. Unfortunately, the practical performance is inevitably circumscribed by the structural deterioration deriving from the Ni/Li antisite disorder, leading to severe capacity loss and life attenuation. Herein, we propose an economical and facile rejuvenation strategy by employing the magneto-electrochemical synergistic activation targeting the positive electrode in assembled Li-ion batteries. This approach induces a transition of Ni3+ from high-spin to low-spin, reducing the super-exchange interaction of Ni-O-transition metal (TM). Meanwhile, electrochemical reaction drives Li+ from the host material and promotes Ni3+ to reoccupy TM layer, recovering intrinsic Li site and extending cycle life. The strategy demonstrates that low-quality positive electrodes can be converted to high-quality ones. Notably, the method can revitalize an aged Li-ion pouch cell (SiC||NCM811, 8 Ah nominal capacity) via optimizing cation occupancy and increase its capacity by 10% from 6.49 to 7.14 Ah at 1 C, illustrating the benefits of the upcycling process. Severe Ni/Li antisite disorder in nickel-rich layered oxides leads to structural degradation and performance decay in Li-ion batteries. Here, authors report a noninvasive strategy of magnetoelectrochemical synergistic activation to realize ordered cation rearrangement and recovery battery capacity. [ABSTRACT FROM AUTHOR]

Silicon is widely recognized as an ideal anode material due to its high specific capacity, low lithiation potential, high abundance, and environmental friendliness. Nevertheless, the immense volume expansion during the lithiation leads to pulverization of silicon particles, which causes electrode failure with a rapid capacity decay. Herein, the polymerized 1, 3‐dioxolane (PDOL) electrolyte is used to stabilize the micro‐silicon Si anode via in situ polymerization route. The conformality of the quasi‐solid electrolyte suppresses the pulverization of the Si microparticles (SiMPs) effectively and thus alleviates the capacity decay. The SiMPs/PDOL anode shows an excellent initial CE of 97.5% and maintains a reversible capacity of 1837.1 mAh g−1 at 500 mA g−1 after 100 cycles. The Si/PDOL/LiFePO4 full cells also exhibit a stable cycling performance with a capacity retention of 76.3% after 300 cycles. This work provides a new and easy path for the practical application of silicon anode at low cost. [ABSTRACT FROM AUTHOR]

To non‐destructively resolve and diagnose the degradation mechanisms of lithium‐ion batteries (LIBs), it is necessary to cross‐scale decouple complex kinetic processes through the distribution of relaxation times (DRT). However, LIBs with low interfacial impedance render DRT unreliable without data processing and closed‐loop validation. This study proposes a hierarchical analytical framework to enhance timescale resolution and reduce uncertainty, including interfacial impedance reconstruction and multi‐dimensional DRT analysis. Interfacial impedance is reconstructed by eliminating simulated inductive and diffusive impedance based on a high‐fidelity frequency‐domain model. Multi‐dimensional DRT decouples solid electrolyte interphase (SEI) and charge transfer (CT) processes by the reversibility of electrochemical reactions with state of charge (SOC) to characterize electrode kinetic evolution driven by SOC and temperature through timescales and peak area. The findings reveal that reconstructed impedance improves the accuracy of identified time constants by ≈20%. Cross‐scale DRT results reveal that SOCs below 10% at 25 °C effectively distinguish electrode kinetics due to the high correlation between cathodic CT and SOC. Kinetic metrics characterize that anodic SEI or CT are different control steps limiting the low‐temperature performance of different cells. This work underscores the potential of the proposed framework for non‐destructive diagnostics of kinetic evolution. [ABSTRACT FROM AUTHOR]

The cathode affects the capacity, working voltage, and cost of lithium-ion batteries. Although the binder is a small part of the cathode material, it is particularly important to the performance of the batteries. Therefore, the design and development of polymer binders with different structures and characteristics is an important topic. In this paper, an NCM811 cathode (PPC-NCM) was prepared by a solvent-free method using poly (propylene carbonate) (PPC) as the binder, with an active substance loading of 10 mg/cm2. To explore the effect of the PPC binder on the electrochemical performance of the NCM811 cathode, the discharge capacity was 112.2 mAh/g with a 76.1% capacity retention after cycling more than 200 cycles at 1 C, which has a significantly better cycling performance than that of a PVDF-NCM/Li battery. The PPC/NCM/graphite full cells were also assembled to demonstrate the practical application potential of this work. It was shown that PPC as a binder can improve the cycling stability of NCM811/Li and NCM811/graphite full cells. The PPC binder used in the NCM811 cathode not only makes it extremely easy to prepare dry electrodes, but also makes it very simple to recover the electrode material by heating in the case of battery failure. This paper provides a new idea for the industrialization and development of a novel binder. [ABSTRACT FROM AUTHOR]

As an important part of the electrode material of lithium‐ion batteries, the binder significantly affects the forming strength of the solid electrolyte interface (SEI), and also determines the mechanical properties and cycling stability. In the silicon anode, binder have greater effect in the chemical and electrochemical stability because of the volume of the silicon anode changes by more than 300 %. Thus, the development of functional new binders with enhanced properties is one of the keys to mitigating the instability of silicon anodes. This concept first briefly introduces the advantages and disadvantages of conventional electrode binders, then the current research progress of silicon anode binders is briefly summarized based on the different types of interaction forces of binders. Finally, we conclude the properties indicators of silicon anode binders with superior performance in batteries, and comment our previous work in detail. [ABSTRACT FROM AUTHOR]

The ratio of the anode (negative electrode) and cathode (positive electrode) areal capacities (N/P ratio), is an important parameter for Lithium‐ion batteries. Considering the manufacturing tolerance and battery safety, almost all of the batteries keep the N/P ratio > 1. Deviating from this ratio can lead to lithium precipitation on the anode surface, which poses significant risks. Here, by using a gradient structured graphite (Gr) anode, a new design concept is proposed that the N/P ratio could be less than 1, which can effectively achieve higher energy density without sacrificing the battery safety. This is achieved by incorporating a small quantity of silver (Ag) nanoparticles into the bottom layer of the anode (Gr‐Agx), which effectively modulates the concentration polarization of lithium ions along the thickness of the electrode. Moreover, the volumetric energy density of 4 Ah LiCoO2||Gr‐Ag0.5 (N/P = 0.8) pouch cell increases by 14.5% compared with LiCoO2||Gr (N/P = 1.1). Furthermore, the universal applicability and efficacy of the N/P < 1 design paradigm in LiFePO4||Gr cells are validated. [ABSTRACT FROM AUTHOR]

Li-based all-solid-state batteries (ASSBs) are considered feasible candidates for the development of the next generation of high-energy rechargeable batteries. However, ASSBs are detrimentally affected by a limited rate capability and inadequate performance at high currents. To circumvent these issues, here we propose the use of Nb1.60Ti0.32W0.08O5-δ (NTWO) as negative electrode active material. NTWO is capable of overcoming the limitation of lithium metal as the negative electrode, offering fast-charging capabilities and cycle stability. Physicochemical and electrochemical characterizations of NTWO in combination with the Li6PS5Cl (LPSCl) solid-state electrolyte demonstrate that the formation of LiWS2 at the electrode|electrolyte interphase is the main responsible for the improved battery performance. Indeed, when an NTWO-based negative electrode and LPSCl are coupled with a LiNbO3-coated LiNi0.8Mn0.1Co0.1O2-based positive electrode, the lab-scale cell is capable of maintaining 80% of discharge capacity retention after 5000 cycles at 45 mA cm−2 at 60 °C and 60 MPa. All-solid-state batteries (ASSB) are designed to address the limitations of conventional lithium ion batteries. Here, authors developed a Nb1.60Ti0.32W0.08O5-δ negative electrode for ASSBs, which improves fast-charging capability and cycle stability. [ABSTRACT FROM AUTHOR]

One-step hydrothermally synthesized over-oxidized Mo3Se4 with enriched selenium exhibited a specific capacity of 1006.75 mA h g−1 at 0.1C. It retained 71% of the initial value during the rate performance test. This novel electrode demonstrated a large specific capacity of 897.62 mA h g−1 at 0.4C at the end of 332 cycles. The exceptional results for mixed phase Mo3Se4 suggest its structural and chemical stability. [ABSTRACT FROM AUTHOR]

High‐nickel layered cathodes exhibit great promise in advancing high‐energy‐density batteries owing to their significant advantages in high energy capacity and low cost, but they suffer severe structural and interfacial deterioration during cycling, resulting in safety risk and reduced cycle life. Herein, drawing inspiration from the low melting point infusion capability of Sb2Se3, a three‐pronged strategy aimed at simultaneously achieving coating on primary and secondary particles surface, Sb doping and elongated and slimed primary particle morphology is proposed and developed to fortify the structural and interfacial stability of high‐nickel LiNi0.9Co0.05Mn0.05O2 (NCM90) cathode. The "melted and infused" Sb2Se3 plays a beneficial role in the defensive effect on primary and secondary particle's surfaces, mitigating the interfacial deterioration. In addition, the enhanced structural stability is achieved by both Sb5+ doping and regulated primary particle morphology, contributing to the alleviated particle breakage and ultimately reinforced cycling stability. Consequently, the Sb2Se3‐NCM90 electrodes significantly improve cycling performance, which maintain higher capacity retentions of 96.6% at 4.3 V after 100 cycles and 80.2% at 1C/5C after 500 cycles. The proposed coating‐doping‐microstructure regulation three‐in‐one strategy for improving the cycling stability of high‐nickel NCM cathodes offers innovative ideas for the design and advancement of high‐energy‐density lithium‐ion batteries. [ABSTRACT FROM AUTHOR]

Purpose: This paper aims at analyzing the potential of new materials in magnesium-ion batteries (MIBs) with a particular focus on options for electrodes and electrolyte solutions while also carefully considering the barriers to their entry in this application for MIBs, with a particular focus on the material options for electrodes and electrolyte solutions. Design/methodology/approach: Potential materials for MIBs were examined for sustainability, safety and efficiency to develop the sustainable and well-working MIBs. Findings: For anode materials, the use of Mg-bismuth alloys has shown promise, whereas Chevrel phases or layered molybdenum disulfide have potential as cathode materials. Potential electrolytes range from traditional materials to the development of tailored solid-state and liquid-based options. Originality/value: This study considers the growing need for Mg-based ion batteries, as well as the need for suitable electrode and electrolyte materials and analyzes suitable options. Peer review: The peer review history for this article is available at: https://publons.com/publon/10.1108/ILT-03-2023-0081/ [ABSTRACT FROM AUTHOR]

The design of electrode architecture plays a crucial role in advancing the development of next generation energy storage devices, such as lithium-ion batteries and supercapacitors. Nevertheless, existing literature lacks a comprehensive examination of the property tradeoffs stemming from different electrode architectures. This prospective seeks to bridge this gap by focusing on the diverse nanocomposite electrode architectures. Furthermore, the challenges related to designing well-defined electrode architectures for enhanced energy storage are discussed. Finally, this review addresses the interdisciplinary nature of this field by examining the integration of advanced characterization and fabrication techniques, and machine learning methodologies for electrode optimization. Designing electrodes with controlled architecture and leveraging emerging tools such as in situ characterization, additive manufacturing methods, and machine learning facilitates the advancement of energy storage systems. [ABSTRACT FROM AUTHOR]

The poor interfacial stability and undesirable cycling performance caused by their dramatic volume change hinder the large-scale commercial application of SiOx materials for high-energy-density lithium-ion batteries. Herein, a simple two-step carbonization process is employed to prepare highly pyrrolic-nitrogen-doped carbon modified SiOx anode materials (SiOx@NC). The designed SiOx@NC materials exhibit high electron conductivity and favorable electrochemical kinetics. As expected, the SiOx@NC electrode delivers a high specific capacity of 1003.46 mA h g−1 after 200 cycles at 500 mA g−1. The NCM622‖‖SiOx@NC full cell also demonstrates excellent cycling stability and rate performance. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries are widely used in portable electronic devices because of their high energy and power density. To enhance the energy density of these batteries, one strategy involves increasing the active material loading by increasing the thickness of the electrodes. In previous studies, we demonstrated that powder extrusion moulding (PEM) is a scalable and efficient method for producing additive-free LTO and LFP ceramic electrodes, which exhibit remarkable electrochemical performance with thicknesses up to 500 μm. This study focuses on the preparation and optimisation of the entire manufacturing process for thick ceramic electrodes of LiCoO 2 (LCO) with a high mass loading of 180 mg cm−2 using the PEM process. Different powder loadings of mixtures of LCO and a thermoplastic multi-component binder were explored to obtain a formulation suitable for rheology. The optimal formulation comprises 60 vol% of powder. After binder removal via a combination of solvent and thermal treatment, followed by air sintering, parts with varying porosities were obtained. Striking a balance between porosity and thermal degradation is crucial for achieving optimal electrochemical behaviour. Electrochemical evaluations of the electrodes sintered at 900 °C and 1000 °C revealed areal capacity values as high as 17 mAh cm−2 at C/25 and 7 mAh cm−2 at C/6.25, respectively. These values far exceed the 1−2 mAh cm−2 obtained from commercial LCO electrodes. These results indicate a strategy for the production of electrodes to fabricate lithium-ion batteries with a low ratio of inactive materials and, therefore, with higher energy densities. [ABSTRACT FROM AUTHOR]

Titanium niobium oxides (TNO) are chemically recovered from a mineral composed of cassiterite, columbotantalite, rutile and wollastonite. The process involves a series of steps, including pyrometallurgical processes, leaching, and liquid-liquid extraction. It takes advantage of the naturally occurring Ti in the extracted mineral, avoiding the separation of Ti and Nb to directly obtain the valuable Ti–Nb–O compounds. Two compositions can be obtained (Ti 2 Nb 10 O 29 or TiNb 2 O 7 , named TNO-cal and TNO-black, respectively) depending on the thermal treatment after the chemical separation from the original mineral. These compounds have been characterized to describe their composition, morphology and crystallographic properties. The recovered material, without any further purification or functionalization, has been studied as anodes in Lithium-ion batteries (LIBs). Different electrochemical behavior has been observed for voltage ranges of 1–3 V and 0.01–3 V, being the second range which gives best results. In the 1–3V range, TNO-black exhibits a reversible capacity of up to 101.4 mA h g−1 at 1C and maintains 97 % capacity retention after 200 cycles, this is mainly due to Li + insertion/de-insertion processes. Additionally, when expanding the voltage range down to 0.01V, TNO-black displays a specific capacity of approximately 139.1 mA h g−1 after 200 cycles at 1C, whereas TNO-cal reaches a specific capacity of 169 mA h g−1. Extended cycling experiments at a 1C rate for both electrodes reveal that after 200 cycles samples deliver efficiencies relative to the maximum discharge capacity values of 83.4 % (TNO-cal) and 64.4 % (TNO-black), with mean coulombic efficiencies of 97.5 %. These results demonstrate that the recovered materials can effectively function as anodes for LIBs, offering promising application potential, despite the presence of residual silica from the mining process. [ABSTRACT FROM AUTHOR]

Dual‐ion batteries (DIBs) represent a promising alternative for lithium ion batteries (LIBs) for various niche applications. DIBs with polymer‐based active materials, here poly(2,2,6,6‐tetramethylpiperidinyl‐N‐oxyl methacrylate) (PTMA), are of particular interest for high power applications, though they require appropriate electrolyte formulations. As the anion mobility plays a crucial role in transport kinetics, Li salts are varied using the well‐dissociating solvent γ‐butyrolactone (GBL). Lithium difluoro(oxalate)borate (LiDFOB) and lithium bis(oxalate)borate (LiBOB) improve cycle life in PTMA||Li metal cells compared to other Li salts and a LiPF6‐ and carbonate‐based reference electrolyte, even at specific currents of 1.0 A g−1 (≈10C), whereas LiDFOB reveals a superior rate performance, i. e. ≈90 % capacity even at 5.0 A g−1 (≈50C). This is attributed to faster charge‐transfer/mass transport, enhanced pseudo‐capacitive contributions during the de‐/insertion of the anions into the PTMA electrode and to lower overpotentials at the Li metal electrode. [ABSTRACT FROM AUTHOR]

We introduce free-standing FeS2/carbon microlattice composites as electrodes for lithium-ion batteries through 3D printing. The computer-aided design allows for any shape. The microlattice features aligned microchannels, promoting ion transfer, while the carbon skeleton facilitates electron transfer. Overall, this study shows 3D printing is highly promising in advancing sustainable energy applications. [ABSTRACT FROM AUTHOR]

A straightforward hydrothermal technique was employed to develop binder-free CaMoO 4 electrodes that can be utilized as electrodes in Li-ion batteries. Structural analysis was employed to validate the tetragonal scheelite structure and exceptional crystallinity of the electrodes. Examination with scanning electron microscopy revealed that the electrodes exhibited diverse morphologies, including nanorods, sheets, and flowers. The composition of CaMoO 4 was confirmed by analyzing the X-ray photoelectron spectroscopy data, which revealed distinct binding energy peaks corresponding to Ca, Mo, and O. The presence of these elements in the nanostructures was further confirmed by transmission electron microscopy and energy dispersive spectroscopy mapping. Electrochemical tests showed that CaMoO 4 (DIW@EG sample electrode) composite electrodes demonstrated an impressive primary discharge specific capacity of 2383 mAh g−1 and a high rate capacity of 1034 mAh g−1 at 0.5 A g−1 current density. Additionally, a full cell combining LCO with CaMoO 4 achieved a remarkable capacity of 321 mAh g−1 at a current density of 0.5 A g−1, presenting it as a viable substitute for the traditional LCO//graphite system. [ABSTRACT FROM AUTHOR]

The Li‐rich antifluorite‐type oxides Li5FeO4, Li5.5Fe0.5Co0.5O4 and Li6CoO4 have been investigated as positive electrode materials for Li‐ion batteries in a combined operando XANES and XRD experiment. All materials show a similar two‐step behaviour upon initial charge (termed Stage I and Stage II), and reversibility of subsequent cycling depends upon whether the initial charge cycle is terminated following Stage I or allowed to proceed through Stage II. By tracking the energetic evolution of the XANES pre‐edge feature present in both Fe and Co K‐edge spectra, as well as the evolution of X‐ray diffractograms during charge and discharge, we correlate the changes in chemical coordination and oxidation states in both species and the structural changes to the electrochemical potential profile, and infer the role of anionic redox processes. [ABSTRACT FROM AUTHOR]

Developing new battery configurations is a time‐consuming process, electrochemical models can be employed to expedite the process by predicting the performance of battery designs. An electrochemical pseudo‐two‐dimensional modeling framework is created for both LNMO|LiPF6 in EC/PC/sulfolane|Gr and LNMO|PVdF GPE with 1.15 M LiPF6 in EC/PC/FEC/sulfolane|Gr configurations with gelifiable electrodes, leveraging the experimental characterization of battery components for enhanced accuracy. Parametrization experiments include quasi‐open circuit potential, galvanostatic intermittent titration technique, electrochemical impedance spectroscopy, microscopy and the four‐point resistance method. The modeling framework is initiated at full coin cell level and subsequently extended to encompass monolayered, 200 mAh and 500 mAh multilayered pouch cells. Experimental validation, through voltage‐capacity measurements, ensures the accuracy of the models. The discharge curves indicate that cells incorporating GPE show similar performance with liquid electrolytes. The impact of increasing current rates on performance is examined by scrutinizing the polarization trends during discharge and the Li‐ion concentration in the electrolyte phase. Elevated C‐rates induce heightened polarization, detrimentally influencing performance. Importantly, the developed model for full coin cells can be seamlessly expanded to encompass 500 mAh multilayered pouch cells without requiring additional component characterization. This versatility allows the modeling framework to be a valuable tool for evaluating the performance of battery configurations at higher levels. [ABSTRACT FROM AUTHOR]

Electrochemical impedance spectroscopy (EIS) is a powerful characterization technique for the in-depth investigation of kinetic/transport parameters detection, reaction mechanism understanding, and degradation effects exploration in lithium-ion battery (LIB) systems. However, due to the lack of standardized criterion/paradigm, severe misinterpretations occur frequently during an EIS measurement. In this paper, the significance of instrumental accuracy is described and the character/principle of selection on the simulation model is illuminated/proposed, showing that an adequate precision device and an appropriate fitting model are a prerequisite for a correct EIS analysis. Moreover, the drawbacks of conventional two-electrode EIS experiments for typical coin-type cells are rigorously pointed out by comparison with the ideal three-electrode configuration, where the real impedance information of the cathode would be masked by the sum of both the anode film resistance response and the unavoidable inductive loop signal. The three-electrode case enables efficient accurate observations on individual electrodes, thus facilitating abundant and useful information acquisition. Consequently, devices with a sufficient accuracy, rational simulation models, and advanced three-electrode cells are distinctly illustrated as standardized criterion/paradigm for EIS characterizations, which are essentially important for electrode and interface modifications in LIBs. [ABSTRACT FROM AUTHOR]

MXene is investigated as an electrode material for different energy storage systems due to layered structures and metal‐like electrical conductivity. Experimental results show MXenes possess excellent cycling performance as anode materials, especially at large current densities. However, the reversible capacity is relatively low, which is a significant barrier to meeting the demands of industrial applications. This work synthesizes N‐doped graphene‐like carbon (NGC) intercalated Ti3C2Tx (NGC‐Ti3C2Tx) van der Waals heterostructure by an in situ method. The as‐prepared NGC‐Ti3C2Tx van der Waals heterostructure is employed as sodium‐ion and lithium‐ion battery electrodes. For sodium‐ion batteries, a reversible specific capacity of 305 mAh g−1 is achieved at a specific current of 20 mA g−1, 2.3 times higher than that of Ti3C2Tx. For lithium‐ion batteries, a reversible capacity of 400 mAh g−1 at a specific current of 20 mA g−1 is 1.5 times higher than that of Ti3C2Tx. Both sodium‐ion and lithium‐ion batteries made from NGC‐Ti3C2Tx shows high cycling stability. The theoretical calculations also verify the remarkable improvement in battery capacity within the NGC‐Ti3C2O2 system, attributed to the additional adsorption of working ions at the edge states of NGC. This work offers an innovative way to synthesize a new van der Waals heterostructure and provides a new route to improve the electrochemical performance significantly. [ABSTRACT FROM AUTHOR]

To recharge lithium‐ion batteries quickly and safely while avoiding capacity loss and safety risks, a novel electrode design that minimizes cell polarization at a higher current is highly desired. This work presents a dual‐layer electrode (DLE) technology via sequential coating of two different anode materials to minimize the overall electrode resistance upon fast charging. Electrochemical impedance spectroscopy and distribution of relaxation times analysis revealed the dynamic evolution of electrode impedances in synthetic graphite (SG) upon a change in the state of charge (SOC), whereas the natural graphite (NG) maintains its original impedance regardless of SOC variation. This disparity dictates the sequence of the NG and SG coating layers within the DLE, considering the temporal SOC gradient developed upon fast charging. Simulation and experimental results suggest that DLE positioning NG and SG on the top (second‐layer) and bottom (first‐layer), respectively, can effectively reduce the overall resistance at a 4 C‐rate (15‐min charging), demonstrating two times higher capacity retention (61.0%) over 200 cycles than its counterpart with reversal sequential coating, and is higher than single‐layer electrodes using NG or NG/SG binary mixtures. Hence, this study can guide the combinatorial sequence for multi‐layer coating of various active materials for a lower‐resistivity, thick‐electrode design. [ABSTRACT FROM AUTHOR]

The emergence of Li–SOCl2 batteries in the 1970s as a high-energy-density battery system sparked considerable interest among researchers. However, limitations in the primary cell characteristics have restricted their potential for widespread adoption in today's sustainable society. Encouragingly, recent developments in alkali/alkaline-earth metal–Cl2 (AM–Cl2) batteries have shown impressive reversibility with high specific capacity and cycle performance, revitalizing the potential of SOCl2 batteries and becoming a promising technology surpassing current lithium-ion batteries. In this review, the emerging AM–Cl2 batteries are comprehensively summarized for the first time. The development history and advantages of Li–SOCl2 batteries are traced, followed by the critical working mechanisms for achieving high rechargeability. The design concepts of electrodes and electrolytes for AM–Cl2 batteries as well as key characterization techniques are also demonstrated. Furthermore, the current challenges and corresponding strategies, as well as future directions regarding the battery are systematically discussed. This review aims to deepen the understanding of the state-of-the-art AM–Cl2 battery technology and accelerate the development of practical AM–Cl2 batteries for next-generation high-energy storage systems. [ABSTRACT FROM AUTHOR]

The safety concerns associated with current lithium-ion batteries are a significant drawback. A short-circuit within the battery's internal components, such as those caused by a car accident, can lead to ignition or even explosion. To address this issue, a polymer shear thickening electrolyte, free from flammable solvents, has been developed. It comprises a star-shaped oligomer derived from a trimethylolpropane (TMP) core and polyether chains, along with the inclusion of 20 wt.% nanosilica. Notably, the star-shaped oligomer serves a dual function as both the solvent for the lithium salt and the continuous phase of the shear thickening fluid. The obtained electrolytes exhibit an ionic conductivity of the order of 10−6 S cm−1 at 20 °C and 10−4 S cm−1 at 80 °C, with a high Li+ transference number (t+ = 0.79). A nearly thirtyfold increase in viscosity to a value of 1187 Pa s at 25 °C and a critical shear rate of 2 s−1 were achieved. During impact, this electrolyte could enhance cell safety by preventing electrode short-circuiting. [ABSTRACT FROM AUTHOR]

In this paper, we introduce an environmentally friendly approach to recycle used batteries and recover highly valuable manganese-based cathode materials. This study demonstrates the feasibility of fast plasma pyrolysis to recover LiMn2O4 electrode materials (e.g., lithium manganese oxide, LMO) and demonstrate their reuse in newly assembled Li-ion cells. The electrochemical performance of as-recycled cathodes shows an initial discharge capacity of 72 mAh/g and is stable for 100 cycles at 0.1 C. After adding 20 mole % of excess LiOH, the recycled LMO after relithiation at 660 °C can deliver an initial discharge capacity of 96 mAh/g and retain a decent discharge capacity of 88 mAh/g after 50 cycles at a 0.2 C rate. Without relithiation, the as-recycled LMO cathode after heating at 1000 °C delivers the best electrochemical cycling performance, including an initial discharge capacity of 94 mAh/g and 50th cycle capacity of 91 mAh/g at a 0.2 C rate. This study highlights a feasible approach for recycling electrode materials in spent LIBs. Recycling of lithium-ion batteries and especially electrode materials is crucial for the sustained growth of the lithium-ion battery industry and reduced environmental issues. [ABSTRACT FROM AUTHOR]

Organic carbonyl electrode materials offer promising prospects for future energy storage systems due to their high theoretical capacity, resource sustainability, and structural diversity. Although much progress has been made in the research of high-performance carbonyl electrodematerials, systematic and in-depth studies on the underlying factors affecting their electrochemical properties are rather limited. Herein, five polyimides containing different types of diamine linkers are designed and synthesized as cathode materials for Li-ion batteries. First, the incorporation of carbonyl groups increases the active-site density in both conjugated and non-conjugated systems. Second, increased molecular rigidity can improve the accessibility of the active sites. Third, the introduction of the conjugated structure between two carbonyl groups can increase the reactivity of the active sites. Consequently, the incorporation of carbonyl structures and conjugated structures increases the capacity of polyimides. PTN, PAN, PMN, PSN, and PBN exhibit 212, 198, 199, 151, and 115 mAh -1 at 50 mA -1, respectively. In addition, the introduction of a carbonyl structure and a conjugated structure is also beneficial for improving cycling stability and rate performance. This work can deepen the understanding of the structure-function relationship for the rational design of polyimide electrode materials and can be extended to the molecular design of other organic cathode materials. [ABSTRACT FROM AUTHOR]

The low energy density, unsatisfied cycling performance, potential safety issue and slow charging kinetics of the commercial lithium-ion batteries restrained their further application in the fields of fast charging and long-haul electric vehicles. Monoclinic TiNb2O7 (TNO) with the theoretical capacity of 387 mAh g-1 has been proposed as a high-capacity anode materials to replace Li4Ti5O12. In this work, homovalent doping strategy was used to enhance the electrochemical performance of TiNb2O7 (TNO) by employing Zr to partial substitute Ti through solvothermal method. The doping of Zr4+ ions can enlarge the lattice structure without changing the chemical valence of the original elements, refine and homogenize the grains, improve the electrical conductivity, and accelerate the ion diffusion kinetics, and finally enhance the cycle and rate performance. Specifically, Z0.05-TNO shows initial discharge capacity of as high as 312.2 mAh g-1 at 1 C and 244.8 mAh g-1 at 10 C, and still maintains a high specific capacity of 171.3 mAh g-1 after 800 cycles at 10 C. This study provides a new strategy for high-performance fastcharging energy storage electrodes. [ABSTRACT FROM AUTHOR]