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In the UAV-based urban delivery setting, the battery capacity serves as one of the key factors affecting the delivery range of drones. For a typical multi-rotor unmanned aerial vehicle (UAV), the maximum effective working range of a lithium battery for a single flight leg is approximately 20 km. In practice, the lithium battery is replaced each time the UAV completes a delivery, even though the remaining power of the replaced lithium battery is still capable of supporting the following flight legs. Therefore, the one-order-one-swapping strategy significantly brings down the battery utilisation as well as the efficiency of the delivery system. In the present paper, the UAV-based delivery problem with battery swapping decision is considered, where multiple en route pickup and deliveries are allowed. To obtain optimal decisions in terms of flight route, time and location of each battery swapping, a branch-and-price-and-cut algorithm is introduced. First we formulate this problem as a mixed integer linear programming (MILP) model, and then decompose it into a master problem and a pricing sub-problem, where the master problem is considered as a set covering model, and the sub-problem as an elementary shortest path problem with resource constraints (ESPPRC). To speed up the process of column generation, efficient heuristics are also integrated to provide basic feasible solutions. In the pricing sub-problem, a combination of heuristic algorithm and dynamic programming is implemented to improve the computational efficiency. In the numerical experiments, the proposed algorithm is tested on various scales of UAV-based urban delivery instances, the performance of which is analysed and compared with the off-the-shelf commercial solver. [ABSTRACT FROM AUTHOR]

Tiny NiSnO3 nanoparticles with the assistance of polyvinylpyrrolidone (PVP) are prepared to uniformly and stably "bond" on the surface of graphene to form a stable NiSnO3/RGO-PVP structure. At the same time, the excellent performance of lithium-ion batteries (LIBs) with the use of NiSnO3/RGO-PVP structure is verified through a dual combination of experiment and theory. The resulting NiSnO3/RGO-PVP structure enhanced the performance of LIBs with high cycling stability and better rate capability; even after undergoing rate performance tests at different high current densities, the NiSnO3/RGO-PVP electrode can still reach a capacity of 624 mA h g−1 at 200 mA g−1 after 400 cycles. The superior electrochemical performance of NiSnO3/RGO-PVP nanocomposites can be attributed to the synergistic effects between tiny NiSnO3 nanoparticles synthesized with the assistance of PVP and RGO, which can be verified through first-principles calculations based on DFT. The charge transfer between NiSnO3 and RGO through an electron density difference indicates a strong interaction between the two. Meanwhile, the low adsorption energies (−3.914, −0.77, and −0.65 eV), low diffusion barriers (0.025, 0.49, and 0.141 eV), and high diffusion coefficients (1.79 × 10−3, 5.38 × 10−11, and 2.97 × 10−5 cm2 s−1) of lithium ions at three different positions indicate the excellent rate performance of the NiSnO3/RGO-PVP heterostructure, which is consistent with experimental results. This work analyzes the excellent electrochemical performance of NiSnO3/RGO-PVP from the experimental results and supports the reliability of the experimental results through theoretical calculations. [ABSTRACT FROM AUTHOR]

The pursuit of advanced materials to meet the escalating demands of energy storage system has led to the emergence of vertical graphene (VG) as a highly promising candidate. With its remarkable strength, stability, and conductivity, VG has gained significant attention for its potential to revolutionize energy storage technologies. This comprehensive review delves deeply into the synthesis methods, structural modifications, and multifaceted applications of VG in the context of lithium–ion batteries, silicon-based lithium batteries, lithium–sulfur batteries, sodium–ion batteries, potassium–ion batteries, aqueous zinc batteries, and supercapacitors. The review elucidates the intricate growth process of VG and underscores the paramount importance of optimizing process parameters to tailor VG for specific applications. Subsequently, the pivotal role of VG in enhancing the performance of various energy storage and conversion systems is exhaustively discussed. Moreover, it delves into structural improvement, performance tuning, and mechanism analysis of VG composite materials in diverse energy storage systems. In summary, this review provides a comprehensive look at VG synthesis, modification, and its wide range of applications in energy storage. It emphasizes the potential of VG in addressing critical challenges and advancing sustainable, high-performance energy storage devices, providing valuable guidance for the development of future technologies. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs) hold great promise for rechargeable batteries. However, the synthesis of COFs with abundant active sites, excellent stability, and increased conductivity remains a challenge. Here, chemically stable fully sp2 carbon‐conjugated COFs (sp2c‐COFs) with multiple active sites are designed by the polymerization of benzo[1,2‐b:3,4‐b′:5,6‐b′′]trithiophene‐2,5,8‐tricarbaldehyde) (BTT) and s‐indacene‐1,3,5,7(2H,6H)‐tetrone (ICTO) (denoted as BTT‐ICTO). The morphology and structure of the COF are precisely regulated from "butterfly‐shaped" to "cable‐like" through an in situ controllable growth strategy, significantly promoting the exposure and utilization of active sites. When the unique "cable‐like" BTT‐ICTO@CNT is employed as lithium‐ion batteries (LIBs) cathode, it exhibits exceptional capacity (396 mAh g−1 at 0.1 A g−1 with 97.9 % active sites utilization rate), superb rate capacity (227 mAh g−1 at 5.0 A g−1), and excellent cycling performance (184 mAh g−1 over 8000 cycles at 2.0 A g−1 with 0.00365 % decay rate per cycle). The lithium storage mechanism of BTT‐ICTO is exhaustively revealed by in situ Fourier transform infrared, in situ Raman, and density functional theory calculations. This work provides in‐depth insights into fully sp2c‐COFs with multiple active sites for high‐performance LIBs. [ABSTRACT FROM AUTHOR]

Since the safety and costs of current lithium-ion batteries are nonideal, engineering a new energy-storage systems is needed. Mag-nesium/lithium hybrid-ion batteries (MLHBs) combining fast kinetics of Li ions and a dendrite-free Mg anode are promising. Here, we describe our development of an MLHB using lamellar SnSe2/SnSe/SnO2 as cathode material and an all-phenyl complex (APC)-based electrolyte. The multi-layered cathode material generated from a hierarchical precursor is conducive to diffusion of Li+ and Mg2+ ions, and buffers volumetric changes efficiently. After 2000 cycles at 1.0 A g-1 the battery shows a specific capacity of 233 mA h g-1 and a Coulombic efficiency of 100%. It also shows excellent rate performances. These findings suggest that the cathode design working with optimized electrolyte will find many applications for high-performance energy-storage systems. [ABSTRACT FROM AUTHOR]

Gelation of sulfolane-based highly concentrated electrolytes using a partially fluorinated polymer enhances the Li-ion transference number of the electrolytes because acidic protons surrounded by fluorine atoms in the polymer network trap anions, and the high Li+ transference number is effective in suppressing the concentration polarization in Li batteries. [ABSTRACT FROM AUTHOR]

Garnet based solid-state electrolyte Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) is one of the most promising electrolytes for advanced all-solid-state lithium batteries. However, the ceramic electrolyte is difficult to densify under normal sintering conditions, and hence the Li+ transportation via grain boundary is significantly limited by the loose contact between electrolyte granules, resulting in a high Li+ ionic impedance. Herein, we report a novel 2-step approach to obtain a relatively dense LLZTO ceramic pellet by a special Al-doping method, in which the Al was derived from the erosion of the corundum milling beads by LiOH during ball milling. This approach enables the simultaneous distribution of the aluminum (Al) within the LLZTO lattice and uniformly within the grain boundary, serving as a sintering aid, effectively boosts the fusion of grain boundary and reduced the failure rate during the sintering process. The ceramic pellet had a conductivity of 8.13 × 10−4 S cm−1, higher than that without Al-doping or using Al 2 O 3 as dopant. This method provides an easier way to sinter the garnet ceramic electrolyte. [ABSTRACT FROM AUTHOR]

Surface modification of separators with inorganic oxide ceramics such as SiOx, Al2O3, and TiO2 has emerged as a promising strategy to suppress lithium dendrite growth in lithium metal batteries, thereby enhancing safety and extending battery life. However, the binder‐dependent nature of these modifications often leads to increased separator thickness and a heightened risk of detachment during lithium plating, ultimately compromising both battery performance and energy density. In this study, a conformal, ultrathin (≈20 nm) SiOx coating with strong covalent bonding is grown on a porous separator through a liquid polymer‐derived method. Compared to the pristine polyethylene (PE) separators, this SiOx‐co‐PE separator exhibits significantly improved electrolyte wettability, mechanical strength, and thermal stability without any increase in thickness, leading to vastly enhanced cycling stability and dendrite resistance in cells with Li metal anodes. In a practical demonstration, a 402.9 Wh·kg−1 Li‐S pouch cell, with a high sulfur loading of 9 mg cm−2 and a low E/S ratio of 3.3 µL mg−1, is assembled with the SiOx‐co‐PE separator, achieving stable cycling over 70 cycles at 25 °C. [ABSTRACT FROM AUTHOR]

Hypothesis: Porous carbon microspheres (PCMs) with embedded tin di‐oxide (SnO2) quantum dots (QDs) (P‐SnO2@PCMs) are synthesized and employed as polysulfide barriers to enrich the electrochemical properties. Experiments: This composite structure is prepared by spray drying procedure and followed by heat‐treatment, resulting in well‐arranged macropores with a diameter of 59 nm generated by the polystyrene (PS) nanobeads (ϕ = 150 nm) decomposition. P‐SnO2@PCMs is functioned as an electrocatalytic interlayer and offer advantages such as reduced diffusion length for charged particles that guarantees immediate transfer, improved electrode wetting due to efficient electrolyte infiltration, and accommodation of large volume fluctuations during the redox reactions. Furthermore, the incorporation of polar SnO2 QDs within the microspheres allows for efficient chemical confinement and alteration of trapped polysulfide species due to catalytic activity, leading to an extensive use of the active material. Findings: Advancing from the nanostructural eminence, lithium–sulfur (Li–S) cells paired with P‐SnO2@PCMs‐coated separator and conventional sulfur electrode showed outstanding rate performance (321 mA h g−1 at 2.0 C) and prolonged cyclic steadiness at 0.1 C. This innovative synthesis strategy provides valuable insights for developing novel nanostructures applicable to various rechargeable devices. [ABSTRACT FROM AUTHOR]

The construction of poly‐dioxolane (PDOL) solid‐state electrolytes by in situ polymerization is an effective way to achieve high performance lithium‐metal batteries. However, the poor electrochemical stability and safety issues of linear PDOL limit their further application. In this work, a multifunctional crosslinker has been introduced to construct a flame retardant crosslinked quasi solid‐state electrolyte (FCDOL). Due to the synergistic effect of the crosslinked network, the prepared FCDOL achieves excellent room temperature ionic conductivity (0.72 mS cm−1), high Li+ transference number (0.655), wide electrochemical stabilization window (4.8 V vs Li/Li+), and impressive performance when matched with lithium metal anodes (>4000 h plating/stripping) and high‐voltage cathodes, and the corresponding pouch cells can withstand abusive tests such as bending and cutting, encouraging that in situ polymerization of SPEs provides new insights into high‐energy density and high‐safety solid‐state batteries. [ABSTRACT FROM AUTHOR]

Garnet‐type solid‐state electrolytes (SSEs) exemplified by Li6.5La3Zr1.5Ta0.5O12 (LLZT) are chemically unstable when exposed to air, leading to the formation of impurities and poor wettability with Li metal. Herein, a protocol to address this Li/LLZT interface challenge is demonstrated by constructing a lithiophilic MgF2 nanofilm on the LLZT pellet. Specifically, a solution‐based process is developed for the surface engineering of LLZT, utilizing magnesium trifluoroacetate (MTF) as the molecular precursor while poly(acrylic acid) (PAA) as the coordinating agent in a sol‐gel process. It is demonstrated that a facile spin‐coating treatment followed by high‐temperature annealing reliably forms crack‐free MgF2 nanofilms with precise thickness control. Introduction an MgF2 interlayer transforms the LLZT pellet into a highly lithophilic, facilitating close contact with the lithium anode, thereby leading to a significantly reduced interfacial resistance from 1190 Ω cm2 to 6 Ω cm2. Such an interfacial engineering enables stable cycling of full batteries with high reversibility and rate capability using commercial LiFePO4 and LiNi0.83Co0.07Mn0.1O2 as cathodes. This study unfolds the possibility of a solution‐based method as a facile and scalable process for the construction of fluoride nanofilms, which is promising to address the critical interfacial challenges of solid‐state batteries (SSBs) to facilitate its practical applications. [ABSTRACT FROM AUTHOR]

Rechargeable lithium batteries (LBs) are considered the most promising electrochemical energy storage systems for utilizing renewable energies like solar and wind, ushering society into an electric era. However, the development of LBs faces challenges due to interfacial issues caused by side reactions between existing electrode and electrolyte materials. Magnetron sputtering (MS), a type of physical vapor deposition technology, offers solutions with its wide material selection, gentle deposition process, high uniformity of nano/micro‐scale thin films, and strong thin‐film adhesion. This review outlines the main operating principles of MS technology and explores its advanced applications in interfacial modification of various cathodes, anodes, separators, solid‐state electrolytes, and thin‐film LBs integrated with other microelectronic devices. Furthermore, the review discusses the potential of MS technology to accelerate scientific research and industrial progress toward higher‐performance LBs, advancing human society. [ABSTRACT FROM AUTHOR]

Various advanced sources have been developed to cope with the exponential need for world energies, such as hydrogen production, photovoltaic solar cells, lithium batteries and fuel cells, etc. Among these, fuel cells are better owing to their power production, renewability, and green natural technology. In fuel cells, chemical energy is converted into electrical energy with the help of an electrochemical device, having three major components, i.e. electrodes, electrolytes and catalysts. Bismuth-based materials would be a good choice to develop an efficient fuel cell and can be used as electrodes, electrolytes, and catalysts. Bi2SiO5@NG(NG = nitrogen-doped graphene) is a Bi-based nano-composite used as a cathodic catalyst to enhance the oxygen reduction reaction (ORR). Co−Bi@rGO (rGO = reduced graphene oxide) is used as an anode for an EtOH fuel cell due to its low cost and high efficiency. Bi-based solid oxide electrolytes, e.g. sulfonated poly(ether, ketone) (SPEEK) polymer having 7.5 wt.% of bismuth cobalt zinc oxide (BCZO) with a high-power density of 574 mW cm−2 have been reported in this regard. These factors accentuate the relevance of bismuth-based materials for the production of components for fuel cells that have excellent performance. This review examines the published literature on bismuth-based materials and anticipates the synthesis, and role of material in fuel cells. Finally, current challenges and future perspectives present comprehensive guidelines for future research. [ABSTRACT FROM AUTHOR]

The promotion of electric vehicles brings notable environmental and economic advantages. Precisely estimating the state of health (SOH) of lithium-ion batteries is crucial for maintaining their efficiency and safety. This study introduces an SOH estimation approach for lithium-ion batteries that integrates multi-feature analysis with a convolutional neural network and kolmogorov-arnold network (CNN-KAN). Initially, we measure the charging time, current, and temperature during the constant voltage phase. These include charging duration, the integral of current over time, the chi-square value of current, and the integral of temperature over time, which are combined to create a comprehensive multi-feature set. The CNN's robust feature extraction is employed to identify crucial features from raw data, while KAN adeptly models the complex nonlinear interactions between these features and SOH, enabling accurate SOH estimation for lithium batteries. Experiments were carried out at four different charging current rates. The findings indicate that despite significant nonlinear declines in the SOH of lithium batteries, this method consistently provides accurate SOH estimations. The root mean square error (RMSE) is below 1%, with an average coefficient of determination (R 2 ) exceeding 98%. Compared to traditional methods, the proposed method demonstrates significant advantages in handling the nonlinear degradation trends in battery life prediction, enhancing the model's generalization ability as well as its reliability in practical applications. It holds significant promise for future research in SOH estimation of lithium batteries. [ABSTRACT FROM AUTHOR]

Electrolytes with fluorinated solvents have been regarded as a promising strategy to stabilize high‐voltage cathodes and the interphase of lithium anode in lithium metal batteries (LMBs). However, the rigorous synthesis approach and high cost have led to a demand for developing cost‐effective solvents with suitable properties for LMBs. Herein, we explored the possibility of using chlorinate solvents as electrolytes using density functional theory (DFT) and classical molecular dynamics (MD) simulation. Taking ether (1,2‐dimethoxyethane [DME], 1,3‐dioxolane [DOL]), carbonate (dimethyl carbonate [DMC], and ethylene carbonate [EC]) as examples, we first compared the energy variation of the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) upon Cl and F substitution. In particular, we found that 1,2‐bis(chloromethoxy)ethane (DME‐2Cl‐2) has the lowest HOMO and the highest LUMO level among the chlorinated DME after coordinating with Li+, enabling a potentially wide voltage stability. Further MD simulation reveals that lithium ions in DME‐2Cl‐2 has a weaker solvation coordination with solvents but stronger interaction with anions than DME and 1,2‐bis(Fluoromethoxy)ethane (DME‐2F‐2), which is more beneficial for forming stable anion‐derived solid electrolyte interphase (SEI). Our findings suggest that chlorinated solvents can be used as promising electrolytes for LMBs. [ABSTRACT FROM AUTHOR]

The solid‐state batteries (SSBs) with Li anode present one of the most promising energy storage systems due to their enhanced energy density and safety. However, interfacial problems between Li anode and solid‐state electrolyte hinder the advancement of SSBs. Among them, insufficient solid‐solid interfacial contact is the main issue, which causes large resistance and hinders Li+ diffusion, leading to current distribution unevenness and lithium dendrites growth. To meet these challenges, a silver/carbon interlayer composed of ultrafine Ag nanoparticles (≈5 nm) grown on COOH‐CNTs (nano‐Ag@COOH‐CNTs) is constructed. In which, nano‐Ag is designed to guide homogeneous Li deposition, while CNTs substrate bonds with Li6.5La3Zr1.5Ta0.5O12 (LLZTO) electrolyte by reactions between ─COOH groups and LLZTO alkaline surface, thus transforming loose physical solid‐solid contact to chemical bonding contact. In addition, nano‐Ag is immobilized by CNTs, avoiding the migration of Li+ implanted nano‐Ag during cycling. Therefore, nano‐Ag@COOH‐CNTs interlayer can boost Li+ transport at LLZTO/Li interface and inhibit Li dendrites, achieving an ultra‐low interfacial resistance of 0.25 Ω cm2, a high critical current density of 1.7 mA cm−2 and a long cycling over 2155 h at 0.5 mA cm−2. The modified SSBs with LiNi0.83Co0.12Mn0.05O2 cathode cycles stably over 500 cycles. Moreover, high‐loading SSBs operate stably for 85 cycles. [ABSTRACT FROM AUTHOR]

Lithium sulfide (Li2S) is a promising electrode material with high specific capacity and can be paired with commercial anode materials such as graphite. However, bulk Li2S requires a high activation energy during the initial charge due to its inert electrochemical activity, resulting in high charge overpotential. Here, lithium phenyl selenide (PhSeLi) is proposed as a mediator that can effectively activate Li2S by altering the oxidation pathway in the initial charge process. It enables Li2S to release normal capacity over the general voltage range (1.5–3 V). The composite cathode with the Li2S:PhSeLi molar ratio of 4:1 exhibits a high reversible capacity of 615.9 mAh g−1 at 0.2 A g−1 after 400 cycles in all‐solid‐state batteries with Li7P3S11 sulfide electrolyte and In–Li anode (the corresponding capacity based on Li2S is 1016.6 mAh g−1). In a full cell with a partially pre‐lithiated silicon anode, it can still provide an average discharge capacity of 524 mAh g−1 at 0.1 A g−1 (the capacity based on Li2S is 844.2 mAh g−1). This work will contribute to the further development of Li2S‐based all‐solid‐state Li–S batteries. [ABSTRACT FROM AUTHOR]

Lithium‐ion cells encompassing LiPF6 as the lithium salt and high‐voltage (LiNi0.5Mn1.5O4, LNMO) or high‐capacity (LiNi0.8Mn0.1Co0.1O2, NMC811) cathode materials are prone to transition metal (TM) dissolution caused by HF, whose formation is catalyzed by H2O traces. TM ions can shuttle to the anodic compartment, increasing the cell degradation rate. Accordingly, specific self‐healing strategies are helpful to develop scavengers able to eliminate HF and absorb TM ions so avoiding their shuttling. In this work, the fabrication and test of a bi‐functional, autonomous scavenging agent made of Al2O3 particles decorated is reported with chitosan. The nanometric Al2O3 core is a trap for HF by chemical bonding. The chitosan coating is acid‐sensitive, and the opening of such a capping layer is triggered in the presence of even small amounts of HF, leading to an efficient TM ion‐trapping. In addition, chitosan is biocompatible, biodegradable, and abundant, which is relevant for design‐for‐recycling scopes. With ≈200 ppm of water in the electrolyte, 12 wt% of scavenger causes, after 200 cycles at 1C, an increase of capacity retention from 73% to 88% for LNMO, and, impressively, from 46% to 84% for NMC811. This autonomous self‐healing mechanism is promising for application in next‐generation smart cells without requiring any external sensing. [ABSTRACT FROM AUTHOR]

Increasing the upper cut‐off voltage of the LiNixCoyMn1‐x‐yO2 (NCM)‐based lithium‐metal batteries (LMBs) is highly pursued for achieving high battery energy density. However, the cycling stability of high‐voltage LMBs, which is associated with ethylene carbonate electrolytes, remains greatly challenging. Herein, an interphase‐designable additive‐enabled ethylene carbonate‐free electrolyte strategy is proposed for achieving 4.6 V Li||NCM811 battery with long cycling life from 55 to −30 °C. The solvent characteristics of ethyl methyl carbonate endow LMBs with potential merits in high voltage, wide temperature, and cycling stability, which are further strengthened by the additive, 1,5‐difluoro‐2,4‐dinitrobenzene (FNB), for optimizing electrode electrolyte interphases. The sturdy LiF‐rich and LiNxOy‐contained electrode/electrolyte interphase on cathode/anode surfaces can protect two electrodes well from electrolyte corrosion and also reduce excessive electrolyte decomposition. As expected, the Li||NCM811 batteries can maintain 70% capacity retention after 500 cycles with superior high‐temperature and low‐temperature performance (from 55 to −30 °C). The 6.8Ah pouch cells with this electrolyte can achieve a high energy density of up to 505 Wh kg−1. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries are widely recognized as promising alternatives to lithium batteries due to their excellent safety, environmental compatibility, and cost‐effectiveness. Nonetheless, the formation of dendrites, corrosion, and undesirable side reactions on the zinc surface pose significant challenges to the cycling stability of zinc‐ion batteries. In this study, polar propylene carbonate (PC) is paired with tetrafluoroborate anions to establish a strong ion‐dipole interaction. Strong ion‐dipole interaction can not only alter the solvation structure of zinc ions but also facilitate the formation of a dynamic double electric layer on the surface of the zinc electrode, suppressing the formation of ZnF2 interface and carbonate, thereby facilitating uniform zinc ion deposition, and consequently improving battery cycling stability over a broad temperature range. Concretely, the formulated electrolyte enhances the cycling stability of the battery over a wide temperature range of −30 to 40 °C, accompanied by a capacity retention of ≈100% even after 10 000 cycles at −30 °C. The symmetrical battery utilizing this electrolyte exhibits stable cycling performance for over 1200 h at 25 °C and 1900 h at −30 °C, respectively. The findings provide a promising direction for the development of long‐cycle batteries capable of operating over a wide temperature range. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes (SPEs) offer inherent advantages for battery applications, such as high safety and excellent processability, but their practical use is limited by challenges like low ionic conductivity, subpar mechanical properties, and instability of the electrode/electrolyte interface. Here, novel SPEs are developed by embedding 2D MXenes decorated at the surface with methoxypolyethylene glycol chains into poly(vinylidene fluoride)‐hexafluoropropylene matrices, enhanced with succinonitrile as a plasticizer. This innovative design improves the compatibility of the modified MXene in poly(vinylidene fluoride)‐hexafluoropropylene and, together with the synergistic effects of succinonitrile, promotes the dissociation of lithium salt. The SPE achieves ionic conductivity of 1.49 × 10−4 S cm−1 at 30 °C, and a Li‐ion transference number of 0.59. These results are supported by comprehensive experimental characterization, COMSOL simulations, and DFT calculations. This SPE enables stable and reversible Li plating/stripping for over 2100 h in Li/Li symmetric cells, while fabricated Li/LiFePO4 full cells deliver a notable capacity of 135.4 mAh g−1 with an average Coulombic efficiency of 98.9% after 100 cycles at 0.2 C. Furthermore, the Li/LiNi0.6Co0.2Mn0.2O2 full cells also demonstrate a capacity of 140.5 mAh g−1 after over 200 cycles at 0.5 C, showcasing an impressive capacity retention rate of 99.6%. [ABSTRACT FROM AUTHOR]

Elevating the charging cut‐off voltage is an effective strategy to increase the energy density of LiCoO2. However, unstable interfacial structures and unfavorable phase transitions in bulk are inevitably triggered during deep de‐lithiation at high voltage. Herein, an integrated surface‐to‐bulk Ti‐modification strategy is applied to LiCoO2, enabling uniform Li2TiO3 coating on the surface and gradient Ti‐doping toward the structural bulk. The resultant Ti‐modified LiCoO2 (T‐LCO) electrode can be stably cycled up to 4.6 V, providing a high‐rate capability of 137 mAh g−1 at 5C and a long‐life stability with 80.5% capacity retention after 400 cycles at 1C, far outperforming the unmodified LiCoO2 electrode with only 50.7% capacity retention. In situ X‐ray diffraction characterization and density functional theory calculation reveal that the synergistic modification of T‐LCO enhances Li+ diffusion, facilitates the construction of high‐quality cathode/electrolyte interphase, reduces the phase transition from O3 to H1‐3 and Co3d/O2p band overlap, and restrains layer‐to‐spinel phase distortion, thus improving structural stability at 4.6 V. This work presents a “two birds one step” strategy to enhance the cycling stability and achievable capacity of high‐voltage LiCoO2 for developing high energy density lithium‐ion batteries. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes (SPEs) have been treated as a viable solution to build high‐performance solid‐state lithium metal batteries (SSLMBs) at the industrial level, bypassing the safety and energy density dilemmas experienced by today's lithium‐ion battery technology. To promote a wider application of SPEs‐based SSLMBs, the chemical and electrochemical characteristics of lithium metal (Li°) electrode in SPEs have to be clearly elucidated. In this work, the morphological evolution of Li° electrode in the SPEs‐based SSLMBs is comprehensively investigated, via a customized electrochemical cell allowing optical microscopic analyses. The results demonstrate that differing from inorganic solid electrolytes, the elastic feature of SPEs eliminates the “memory effect” of the dendrite formation, in which the previously formed dendrites can be dissolved and the resulting space can be simultaneously occupied by electrolyte components, instead of leaving for a second‐round growth of Li° dendrites. Furthermore, the largely increased electronic conductivities of the as‐formed interphases between Li° electrode and SPEs are found to be responsible for the notoriously soft short‐circuit behavior observed during cycling. These findings bring a fresh understanding of the formation and evolution of lithium dendrites in SPE‐based cells, which are vital for improving the long‐term stability of SSLMBs and other related high‐energy battery systems. [ABSTRACT FROM AUTHOR]

This review introduces solid electrolytes based on sulfide/polymer composites which are used in all‐solid‐state lithium batteries, describing the use of polymers as plasticizer, the lithium‐ion conductive channel, the preparation methods of solid‐state electrolytes (SSEs), including dry methods and wet methods with their advantages and disadvantages. In addition, the physicochemical stability of sulfide/polymer composite based solid‐state electrolytes is analyzed. The sulfide/polymer composite based solid‐state electrolyte can be utilized in lithium metal or lithium sulfur batteries. However, there are still many problems left to be solved in practical applications of these solid‐state electrolytes. In this review, several solutions are explored. Firstly, the ultra‐long life cycle of batteries can be achieved by thinning the composite electrolyte. Secondly, when sulfur is applied as the positive electrode, the thinning electrolyte can reduce polarization and other problems. Finally, an integrated battery is employed to reduce the interface impedance. By addressing these aspects, the review aims to provide valuable insights into the future development of high‐performance solid‐state electrolytes in lithium battery technology. [ABSTRACT FROM AUTHOR]

Coulombic efficiency of over 99 % is rarely achieved for Li metal anode below −40 °C, hindering the practical application of high‐energy‐density Li metal batteries under extreme conditions. Herein, limiting factors for Li metal reversibility are investigated utilizing ether‐based localized high‐concentration electrolytes of different solvent‐diluent combinations. We find that along with the desolvation barrier, bulk ion transport properties including ionic conductivity, transference number, and diffusivity are also crucial factors for low‐temperature Li deposition behavior. Superior Li metal reversibility was observed within the combination of the solvent with moderately weak solvating power and the diluent with minimal viscosity, highlighting the role of ion transport and the necessity for a trade‐off with desolvation. The optimized electrolyte composed of lithium bis(fluorosulfonyl)imide, methyl n‐propyl ether, and 1,1,2,2‐tetrafluoroethyl methyl ether delivers exceptional Coulombic efficiency of 99.34 % at −40 °C and 98.96 % at −60 °C under a current density of 0.5 mA cm−2. Furthermore, Li||LiCoO2 (2.7 mAh cm−2) cells demonstrate impressive reversible capacity and cycling stability at these temperatures. This work sheds light on the less‐recognized relevance of bulk ion transport to low‐temperature performance and provides guidelines for the electrolyte design of Li metal batteries operating in cold environments. [ABSTRACT FROM AUTHOR]

Lithium‐metal solid‐state batteries are attractive as next generation of Li‐ion batteries due to higher safety and potentially higher energy density. To improve processability, solid‐composite separators combine advantages of inorganic and polymer separators in hybrid structure. We report a systematic approach to fabricate composite separators with high content (90–95 wt %) of ceramic Li‐ion conducting Li6.45Al0.05La3Zr1.6Ta0.4O12 (LLZO) powder embedded in a polyethylene oxide (PEO)‐LiTFSI (20 : 1) matrix and understand factors affecting their properties and performance. Separators with good mechanical flexibility and excellent thermal stability were obtained, by optimizing materials and processing parameters. It was found that PEO molecular weight strongly influences the microstructure and electrochemical properties of the separators. In optimized separator with 90 wt % of LLZO and PEO with Mw 300,000 g/mol, a total ionic conductivity of 1.4×10−5 S/cm at 60 °C was achieved. The ceramic‐rich separator showed excellent long‐term cycling stability for more than 460 cycles (1000 h) at 0.1 mA/cm2 in Li/Li symmetrical cells and achieved a critical current density of 0.25 mA/cm2. The separators also enabled initial discharge capacities of more than 160 mAh/g in full cells with Li metal anode and composite solid‐state LiNi0.6Co0.2Mn0.2O2 cathode, although rapid capacity fade was observed after 10 cycles in fully solid‐state configuration. [ABSTRACT FROM AUTHOR]

The solid‐state batteries (SSBs) with Li anode present one of the most promising energy storage systems due to their enhanced energy density and safety. However, interfacial problems between Li anode and solid‐state electrolyte hinder the advancement of SSBs. Among them, insufficient solid‐solid interfacial contact is the main issue, which causes large resistance and hinders Li+ diffusion, leading to current distribution unevenness and lithium dendrites growth. To meet these challenges, a silver/carbon interlayer composed of ultrafine Ag nanoparticles (≈5 nm) grown on COOH‐CNTs (nano‐Ag@COOH‐CNTs) is constructed. In which, nano‐Ag is designed to guide homogeneous Li deposition, while CNTs substrate bonds with Li6.5La3Zr1.5Ta0.5O12 (LLZTO) electrolyte by reactions between ─COOH groups and LLZTO alkaline surface, thus transforming loose physical solid‐solid contact to chemical bonding contact. In addition, nano‐Ag is immobilized by CNTs, avoiding the migration of Li+ implanted nano‐Ag during cycling. Therefore, nano‐Ag@COOH‐CNTs interlayer can boost Li+ transport at LLZTO/Li interface and inhibit Li dendrites, achieving an ultra‐low interfacial resistance of 0.25 Ω cm2, a high critical current density of 1.7 mA cm−2 and a long cycling over 2155 h at 0.5 mA cm−2. The modified SSBs with LiNi0.83Co0.12Mn0.05O2 cathode cycles stably over 500 cycles. Moreover, high‐loading SSBs operate stably for 85 cycles. [ABSTRACT FROM AUTHOR]

This article presents a novel aging-coupled predictive thermo-electrical dynamic modeling tool tailored for primary lithium manganese dioxide ( L i - M n O 2 ) batteries in active implantable medical devices (AIMDs). The aging mechanisms of rechargeable lithium batteries are well documented using computationally intensive physics-based models, unsuitable for real-time onboard monitoring in AIMDs due to their high demands. There is a critical need for efficient, less demanding modeling tools for accurate battery health monitoring and end-of-life prediction as well as battery safety assessment in these devices. The presented model in this article simulates the battery terminal voltage, remaining capacity, temperature, and aging during active discharge, making it suitable for real-time health monitoring and end-of-life prediction. We incorporate a first-order dynamic for internal resistance growth, influenced by time, temperature, discharge depth, and load current. By adopting Arrhenius-type kinetics and polynomial relationships, this model effectively simulates the combined impact of these variables on battery aging under diverse operational conditions. The simulation handles both the continuous micro-ampere-level demands necessary for device housekeeping and periodic high-rate pulses needed for therapeutic functions, at a constant ambient temperature of 37 °C, mimicking human body conditions. Our findings reveal a gradual, nonlinear increase in internal resistance as the battery ages, rising by an order of magnitude over a period of 5 years. Sensitivity analysis shows that as the battery ages and load current increases, the terminal voltage becomes increasingly sensitive to internal resistance. Specifically, at defibrillation events, the ∂ V ∂ R trajectory dramatically increases from 10 − 12 to 10 − 8 , indicating a fourth-order-of-magnitude enhancement in sensitivity. A model verification against experimental data shows an R2 value of 0.9506, indicating a high level of accuracy in predicting the L i - M n O 2 cell terminal voltage. This modeling tool offers a comprehensive framework for effectively monitoring and optimizing battery life in AIMDs, therefore enhancing patient safety. [ABSTRACT FROM AUTHOR]

Li–S batteries are promising large-scale energy storage systems but currently suffer from performance issues; a major reason is the dissolution of polysulfides in electrolytes. To this end, we report a high-energy-density Lithium–Sulfur (Li–S) battery that combines a catholyte and a sulfur-free carbon nanofiber (CNF) cathode. The cathode was synthesized by carbonizing binder-free polyacrylonitrile (PAN) nanofibers, affording a high surface area. In the catholyte, added polysulfides acted as both conductive Li salts and active materials. Investigating the electrochemical performance of this concept in both Swagelok- and pouch-type cells afforded energy densities exceeding 3 mAh cm−2 at a discharge rate of 0.1 C. This combination could also be utilized in high-capacity pouch cells with capacities of up to 250 mAh g−1. Both cell types exhibited good cycle performance. Adding LiNO3 to the electrolyte suppressed the redox shuttle reactions. Moreover, the cathode being binder-free increased the energy density and simplified cathode fabrication. Characterizing the cathode before and after cycling revealed that deposition was reversible, and that cell reactions at least partially formed sulfur as the end product, resulting in high sulfur amounts in the cell. We expect our concept to greatly aid in the development of practically applicable Li–S cells. [ABSTRACT FROM AUTHOR]

Lithium‐metal anodes (LMAs) are the ultimate choice for realizing high‐energy‐density batteries; however, its use is hindered by problematic Li growth in the form of dendrites. To alleviate dendritic Li growth, the preparation of LMAs with a lithiophilic current collector (CC) is effective; however, applying a lithiophilic CC to LMAs is still challenging due to the manufacturing complexity involved in the separate lithiophilic treatment and lithiation processes. Herein, a facile one‐pot LMA fabrication method by utilizing thiourea (TU) as a precursor is proposed. A lithiophilic Cu2S layer is formed on Cu foam (CF) by the in situ electrochemical oxidation of TU (CuxSCF), and the lithiation of CC is performed via subsequent Li electrodeposition (Li@CuxSCF). The Cu2S on CuxSCF can lead to uniform Li deposition by providing lithiophilic sites, and it is converted to form ionic‐conductive Li2S‐rich solid electrolyte interphase layer. Resultantly, CuxSCF significantly enhances the cycling performance of LMAs compared to CF. Specifically, a LiFePO4/Li@CuxSCF full‐cell lithium‐metal battery (LMB) with a low n/p ratio (1.6) exhibits capacity retention of 95.6% at 0.5 C (220 cycles) and can maintain 85.0% of initial capacity (425 cycles, n/p = 4) at 2.0 C. LMBs with LiNi0.6Co0.2Mn0.2 and LiNi0.8Co0.1Mn0.1 also exhibit improved electrochemical performance. [ABSTRACT FROM AUTHOR]

The high energy density advantage of lithium (Li) metal batteries (LMBs) makes them increasingly desirable; however, problems such as strong reactivity and dendrite growth of Li metal anode limit their practical uses. In this work, a novel Li‐containing glycerol (LiGL) or lithicone protection layer on a 50 μm thick Li metal anode is employed for improving the performance of LMBs. This LiGL layer was accurately deposited via a molecular layer deposition (MLD) process at 150 °C, using lithium tert‐butoxide and glycerol as precursors. The as‐formed LiGL coating layer is highly tunable in its thickness by simply adjusting MLD cycles and shows a good stability and outstanding ionic transport properties. The LiGL layer is found to effectively mitigate side reactions and enhance cycling stability in both symmetric cells and full cells. Specifically, the LMBs with LiGL@Li anode of 400 MLD cycles and LiNi0.6Mn0.2Co0.2O2 cathode enable a capacity retention of ≈87%, much higher than ≈35% of the cells with bare Li after 200 cycles at a charge/discharge current density of 2.1 mA cm−2. This work paves a feasible way for practical LMBs with improved capacity and stability through applying an innovative protection layer on Li metal anodes. [ABSTRACT FROM AUTHOR]

In current researches on belief rule base (BRB), input parameters are tended to be expressed in the form of quantitative values through expert knowledge combined with optimization methods. A singular quantitative value fails to capture the statistical properties, leading to irrational outcomes. Therefore, an attempt on attribute weights is made in this paper, and a new model with probability distribution attribute weights (pdw) called BRB-pdw is proposed. The combination of two attributes is in detail discussed, where attribute weights are described as random variables with specific probability distribution. To characterize the output of probability distribution attribute weight, a new concept of expectation of activation weight is proposed. In addition, the BRB-pdw is extended to multiple attributes to demonstrate its universality. Furthermore, fundamental properties and characteristics of the BRB-pdw are further validated by rigorous mathematical derivation. Finally, practicability of the BRB-pdw is validated with NASA lithium battery open dataset, and experiments show that the BRB-pdw model is more robust while maintaining precision. [ABSTRACT FROM AUTHOR]

The introduction of Zn improves the wettability and surface lithiophilicity of Cu foam toward Li metal, and a sublevel scaffold of Li x Zn alloy is constructed in the pores of Cu foam, regulating uniform Li deposition in the modified 3D skeleton. [Display omitted] Lithium (Li) metal anode (LMA) is one of the most promising anodes for high energy density batteries. However, its practical application is impeded by notorious dendrite growth and huge volume expansion. Although the three-dimensional (3D) host can enhance the cycling stability of LMA, further improvements are still necessary to address the key factors limiting Li plating/stripping behavior. Herein, porous copper (Cu) foam (CF) is thermally infiltrated with molten Li-rich Li-zinc (Li-Zn) binary alloy (CFLZ) with variable Li/Zn atomic ratio. In this process, the LiZn intermetallic compound phase self-assembles into a network of mixed electron/ion conductors that are distributed within the metallic Li phase matrix and this network acts as a sublevel skeleton architecture in the pores of CF, providing a more efficient and structured framework for the material. The as-prepared CFLZ composite anodes are systematically investigated to emphasize the roles of the tunable lithiophilicity and hierarchical structure of the frameworks. Meanwhile, a thin layer of Cu-Zn alloy with strong lithiophilicity covers the CF scaffold itself. The CFLZ with high Zn content facilitates uniform Li nucleation and deposition, thereby effectively suppressing Li dendrite growth and volume fluctuation. Consequently, the hierarchical and lithiophilic framework shows low Li nucleation overpotential and highly stable Coulombic efficiency (CE) for 200 cycles in conventional carbonate based electrolyte. The full cell coupled with LiFePO 4 (LFP) cathode demonstrates high cycle stability and rate performance. This work provides valuable insights into the design of advanced dendrite-free 3D LMA toward practical application. [ABSTRACT FROM AUTHOR]

[Display omitted] • N doped carbon coating CoP hollow nanofibers was successfully fabricated. • Multifunctional materials N/C@CoP-HNFs are used for PIBs and Li-S batteries. • N/C@CoP-HNFs with unique structures show good performance in PIBs and Li-S batteries. • Phase variations of electrodes at different states are studied. • DFT are used to understand electrochemical properties at the atomic level. Herein, a composite of N -doped carbon coated phosphating cobalt hollow nanofibers (N/C@CoP-HNFs) was synthesized by electrospinning, phosphating, and carbon coating processes. When employed as multifunctional electrode materials for potassium-ion batteries (PIBs) and lithium-sulfur (Li-S) batteries, the N/C@CoP-HNFs demonstrated notable electrochemical properties. Specifically, it delivered an initial specific capacity of 420.4 mA h g−1 at a current density of 100 mA g−1, with a sustained capacity of 190.8 mA h g−1 after 200 cycles in PIBs, and a specific capacity of 1448 mA h g−1 at a current density of 0.5C in Li-S batteries, which is considered relatively high for these types of battery technology. This good performance may due to the combination of the carbon nitrogen layer and cobalt phosphide bilayer hollow tube structure, which is conducive to telescoping the diffusion length of ions and electrons and buffer volume variation, and effectively inhibits the shuttle effect. Density functional theory (DFT) calculations were also used to explore the energy storage mechanism of the material. The possible adsorption sites and corresponding adsorption energy of K+ were analyzed, and the advantages of the material were explored by calculating the diffusion barrier and state density. The theoretical simulations further validated the strong adsorption capability of CoP for polysulfides. This work is expected to provide new ideas for new energy storage materials. [ABSTRACT FROM AUTHOR]

Three-dimensional (3D) host materials for lithium metal anodes (LMAs) have gained attention because they can mitigate volume expansion and local current density through their large surface area and suppress the dendritic growth of lithium. Recent research on 3D host materials has focused on conductive materials; however, the benefits of 3D host materials cannot be fully utilized because lithium deposition begins at the top of the structure. Herein, we fabricate SiO2-TiO2 composite microspheres with bimodal pore structures (bi-SiTiO) by simple spray pyrolysis. These microspheres effectively store lithium within the structure from the bottom of the electrode while preventing lithium dendrite formation. Focused ion beam-scanning transmission electron microscopy (FIB-STEM) analysis reveals that the lithiophilic properties of composite microspheres enhanced their effectiveness in storing lithium, with small pores acting as "lithium-ion sieves" for a uniform lithium-ion flux and large pores that provide sufficient volume for lithium deposition. The bi-SiTiO composite microspheres exhibit a high Coulombic efficiency of 98.5% over 200 cycles at 2.0 mA·cm−2 when operated in a lithium half-cell. With a high lithium loading of 5.0 mAh·cm−2, the symmetrical cell of the bi-SiTiO electrode sustains more than 900 h. A full cell coupled with an LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode also exhibits enhanced electrochemical properties in terms of cycling stability and rate capability. [ABSTRACT FROM AUTHOR]

Solid-state polymer electrolytes (SPEs) are candidate schemes for meeting the safety and energy density needs of advanced lithium-based battery because of their improved mechanical and electrochemical stability compared to traditional liquid electrolytes. However, low ionic conductivity and side reactions occurring in traditional high-voltage lithium metal batteries (LMBs) hinder their practical applications. Here, amino-modified metal-organic frameworks (UiO-66-NH2) with abundant defects as multifunctional fillers in the polyurethane based SPEs achieve the collaborative promotion of the mechanical strength and room temperature ionic conductivity. The surface modified amino groups serve as anchoring points for oxygen atoms of polymer chains, forming a firmly hydrogen-bond interface with polycarbonate-based polyurethane frameworks. The rich interfaces between UiO-66-NH2 and polymers dramatically decrease the crystallization of polymer chains and reduce ion transport impedance, which markedly boosted the ionic conductivity to 2.1 × 10−4 S·cm−1 with a high Li+ transference numbers of 0.71. As a result, LiFePO4∣SPEs∣Li cells exhibit prominent cyclability for 700 cycles under 0.5 C with 96.5% capacity retention. The LiNi0.6Co0.2Mn0.2O2 (NCM622)∣SPEs∣Li cells deliver excellent long-term lifespan for 260 cycles with a high capacity retention of 91.9% and high average Coulombic efficiency (98.5%) under ambient conditions. This simple and effective hybrid SPE design strategy sheds a milestone significance light for high-voltage Li-metal batteries. [ABSTRACT FROM AUTHOR]

Accurately estimating the State of Health (SOH) of batteries is of great significance for the stable operation and safety of lithium batteries. This article proposes a method based on the combination of Capacity Incremental Curve Analysis (ICA) and Whale Optimization Algorithm-Radial Basis Function (WOA-RBF) neural network algorithm to address the issues of low accuracy and slow convergence speed in estimating State of Health of batteries. Firstly, preprocess the battery data to obtain the real battery SOH curve and Capacity-Voltage (Q-V) curve, convert the Q-V curve into an IC curve and denoise it, analyze the parameters in the IC curve that may serve as health features; Then, extract the constant current charging time of the battery and the horizontal and vertical coordinates of the two IC peaks as health features, and perform correlation analysis using Pearson correlation coefficient method; Finally, the WOA-RBF algorithm was used to estimate the battery SOH, and the training results of LSTM, RBF, and PSO-RBF algorithms were compared. The conclusion was drawn that the WOA-RBF algorithm has high accuracy, fast convergence speed, and the best linearity in estimating SOH. The absolute error of its SOH estimation can be controlled within 1%, and the relative error can be controlled within 2%. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc-metal batteries, considered as the possible post-lithium-ion battery technology for large-scale energy storage, face severe challenges such as dendrite growth and hydrogen evolution side reaction (HER) on Zn negative electrode. Herein, a three-dimensional Cu-In alloy interface is developed through a facile potential co-replacement route to realize uniform Zn nucleation and HER anticatalytic effect simultaneously. Both theoretical calculations and experimental results demonstrate that this bifunctional Cu-In alloy interface inherits the merits of low Zn-nucleation overpotential and high HER overpotential from individual copper and indium constituents, respectively. Moreover, the dynamical self-reconstruction during cycling leads to an HER-anticatalytic and zincophilic gradient hierarchical structure, enabling highly reversible Zn chemistry with dendrite-free Zn (002) deposition and inhibited HER. Moreover, the improved interface stability featured by negligible pH fluctuations in the diffusion layer and suppressed by-product formation is evidenced by in-situ scanning probe technology, Raman spectroscopy, and electrochemical gas chromatography. Consequently, the lifespan of the CuIn@Zn symmetric cell is extended to more than one year with a voltage hysteresis of 6 mV. Importantly, the CuIn@Zn negative electrode is also successfully coupled with high-loading iodine positive electrode to fabricate Ah-level (1.1 Ah) laminated pouch cell, which exhibits a capacity retention of 67.9% after 1700 cycles. Rechargeable aqueous Zn metal batteries are impeded by dendrite growth and the hydrogen evolution side reaction. Here, authors develop a bifunctional Cu-In alloy interface to realize uniform Zn nucleation and prevent hydrogen evolution, enabling operation of Ah-level Zn metal pouch cells. [ABSTRACT FROM AUTHOR]

Titanium niobium oxide (TiNbxO2 + 2.5x) is emerging as a promising electrode material for rechargeable lithium‐ion batteries (LIBs) due to its exceptional safety characteristics, high electrochemical properties (e.g., cycling stability and rate performance), and eco‐friendliness. However, several intrinsic critical drawbacks, such as relatively low electrical conductivity, significantly hinder its practical applications. Developing reliable strategies is crucial to accelerating the practical use of TiNbxO2 + 2.5x‐based materials in LIBs, especially high‐power LIBs. Here, we provide a chronicle review of the research progress on TiNbxO2 + 2.5x‐based anodes from the early 1950s to the present, which is classified into early stage (before 2008), emerging stage (2008–2012), explosive stage (2013–2017), commercialization (2018), steady development (2018–2022), and new breakthrough stage (since 2022). In each stage, the advancements in the fundamental science and application of the TiNbxO2 + 2.5x‐based anodes are reviewed, and the corresponding developing trends of TiNbxO2 + 2.5x‐based anodes are summarized. Moreover, several future research directions to propel the practical use of TiNbxO2 + 2.5x anodes are suggested based on reviewing the history. This review is expected to pave the way for developing the fabrication and application of high‐performance TiNbxO2 + 2.5x‐based anodes for LIBs. [ABSTRACT FROM AUTHOR]

High‐capacity nickel‐rich layered oxides are promising cathode materials for high‐energy‐density lithium batteries. However, the poor structural stability and severe side reactions at the electrode/electrolyte interface result in unsatisfactory cycle performance. Herein, the thin layer of two‐dimensional (2D) graphitic carbon‐nitride (g‐C3N4) is uniformly coated on the LiNi0.8Co0.1Mn0.1O2 (denoted as NCM811@CN) using a facile chemical vaporization‐assisted synthesis method. As an ideal protective layer, the g‐C3N4 layer effectively avoids direct contact between the NCM811 cathode and the electrolyte, preventing harmful side reactions and inhibiting secondary crystal cracking. Moreover, the unique nanopore structure and abundant nitrogen vacancy edges in g‐C3N4 facilitate the adsorption and diffusion of lithium ions, which enhances the lithium deintercalation/intercalation kinetics of the NCM811 cathode. As a result, the NCM811@CN‐3wt% cathode exhibits 161.3 mAh g−1 and capacity retention of 84.6% at 0.5 C and 55 °C after 400 cycles and 95.7 mAh g−1 at 10 C, which is greatly superior to the uncoated NCM811 (i.e. 129.3 mAh g−1 and capacity retention of 67.4% at 0.5 C and 55 °C after 220 cycles and 28.8 mAh g−1 at 10 C). The improved cycle performance of the NCM811@CN‐3wt% cathode is also applicable to solid–liquid‐hybrid cells composed of PVDF:LLZTO electrolyte membranes, which show 163.8 mAh g−1 and the capacity retention of 88.1% at 0.1 C and 30 °C after 200 cycles and 95.3 mAh g−1 at 1 C. [ABSTRACT FROM AUTHOR]

The current global warming, coupled with the growing demand for energy in our daily lives, necessitates the development of more efficient and reliable energy storage devices. Lithium batteries (LBs) are at the forefront of emerging power sources addressing these challenges. Recent studies have shown that integrating hexagonal boron nitride (h‐BN) nanomaterials into LBs enhances the safety, longevity, and electrochemical performance of all LB components, including electrodes, electrolytes, and separators, thereby suggesting their potential value in advancing eco‐friendly energy solutions. This review provides an overview of the most recent applications of h‐BN nanomaterials in LBs. It begins with an informative introduction to h‐BN nanomaterials and their relevant properties in the context of LB applications. Subsequently, it addresses the challenges posed by h‐BN and discusses existing strategies to overcome these limitations, offering valuable insights into the potential of BN nanomaterials. The review then proceeds to outline the functions of h‐BN in LB components, emphasizing the molecular‐level mechanisms responsible for performance improvements. Finally, the review concludes by presenting the current challenges and prospects of integrating h‐BN nanomaterials into battery research. [ABSTRACT FROM AUTHOR]

The practical application of lithium (Li) metal anodes in high‐capacity batteries is impeded by the formation of hazardous Li dendrites. To address this challenge, this research presents a novel methodology that combines laser ablation and heat treatment to precisely induce controlled grain growth within laser‐structured grooves on copper (Cu) current collectors. Specifically, this approach enhances the prevalence of Cu (100) facets within the grooves, effectively lowering the overpotential for Li nucleation and promoting preferential Li deposition. Unlike approaches that modify the entire surface of collectors, our work focuses on selectively enhancing lithiophilicity within the grooves to mitigate the formation of Li dendrites and exhibit exceptional performance metrics. The half‐cell with these collectors maintains a remarkable Coulombic efficiency of 97.42% over 350 cycles at 1 mA cm−2. The symmetric cell can cycle stably for 1600 h at 0.5 mA cm−2. Furthermore, when integrated with LiFePO4 cathodes, the full‐cell configuration demonstrates outstanding capacity retention of 92.39% after 400 cycles at a 1C discharge rate. This study introduces a novel technique for fabricating selective lithiophilic three‐dimensional (3D) Cu current collectors, thereby enhancing the performance of Li metal batteries. The insights gained from this approach hold promise for enhancing the performance of all laser‐processed 3D Cu current collectors by enabling precise lithiophilic modifications within complex structures. [ABSTRACT FROM AUTHOR]

All‐solid‐state lithium metal batteries (ASSLMBs) featuring sulfide solid electrolytes (SEs) are recognized as the most promising next‐generation energy storage technology because of their exceptional safety and much‐improved energy density. However, lithium dendrite growth in sulfide SEs and their poor air stability have posed significant obstacles to the advancement of sulfide‐based ASSLMBs. Here, a thin layer (approximately 5 nm) of g‐C3N4 is coated on the surface of a sulfide SE (Li6PS5Cl), which not only lowers the electronic conductivity of Li6PS5Cl but also achieves remarkable interface stability by facilitating the in situ formation of ion‐conductive Li3N at the Li/Li6PS5Cl interface. Additionally, the g‐C3N4 coating on the surface can substantially reduce the formation of H2S when Li6PS5Cl is exposed to humid air. As a result, Li–Li symmetrical cells using g‐C3N4‐coated Li6PS5Cl stably cycle for 1000 h with a current density of 0.2 mA cm−2. ASSLMBs paired with LiNbO3‐coated LiNi0.6Mn0.2Co0.2O2 exhibit a capacity of 132.8 mAh g−1 at 0.1 C and a high‐capacity retention of 99.1% after 200 cycles. Furthermore, g‐C3N4‐coated Li6PS5Cl effectively mitigates the self‐discharge behavior observed in ASSLMBs. This surface‐coating approach for sulfide solid electrolytes opens the door to the practical implementation of sulfide‐based ASSLMBs. [ABSTRACT FROM AUTHOR]

This work demonstrates a novel polymerization‐derived polymer electrolyte consisting of methyl methacrylate, lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate. The polymerization of MMA was initiated by the amino compounds following an anionic catalytic mechanism. LiTFSI plays both roles including the initiator and Li ion source in the polymer electrolyte. Normally, lithium bis(trifluoromethanesulfonyl)imide has difficulty in initiating the polymerization reaction of methyl methacrylate monomer, a very high concentration of lithium bis(trifluoromethanesulfonyl)imide is needed for initiating the polymerization. However, the fluoroethylene carbonate additive can work as a supporter to facilitate the degree of dissociation of lithium bis(trifluoromethanesulfonyl)imide and increase its initiator capacity due to the high dielectric constant. The as‐prepared poly‐methyl methacrylate‐based polymer electrolyte has a high ionic conductivity (1.19 × 10−3 S cm−1), a wide electrochemical stability window (5 V vs Li+/Li), and a high Li ion transference number (tLi+) of 0.74 at room temperature (RT). Moreover, this polymerization‐derived polymer electrolyte can effectively work as an artificial protective layer on Li metal anode, which enabled the Li symmetric cell to achieve a long‐term cycling performance at 0.2 mAh cm−2 for 2800 h. The LiFePO4 battery with polymerization‐derived polymer electrolyte‐modified Li metal anode shows a capacity retention of 91.17% after 800 cycles at 0.5 C. This work provides a facile and accessible approach to manufacturing poly‐methyl methacrylate‐based polymerization‐derived polymer electrolyte and shows great potential as an interphase in Li metal batteries. [ABSTRACT FROM AUTHOR]

Lithium metal batteries (LMBs) are considered the ideal choice for high volumetric energy density lithium‐ion batteries, but uncontrolled lithium deposition poses a significant challenge to the stability of such devices. In this paper, we introduce a 2.5 μm‐thick asymmetric and ultrastrong separator, which can induce tissue‐like lithium deposits. The asymmetric separator, denoted by utPE@Cu2O, was prepared by selective synthesis of Cu2O nanoparticles on one of the outer surfaces of a nanofibrous (diameter ~10 nm) ultrastrong ultrahigh molecular weight polyethylene (UHMWPE) membrane. Microscopic analysis shows that the lithium deposits have tissue‐like morphology, resulting in the symmetric lithium cells assembled using utPE@Cu2O with symmetric Cu2O coating exhibiting stable performance for over 2000 h of cycling. This work demonstrates the feasibility of a facile approach ultrathin separators for the deployment of lithium metal batteries, providing a pathway towards enhanced battery performance and safety. [ABSTRACT FROM AUTHOR]

The intense research of lithium‐ion batteries has been motivated by their successful applications in mobile devices and electronic vehicles. The emerging of intelligent control in kinds of devices brings new requirements for battery systems. The high‐energy lithium batteries are expected to respond or react under different environmental conditions. In this work, a tri‐salt composite electrolyte is designed with a temperature switch function for intelligently temperature‐controlled lithium batteries. Specifically, the halide Li3YBr6 together with LiTFSI and LiNO3 works as active fillers in a low‐melting‐point polymer matrix (polyethyleneglycol dimethyl ether (PEGDME) and polyethylene oxide (PEO)), which is further filled into the pre‐lithiated alumina fiber skeleton. Above 60 °C, the composite electrolyte exists in the liquid state and fully contacts with the working electrodes on the liquid–solid interface, effectively minimizing the interfacial resistance and leading to high discharge capacity in the cell. The electrolyte is changed into a solid state below 30 °C so that the ionic conductivity is significantly reduced and the interface resistance is increased dramatically on the solid–solid interface. Therefore, by simply adjusting the temperature, the cell can be turned "ON" or "OFF" intentionally. This novel function of the composite electrolyte has enlightening significance in developing intelligently temperature‐controlled lithium batteries. [ABSTRACT FROM AUTHOR]

Thermal runaway propagation (TRP) in lithium batteries poses significant risks to energy‐storage systems. Therefore, it is necessary to incorporate insulating materials between the batteries to prevent the TRP. However, the incorporation of insulating materials will impact the battery thermal management system (BTMS). In this article, the influence of aerogel insulation on liquid‐cooled BTMS is analyzed employing experiments and simulations. In the experiment results, it is revealed that aerogel reduces heat dissipation from liquid‐cooled battery packs, leading to elevated peak temperatures and steeper temperature gradients. Simulation of battery pack discharge warming based on the 3D model shows that the result matches very well with that in the experiment., indicating a maximum temperature rise from 34.92 to 42.57 °C at 2C when aerogel thickness is increased to 5 mm, alongside a temperature differential expansion from 11.11 to 17.50 °C. Nonetheless, beyond 3 mm thickness, further increases in aerogel thickness cause negligible (<0.1 °C) temperature alterations, defining the saturation thickness of aerogel. Furthermore, maintaining consistent thickness and stacking more aerogel layers do not mitigate its detrimental effects. Interestingly, augmenting the battery's through‐thickness thermal conductivity counteracts the adverse outcomes of aerogel usage. [ABSTRACT FROM AUTHOR]

Due to its exceptionally high theoretical energy density, fluorinated carbon has been recognized as a strong contender for the cathode material in lithium primary batteries particularly valued in aerospace and related industries. However, CF x cathode with high F/C ratio, which enables higher energy density, often suffer from inadequate rate capability and are unable to satisfy escalating demand. Furthermore, their intrinsic low discharge voltage imposes constraints on their applicability. In this study, a novel and high F/C ratio fluorinated carbon nanomaterials (FNC) enriched with semi-ionic C–F bonds is synthesized at a lower fluorination temperature, using aggregated nanocarbon as the precursor. The increased presence semi-ionic C–F bonds of the FNC enhances conductivity, thereby ameliorating ohmic polarization effects during initial discharge. In addition, the spherical shape and aggregated configuration of FNC facilitate the diffusion of Li+ to abundant active sites through continuous paths. Consequently, the FNC exhibits high discharge voltage of 3.15 V at 0.01C and superior rate capability in lithium primary batteries. At a high rate of 20C, power density of 33,694 W kg–1 and energy density of 1,250 Wh kg–1 are achieved. Moreover, FNC also demonstrates notable electrochemical performance in sodium/potassium-CF x primary batteries. This new-type alkali-metal/CF x primary batteries exhibit outstanding rate capability, rendering them with vast potential in high-power applications. [ABSTRACT FROM AUTHOR]

The use of all‐solid‐state lithium metal batteries (ASSLMBs) has garnered significant attention as a promising solution for advanced energy storage systems. By employing non‐flammable solid electrolytes in ASSLMBs, their safety profile is enhanced, and the use of lithium metal as the anode allows for higher energy density compared to traditional lithium‐ion batteries. To fully realize the potential of ASSLMBs, solid‐state electrolytes (SSEs) must meet several requirements. These include high ionic conductivity and Li+ transference number, smooth interfacial contact between SSEs and electrodes, low manufacturing cost, excellent electrochemical stability, and effective suppression of dendrite formation. This paper delves into the essential requirements of SSEs to enable the successful implementation of ASSLMBs. Additionally, the representative state‐of‐the‐art examples of SSEs developed in the past 5 years, showcasing the latest advancements in SSE materials and highlighting their unique properties are discussed. Finally, the paper provides an outlook on achieving balanced and improved SSEs for ASSLMBs, addressing failure mechanisms and solutions, highlighting critical challenges such as the reversibility of Li plating/stripping and thermal runaway, advanced characterization techniques, composite SSEs, computational studies, and potential and challenges of ASS lithium–sulfur and lithium–oxygen batteries. With this consideration, balanced and improved SSEs for ASSLMBs can be realized. [ABSTRACT FROM AUTHOR]