Cobalt-free lithium-rich manganese-based cathode materials (LRMs) have garnered significant attention due to their high specific capacity and low cost, making them promising candidates for next-generation lithium-ion batteries. However, their practical application remains limited by low initial coulombic efficiency and significant capacity and voltage degradation during cycling. Therefore, structural design has become a key strategy to overcome these challenges. While polycrystalline materials have been extensively studied, single-crystal cathode materials have recently gained research focus due to their superior structural stability and enhanced cycling performance. Nonetheless, single-crystal materials still suffer from fundamental issues such as lattice oxygen instability and sluggish lithium-ion diffusion kinetics, which hinder long-term stability and rate capability. To address these limitations, fluorine doping is widely recognized as an effective approach to stabilize the lattice oxygen framework and improve lithium-ion transport. Herein, polyvinylidene fluoride (PVDF) is introduced as a safe, controllable, and industry-compatible fluorine source. During high-temperature sintering, PVDF decomposes and enables uniform in situ fluorination of the single-crystal Li1.2Ni0.2Mn0.6O2 lattice. The resulting Li1.2Ni0.2Mn0.6O1.95F0.05 cathode delivers an initial discharge capacity of 242 mAh g- 1 at 1C and retains 83.14% capacity after 200 cycles, demonstrating excellent cycling stability and improved lithium-ion diffusion kinetics. This facile and scalable single-crystal fluorination strategy offers valuable insights for advancing high-energydensity, cobalt-free lithium-rich cathodes for next-generation lithium-ion batteries.

Understanding and tuning π-d conjugation is essential for advancing metal-organic materials in metal-ion batteries. Here, we applied density functional theory (DFT) to systematically investigate π-d conjugation in metal-organic systems. Using a Ni-based metal-organic polymer as the model system, our results show that strong π-d conjugation originates from effective hybridization between Ni 3d orbitals and ligand π orbitals mediated by bridging groups. Among the three bridging groups (─O, ─S, and ─NH), S provides the strongest coupling due to favorable orbital overlap. Ligand functionalization further modulates this interaction via energy level alignment, where electron-withdrawing groups enhance π-d hybridization and charge delocalization, while electron-donating groups weaken it. These factors collectively influence Li adsorption and electrochemical performance. This study establishes a unified design strategy combining bridge atom selection and functional group tuning to optimize π-d conjugation for high- performance metal-organic electrode materials.

ABSTRACT Fast charging technology in lithium‐ion batteries (LIBs) is critically dependent on the mechanical robustness of electrode materials, which must withstand significant stress and strains during rapid cycling. However, a comprehensive study of the relationship between mechanical property and battery performance remains rare, particularly under fast‐charging conditions. In this work, we bridge this knowledge gap by developing a one‐dimensional conductive metal–organic polymer (MOP, i.e., Cu‐DDA) that exhibits high fracture toughness for fast charging. Moreover, the robust π‐d conjugation structure of Cu‐DDA minimizes lattice deformation and volume expansion, thereby preserving structural stability under high current densities. As a result, the Cu‐DDA cathode achieves an attractive reversible capacity of 190 mAh g −1 at a high current density of 15 A g −1 and remarkable capacity retention of 78% after 400 cycles at 5 A g −1 . This study demonstrates the significant impact of inherent mechanical properties, providing important design insights for next‐generation fast‐charging electrode materials.

Organic electrode materials (OEMs) hold great promise for sodium-ion batteries (SIBs) due to their exceptional structural tunability and sustainability. However, the development of OEMs with fast redox kinetics and robust structure integrity remains challenging, especially under wide-temperature conditions. Herein, we propose an effective strategy to address both sluggish redox kinetics and structure instability in OEMs by constructing an intramolecular redox-site interplay effect. This effect is demonstrated by two hexaazatrinaphthylene-carboxylates isomers, namely HATN-m-COONa and HATN-o-COONa. Systematic experimental and theoretical calculation results jointly reveal the intramolecular redox-site interplay effect in HATN-o-COONa decreases the rigid π-π stacking interactions and minimizes the skeleton structure distortion, offering faster redox kinetics and enhanced structure integrity in HATN-o-COONa compared to HATN-m-COONa (without intramolecular redox-site interplay effect). Consequently, HATN-o-COONa exhibits superior rate performance (258 mA h g-1 at 10 A g-1) and enhanced cycle stability (93% after 1000 cycles at 5 A g-1) compared to HATN-m-COONa. More importantly, HATN-o-COONa demonstrates exceptional wide-temperature adaptability, ranging from 60 °C (343 mA h g-1 at 5 A g-1) to -40 °C (315 mA h g-1 at 0.1 A g-1). This work establishes a promising design rationale for developing fast-charging and wide-temperature adaptable OEMs for energy storage systems.

Carbonyl sulfide (COS) removal via catalytic hydrolysis is a cornerstone of industrial purification; however, conventional catalysts suffer from sluggish kinetics, rapid deactivation, and poor tolerance to harsh flue gas components (dust and HCl). This research aims to optimize the working condition for ZrO2@γ-Al2O3 hollow sphere catalyst and elucidate its superior anti-poisoning mechanisms and long-term stability under complex process conditions. Under the optimized conditions (80℃, 38

Rechargeable sodium-ion batteries (SIBs) offer a promising solution for large-scale energy storage systems due to their abundant availability and cost-effectiveness. Recently, all-solid-state sodium-ion batteries (ASSSIBs) with solid electrolytes have garnered significant attention for their superior energy density and safety compared to traditional SIBs with organic liquid electrolytes (OLEs). Despite notable progress, the sluggish ion transport remains a substantial barrier to the practical application of ASSSIBs. This review comprehensively examines the ion transport mechanisms and challenges in solid electrolytes, electrode/solid electrolyte interfaces, and electrodes of ASSSIBs. Additionally, it systematically explores representative strategies to enhance ion transport through engineering solid electrolytes, interfaces, and electrodes. Furthermore, it addresses the remaining challenges and future directions for advancing high-performance practical ASSSIBs. By providing development history, fundamental insights, effective strategies, and perspectives on designing ASSSIBs for rapid ion transport, this review could serve as a comprehensive guide for scientific research and practical development in the field.

High-nickel layered oxide LiNi x Co y Mn1-x-y O2 (NCM, x >= 0.8) materials are considered optimal cathodes for lithium-ion power batteries owing to their high energy density, commendable cycling performance, and cost-effectiveness. However, structural collapse and interface instability during cycling result in diminished cycling stability, significantly hindering their commercial viability. Consequently, this study proposes inducing a multifunctional integrated structure via the quenching process, successfully synthesizing a modified NCM cathode with an inner La/Ca-doped layered structure and a near-surface Li-deficient La x Ca y NiO3-delta structure. A series of tests, complemented by density functional theory (DFT) calculations, demonstrated that inner La/Ca doping effectively increases the lattice spacing, enhancing the Li+ diffusion coefficient and lattice stability. The external La x Ca y NiO3-delta structure offers a stable interface and abundant oxygen vacancies, significantly suppressing side reactions and oxygen evolution reactions at the interface. More importantly, DFT calculations analyzed the doping preference of La3+/Ca2+ in NCM, revealing that La3+/Ca2+ predominantly occupy Li sites, with some La3+ also occupying Ni sites, which further confirming the feasibility of ion exchange. Additionally, electronic effects of La 3d and Ca 2p orbitals effectively enhance the electrical conductivity of NCM cathodes. Subsequent electrochemical tests demonstrated that the multifunctional integrated structure significantly enhanced the rate performance and cycling stability of high-nickel NCM cathodes. At a 4.3 V cutoff voltage, the LCNCM cathode exhibited significant improvements in cycling stability at 0.5, 1.0, and 2.0C rates. Even at the higher cutoff voltage of 4.4 V, the LCNCM cathode maintained a reversible capacity of 185.0 mAh g-1 and a capacity retention rate of 89.7% after 100 cycles at 1.0C, demonstrating substantial improvements in electrochemical performance.

High-nickel layered oxide LiNixCoyMn1-x-yO2 (NCM, x ≥ 0.8) materials are considered optimal cathodes for lithium-ion power batteries owing to their high energy density, commendable cycling performance, and cost-effectiveness. However, structural collapse and interface instability during cycling result in diminished cycling stability, significantly hindering their commercial viability. This study reports a strategy to improve the stability of the cathode structure and suppress surface degradation of high-nickel NCMs by introducing LCO (Li2CeO3) coatings. The LCO coating provides a stable surface structure and enhances structural stability under high Li-extraction conditions, significantly mitigating the formation of unstable cathode-electrolyte interfaces and reducing electrolyte corrosion and side reactions. Meanwhile, the partially bulk-phase doped Ce4+ primarily optimizes the lattice parameters by modulating the crystal structure and altering the electronic environment of the transition metal layer, which promotes the Li+ diffusion kinetics and effectively suppresses the bulk expansion and irreversible phase transition. As expected, the modified cathode exhibits superior improvements in rate performance and cycling stability, with an initial discharge capacity of 202.5 mA h g-1 and a first-cycle Coulombic efficiency of 95.4%, compared to 89% for pristine NCM. Notably, 1.0%-LCO@NCM maintains a capacity retention of 83.52% after 200 cycles at 1.0 C, significantly higher than the 65.29% retention of pristine NCM under the same conditions. Furthermore, 1.0%-LCO@NCM consistently demonstrates lower interfacial impedance and higher Li+ diffusion coefficients throughout the cycling process. After 200 cycles, its impedance remains lower, with reduced interfacial film impedance. The oxygen vacancy-rich surface LCO achieves dual optimization of the structural integrity and oxygen redox activity of the high-Ni cathode, further improving cycle life and multiplier performance.

The evolution of modern society demands sustainable rechargeable lithium-ion batteries (LIBs) with higher capacity and improved safety standards. High voltage Ni-rich layered transition metal oxides (i.e., LiNi1-x-yCoxMnyO2, NCM) have emerged as one of the most promising cathode materials in meeting this demand. However, the instability of Ni-rich NCMs cathodes presents challenges in large-scale commercialization. This review examines the energy storage mechanism, e.g., possible (electro)chemical reactions, occurring at the bulk and surface and degradation mechanism of the Ni-rich NCMs cathode materials. To address the challenging instability issue, we highlight recent advances and strategies for bulk and surface engineering of Ni-rich NCMs, including lattice, composition, and microstructure engineering, and electrolyte and materials interfacial engineering. By addressing degradation mechanisms and improving overall stability, this work sheds lights on the potential avenues on the commercialization of Ni-rich cathode-based high-performance LIBs.

Redox-active polymers are regarded as one of the most promising electroactive materials for non-lithium electrochemical energy storage devices due to the inherent molecular flexibility that can tolerate the structure change during the charge/discharge process. Their diverse functional groups provide abundant active sites to accommodate large-sized electrolyte ions. In this work, for the first time, the 2,2,6,6-tetramethylpiperidine-1oxyl (TEMPO) radical group, equipped at poly(TEMPO-acrylamide) (PTAm), is employed as an active cathode for potassium dual-ion batteries (KDIBs). Carbon nanotubes (CNTs) assist morphological engineering of the PTAm to create a conductive nanostructured composite, namely PTAm@CNTs. Systematic material characterizations and electrochemical evaluation suggest that the PTAm@CNTs nanocomposite possesses significant surface area and nanopores, enabling enhanced electronic and ionic conductivity. The PTAm@CNTs cathode reversibly stores hexafluorophosphate (PF6-) anions in KDIBs, delivering high energy density, rate capability, and robust cycling stability. The fast reaction kinetics of nitroxide radicals (N-O.), the redox-active groups on the PTAm, and their association with the PF6- anions contribute to the dual-ion storage. As a result, the PTAm@CNTs cathode delivers a high specific capacity of 108 mAh g(-1) at 2 A g(-1) (16.8C) over 300 cycles. The work suggests a promising pathway to design and synthesize functional organic electrode materials for potassium dual-ion batteries.

Due to the seamless interfaces between solid polymer electrolytes (SPEs) and electrode materials, SPEs-based all-solid-state sodium-ion batteries (ASSSIBs) are considered promising energy storage systems. However, the sluggish Na + transport and uncontrollable Na dendrite propagation still hinder the practical application of SPEs-based ASSSIBs. Herein, Ca-doped CeO 2 (Ca−CeO 2 ) nanotube framework is synthesized and integrated with poly (ethylene oxide) methyl ether acrylate-perfluoropolyether copolymer (PEOA-PFPE), resulting in multifunctional solid nanocomposite electrolytes (namely SNEs, i.e., PEOA-PFPE/Ca−CeO 2 ). Our investigations demonstrate that the fluorous effect incurred by the fluorine-containing PEOA-PFPE and the oxygen vacancy effect induced by the Ca−CeO 2 framework could synergistically promote the dissociation of sodium salt, ultimately enhancing the Na + mobility in SNEs. Besides, the resultant SNEs construct rapid Na + transport channels and homogenize the Na deposition in SNEs/Na interface, which effectively prevents the Na dendrite growth. Furthermore, the assembled carbon-coated sodium vanadium phosphate (NVP@C)||PEOA-PFPE/Ca−CeO 2 ||Na coin cell delivers impressive rate capability of 97.9 mAh g −1 at 2 C and outstanding cycling stability with capacity retention of 84.3 % after 300 cycles at 1 C. This work illustrates that constructing multifunctional SNEs via incorporating functional inorganic frameworks into fluorine-containing SPEs could be a promising strategy for the commercialization of robust and high-performance ASSSIBs.

From the perspective of safe electric vehicle operation, accurately assessing the state of health (SOH) and remaining useful life (RUL) of lithium batteries holds paramount importance. This paper introduces a novel multi-task learning data-driven model named GBLS Booster, focusing on the joint estimation and prediction of SOH and RUL. GBLS Booster integrates the strengths of GBLS, offering reduced computation, swift computing speed, and harnesses the powerful feature extraction capabilities of the CNN-Transformers algorithm-based Booster. Additionally, the Tree-structured Parzen Estimator (TPE) algorithm is applied to optimize the model. In this study, 10 healthy indicators (HIs) are devised to capture variations in battery SOH. These HIs are derived from readily available sensor data, encompassing current, voltage, and temperature information. The random forest method (RF) is employed to further refine features and minimize data dimensions. Concerning the RUL prediction, the capacity data is often plagued by significant noise. To address this challenge, the complete empirical mode decomposition (CEEMDAN) method is employed for noise reduction decomposition, followed by the utilization of the Pearson correlation coefficient to eliminate noisy data points. The proposed method is rigorously evaluated using the NASA dataset and CLACE dataset for modeling simulation and verification. Comparative analysis with other algorithms is conducted. The results demonstrate the superior performance of the proposed model, showcasing exceptional accuracy (with a minimum Mean Absolute Percentage Error (MAPE) of 0.3348 % for SOH and a minimum Relative Error (RE) of 0.01 % for RUL), robustness, and generalization capabilities.

Metal–Organic Polymers (MOPs) have attracted growing attention for lithium-ion battery (LIB) applications due to their merits in orderly ionic transportation and robust structure stability in electrochemical reactions. However, they suffer from poor electronic conductivity. In this work, we apply first-principles density functional theory to explore the potential of three one-dimensional (1D) electrically conductive C6H2S4TM (TM = Fe, Co, and Ni) MOPs with the π–d conjugated coordination as anode materials for Li+ ions storage. Our theoretical results reveal that these 1D MOPs possess a superior theoretical capacity of over 748 mA h g−1. In particular, the 1D C6H2S4Ni MOP shows an exceptional theoretical specific capacity of 1110 mA h g−1 based on the three-electron transferring reaction, which significantly outperforms the traditional graphite-based anode material in LIBs. Moreover, the resonant charge transfer between Ni metal and ligand within the 1D C6H2S4Ni MOP reduces the diffusion energy barrier of the Li atoms when they migrate on the surface of the MOP. The ultrahigh theoretical specific capacity of the C6H2S4Ni MOP predicts that it can be a promising anode material for LIBs.

The photovoltaic (PV) industry annually generates substantial quantities of silicon cutting waste (SCW), posing significant environmental pressure and leading to considerable resource wastage. To address this issue and capitalize on wasted high-purity silicon, a novel, highly dispersed Si-based composite from SCW was developed for use as a high-performance anode in lithium-ion batteries. This study presents a novel approach for the fabrication of a composite material comprising SCW-derived silicon nanoparticles (SiNPs) and carbon nanotubes (CNTs) embedded within a carbon nanofiber (CNFs) network (Si/CNTs@CNFs). SCW was subjected to acid washing, high-temperature pyrolysis, and ball milling to produce nanoscale SiNPs. These SiNPs were then mixed with CNTs to produce Si/CNTs@CNFs via a modified electrospinning process, in which poly(vinylpyrrolidone) (PVP) was used as a stabilizing agent to prevent the agglomeration of SiNPs. This ensured that both SiNPs and CNTs were uniformly dispersed throughout the interconnected CNFs, leading to enhanced electrical conductivity, improved structural stability, and better electrochemical performance for this Si-based anode. The highly dispersed Si/CNTs@CNFs composite material exhibits a reversible capacity of 571.5 mAh g(-1) after 200 cycles at a current density of 1 A g(-1), showcasing superior electrical performance compared to samples without PVP or without ball milling. This study presents a novel pathway for recycling silicon cutting waste from the solar PV industry, thereby contributing to sustainability and the advancement of renewable energy resources.

A ten-fold higher specific capacity than commercial graphite anodes makes lithium metal anodes extremely attractive for rechargeable battery applications. However, the safety concerns associated with lithium dendrites represent a major barrier to the practical application of lithium metal batteries. Over the past decades, several mechanisms for the growth of lithium dendrites have been proposed from different perspectives. This has led to a variety of strategies to protect the lithium metal anode, such as preparation of artificial solid electrolyte interphase (SEI) and pseudo-liquid anodes. In this review, we present an overview of protection strategies for lithium metal anodes in terms of preventing lithium dendrite growth and regulating lithium deposition behaviours or healing the existing lithium dendrites. Firstly, the mechanisms of dendrite growth and anode corrosion are summarized and compared to better understand the lithium-ion deposition behaviours, which is critical for theoretically guiding the exploration of highly stable lithium anodes. Subsequently, the potential for integrating different strategies is discussed to combine and make full use of the advantages of each strategy, which can facilitate the development of emerging strategies and the improvement of established ones. The availability of the proposed strategies will further narrow the gap between experimental research and the commercial application of rechargeable lithium metal batteries.

Organic electrode materials (OEMs), valued for their sustainability and structural tunability, have been attracting increasing attention for wide application in sodium-ion batteries (SIBs) and other rechargeable batteries. However, most OEMs are plagued with insufficient specific capacity or poor cycling stability. Therefore, it′s imperative to enhance their specific capacity and cycling stability through molecular design. Herein, we designed and synthesized a heteroaromatic molecule 2,3,8,9,14,15-hexanol hexaazatrinaphthalene (HATN-6OH) by the synergetic coupling of catechol (the precursor of ortho -quinone)/ ortho -quinone functional groups and HATN conjugated core structures. The abundance of catechol/ ortho -quinone and imine redox-active moieties delivers a high specific capacity of nine-electron transfer for SIBs. Most notably, the π–π interactions and intermolecular hydrogen bond forces among HATN-6OH molecules secure the stable long-term cycling performance of SIBs. Consequently, the as-prepared HATN-6OH electrode exhibited a high specific capacity (554 mAh g −1 at 0.1 A g −1 ), excellent rate capability (202 mAh g −1 at 10 A g −1 ), and stable long-term cycling performance (73 % after 3000 cycles at 10 A g −1 ) in SIBs. Additionally, the nine-electron transfer mechanism is confirmed by systematic density functional theory (DFT) calculation, attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and Raman analysis. The achievement of the synergetic coupling of the redox-active sites on OEMs could be an important key to the enhancement of SIBs and other metal-ion batteries.

High-entropy oxides (HEOs) can be well suited for lithium-ion battery anodes because of their multi-principal synergistic effect and good stability. The appropriate selection and combination of elements play a crucial role in designing conversion-type anode materials with outstanding electrochemical performance. In this study, we have successfully built a single-phase spinel-structured HEO material of (Mn0.23Fe0.23Co0.22Cr0.19Zn0.13)3O4 (HEO-MFCCZ). When the HEO-MFCCZ materials transform into a coexisting state of amorphous and nanocrystalline structures during the cycling process, the inert Zn element can initiate a pegging effect, causing enhanced stability. The transition also introduces many defect sites, effectively reducing the potential barrier for ion transport and accelerating ion transport. The increased electronic and ionic conductivities and pseudocapacitive contribution significantly enhance the rate performance. As a result, a unique and practical approach is provided for developing anode materials for lithium-ion batteries.

Hard carbons (HCs) have great potential as anode material for high‐performance potassium ion batteries (PIBs). However, due to the complexity of HCs, the relationship between their structures and potassium (K) storage behaviors is still not quite clear. Here, three types of HCs with different structures are designed for further understanding the electrochemical storage processes. Among them, the carbon spheres (CS) exhibit impressive rate performance (161.6 mAh g−1 at 2 A g−1) and cycle stability (140.2 mAh g−1 at 2 A g−1 after 500 cycles). The superior performance of CS can be mainly ascribed to the intercalation into its locally‐ordered carbon nanocrystallites, and the charge/discharge processes are further characterized with significant pseudocapacitive dominating. Suitable nanocrystalline size and the ratio of defects with proper morphology are the key factors to improve K storage efficiency. This work will contribute to understanding the role of these factors in the K storage performance of carbon materials.

Organic electrode materials (OEMs) can deliver remarkable battery performance for metal-ion batteries (MIBs) due to their unique molecular versatility, high flexibility, versatile structures, sustainable organic resources, and low environmental costs. Therefore, OEMs are promising, green alternatives to the traditional inorganic electrode materials used in state-of-the-art lithium-ion batteries. Before OEMs can be widely applied, some inherent issues, such as their low intrinsic electronic conductivity, significant solubility in electrolytes, and large volume change, must be addressed. In this review, the potential roles, energy storage mechanisms, existing challenges, and possible solutions to address these challenges by using molecular and morphological engineering are thoroughly summarized and discussed. Molecular engineering, such as grafting electron-withdrawing or electron-donating functional groups, increasing various redox-active sites, extending conductive networks, and increasing the degree of polymerization, can enhance the electrochemical performance, including its specific capacity (such as the voltage output and the charge transfer number), rate capability, and cycling stability. Morphological engineering facilitates the preparation of different dimensional OEMs (including 0D, 1D, 2D, and 3D OEMs) via bottom-up and top-down methods to enhance their electron/ion diffusion kinetics and stabilize their electrode structure. In summary, molecular and morphological engineering can offer practical paths for developing advanced OEMs that can be applied in next-generation rechargeable MIBs. Graphical abstract