The growing reliance on batteries in modern society highlights the crucial role of separators in energy storage devices. As the demand for high-performance batteries increases, developing advanced separators─guided by a deep understanding of physical phenomena and structure-property relationships─becomes critical for next-generation energy storage systems. Recent developments in separator technology have evolved from simple polymer-based materials to sophisticated organic/inorganic composites. A key innovation in this field is the incorporation of inorganic particles into separators, which significantly improves their physical and chemical performance. Among these inorganic additives, zeolites and other porous materials stand out due to their ordered pore structures, high porosity, large specific surface areas, and excellent thermal stability. This review highlights the chemical and physical properties of zeolites that make them valuable for designing composite separators. We explore the engineering of polymer/zeolite composite separators, with an emphasis on enhancing mechanical strength, increasing ionic conductivity, and promoting favorable chemical interactions. Furthermore, we evaluate the suitability of synthetic zeolites in various types of energy storage systems, focusing on their structural and thermal advantages relevant to separator performance. Finally, we discuss future research directions, potential technological advancements, and the challenges associated with integrating zeolites into catalysts, adsorbents, battery separators, and solid-state electrolytes.

Simultaneously achieving stable lithium metal batteries (LMBs) under cryogenic and high-voltage conditions remains a fundamental challenge due to uncontrolled interfacial chemistry at lithium anodes and nickel-rich cathodes. Here, we report an intramolecular polarization strategy that jointly regulates Li+ solvation dynamics, solid electrolyte interphase (SEI) formation, and cathode electrolyte interphase (CEI) stress dissipation. An intramolecularly polarized electrolyte featuring orthogonally arranged electron donor-acceptor moieties with a dipole moment (∼4.2 D) establishes a potential-dependent solvation screening effect, reducing Li+ desolvation energy to 38.1 kJ mol-1, while enabling anodic stability beyond 5.3 V. The tailored solvation chemistry induces spontaneous formation of dual-gradient interphases composed of a LiF-rich SEI and a boroxane-incorporated CEI with an interface modulus ∼20 nN. Consequently, Li||Li symmetric cells exhibit stable cycling over 16 000 h with a minimal polarization of 8.3 mV. Full cells employing LiNi0.8Co0.1Mn0.1O2 cathodes retain 90% capacity after 1000 cycles at 4.5 V and maintain 80% at 4.9 V. 3 Ah pouch cells achieve a high energy density of 509 Wh kg-1 at 30°C with 96.8% capacity retention after 80 cycles, while delivering 439.1 Wh kg-1 at -30°C. This work establishes a molecular polarization paradigm for electrolyte and interphase engineering toward high-energy-density LMBs under extreme conditions.

The pursuit of high-energy-density lithium-sulfur (Li-S) batteries necessitates the use of lean electrolyte conditions. However, this goal is severely hampered by the sluggish kinetics of the sulfur reduction reaction (SRR), especially in the "solid-solid" conversion stage, where each step requires distinct active sites with specific electron-donating capabilities. Herein, we report a catalyst architecture that integrates "long-range order" with "local disorder", creating gradient-ordered active sites through amorphous nanodomain modification and precise local electronic structure regulation. This catalyst, termed an electron-pinned interface catalyst (EPIC) and denoted as a-FeOOH@Fe/AlOx, exhibits synergistic catalytic enhancement via multi-level electronic interactions. Operando studies and DFT simulations reveal that the catalyst establishes conductive pathways facilitated by its gradient electron-donating properties, thereby decoupling the SRR process and significantly enhancing the "solid-solid" conversion efficiency. Under lean electrolyte conditions, this catalyst achieves a high areal capacity of 10.7 mAh·cm-2 at a sulfur loading of 10.2 mg·cm-2, exhibits 94.2% capacity retention after 150 cycles in a pouch cell, and enables stable operation of a 3.6 Ah pouch cell with an energy density of 418.6 Wh·kg-1. This strategy effectively overcomes the reaction kinetic limitations in lean electrolyte conditions, providing valuable insights and a novel design paradigm for future high-energy-density Li-S batteries.

Tellurium (Te), a significant metalloid element, holds considerable potential in applications including electronic semiconductors, thermoelectric converters, efficient catalysts, and advanced energy storage systems. Nevertheless, the intricate electrochemical behaviors of Te across varied systems remain insufficiently elucidated, involving multiple factors such as redox reaction pathways in different electrolytes, mechanisms of Te nucleation and growth, interfacial reaction dynamics, and interactions with varying charge carriers. This review systematically summarizes the electrochemical characteristics of Te‐based materials in different configurations, aiming to decipher the complexity of kinetic processes and thereby help provide deeper insights toward optimizing the electrodeposition of Te. Then, the correlation between electrodeposition parameters and the resulting structure and morphology of the deposits is elaborated to achieve greater control of composition and morphology. Additionally, this review surveys important aspects of the application of Te in advanced energy storage, secondary batteries, and thin‐film solar cells. A systematic outline of the electrochemical reaction mechanisms in both monovalent and multivalent metal‐ion batteries is presented. By integrating fundamental electrochemical mechanisms, multiscale identification of reaction kinetics, and device‐level application insights, this work establishes a comprehensive framework and practical guidelines for fabricating stable Te‐based materials efficiently while outlining potential future research directions.

The rapid growth of lithium-ion batteries has intensified the need for efficient recycling of spent LiNi0.5Co0.2Mn0.3O2 (NCM) cathodes. However, direct regeneration is hindered by the high-spin state of Ni2+ (S = 1) in degraded surface structures, which impedes Li+ intercalation and limits repair efficiency. Here, we introduce a strong electronegative ligand field to modulate the surface NiO6 coordination environment, enabling precise regulation of Ni spin state and electronic structure. This strategy alters the occupancy of Ni eg orbitals, converting high-spin Ni2+ (t2 g 6eg 2, S = 1) to low-spin Ni3+ (t2 g 6eg 1, S = 1/2) while downshifting the Ni d-band center. The resulting electronic reconfiguration weakens Ni-Li interactions, enabling efficient lithiation and regeneration of the degraded NCM black mass. The regenerated cathode, when assembled into pouch cells, exhibits Ah-level capacity with electrochemical performance comparable to commercial counterparts. This work establishes a direct correlation between Li+ transport kinetics and the Ni spin-state regulation, offering a new chemical paradigm for the direct regeneration of degraded cathodes.

Solid-state polymer electrolytes (SSEs) are limited by tortuous ion pathways and uncontrolled anion transport, and despite the incorporation of inorganic components, composite electrolytes still suffer from fundamental constraints in ion transport and long-term stability. Here we report a composite electrolyte in which exfoliated MCM-22 lamellae are directionally aligned throughout the polymer matrix via a shear-flow-assisted evaporation process. The resulting long-range ordered framework (Herman factor = 0.91) promotes continuous ion transport pathways while its Lewis-acidic micropores confine TFSI- within the lamellar domains, yielding cooperative structural-chemical regulation of ion transport. This architecture reduces PEO crystallinity and elevates the Li+ transference number to 0.47. As a consequence, the aligned electrolyte exhibits improved electrochemical durability, sustaining stable Li plating/stripping for over 1600 h and retaining 76.1 % of its capacity after 1200 cycles in a Li‖LFP cell at 60°C. These findings establish aligned zeolite frameworks as a powerful platform for designing next-generation solid polymer electrolytes.

Li-ion batteries (LIBs) have powered society for decades since their first commercialization in 1991. However, the current Li-ion chemistry deploying traditional graphite anode is approaching its energy density limit and struggling to meet the growing demand. The use of pure metallic Li with almost ten folds of anodic specific capacity is therefore critical to realize a higher energy density Li metal battery (LMB). A pure Li metal anode faces great challenges before its readiness for commercial applications. In addition to safety issues, which are a subject researched and reviewed widely, drastic Li loss (including the loss from active utilization or storage) is often overlooked, resulting in reduced capacity and eventually limited battery longevity. The Li loss in conventional liquid electrolyte settings, refers to the proportion of Li not taking part in an electrochemically active role for generating energy, and can be mainly categorized as inactive metallic Li, solid–electrolyte interphase (SEI) dissolution, and Li corrosion. To date, the underlying mechanisms involving these Li loss pathways and their dependence on each other are subject of ongoing investigations. This paper summarizes the major forms of Li loss processes when using a Li metal anode in an LMB, and existing strategies to mitigate these losses.

Arising from the increasing demand for electric vehicles (EVs), Ni‐rich LiNixCoyMnzO2 (NCM, x + y + z = 1, x ≥ 0.8) cathode with greatly increased energy density are being researched and commercialized for lithium‐ion batteries (LIBs). However, parasitic crack formation during the discharge–charge cycling process remains as a major degradation mechanism. Cracking leads to increase in the specific surface area, loss of electrical contact between the primary particles, and facilitates liquid electrolyte infiltration into the cathode active material, accelerating capacity fading and decrease in lifetime. In contrast, Ni‐rich NCM when used as a single crystal exhibits superior cycling performances due to its rigid mechanical property that resists cracking during long charge–discharge process even under harsh conditions. In this paper, we present comparative investigation between single crystal Ni‐rich LiNi0.92Co0.04Mn0.04O2 (SC) and polycrystalline Ni‐rich LiNi0.92Co0.04Mn0.04O2 (PC). The relatively improved cycling performances of SC are attributed to smaller anisotropic volume change, higher reversibility of phase transition, and resistance to crack formation. The superior properties of SC are demonstrated by in situ characterization and battery tests. Consequently, it is inferred from the results obtained that optimization of preparation conditions can be regarded as a key approach to obtain well crystallized and superior electrochemical performances.

Lithium-sulfur (Li-S) batteries are regarded as promising candidates for next-generation secondary batteries due to their high energy density and cost-effectiveness. However, the sluggish conversion kinetics of lithium polysulfide (LiPSs) intermediates during charge/discharge cycles severely hinder their practical application. Herein, we propose a relay catalysts design strategy to accelerate the sulfur reduction conversion process in Li-S batteries. To validate this approach, we synthesized a faujasite-type molecular sieve (FAU)-Bi2O3 relay catalyst, in which each component is tailored to optimize distinct stages of the catalytic process. FAU, with its abundant microporous structure, effectively captures and channels LiPSs toward the Bi2O3 interface, where catalytic sites promote rapid conversion and enhance reaction kinetics. Furthermore, integrating the FAU-Bi2O3 catalyst onto a commercial separator not only boosts electrochemical performance but also imparts excellent flame retardancy. Li-S batteries with FAU-Bi2O3 achieve a high specific capacity of 846.8 mAh g- 1 after 100 cycles, while the pouch cell maintains a capacity retention of 81.4 % after 70 cycles. This work presents a rational catalyst design strategy, offering a new pathway for advancing Li-S battery technology toward practical implementation.

Bismuth is a promising anode material for potassium-ion batteries due to its green, non-toxic and high theoretical capacity (384 mAh g-1). However, the sluggish reaction kinetics and excessive volume expansion during cycling limit its practical application. Herein, Bi-induced few-layered graphite frameworks are in situ encapsulated on the surface of Bi nanoparticles, based on the mechanism of graphitization by rearrangement of interstitial carbon atoms during the nucleation process of Bi, while these composite particles are embedded in Bi-doped porous carbon fibers composite. The graphite frameworks can stabilize the structure while serving as an efficient interfacial transfer layer, enabling rapid transport of both potassium ions and electrons. Bi atoms doped into the carbon fiber matrix effectively enhances the potassium ion transport kinetics in amorphous carbon by lowering the migration energy barrier of potassium ions in the carbon layer. The porous structure effectively alleviates the volume expansion of Bi nanoparticles during cycling, which synergistically results in superior high-rate performance and cycling stability. Finally, the capacity can reach 215 mAh g-1 at 10 A g-1, and a capacity retention rate of 83.8% is achieved after 6000 cycles at 10 A g-1 with an ultra-low decay rate of 0.00278% per cycle.

Lithium metal batteries (LMBs) offer exceptional energy density and output voltage. However, their practical application remains hindered by sluggish ion transport and uncontrolled lithium dendrite formation, particularly under fast-charging conditions. Here, we report a facet-engineered anion-regulating separator based on zeolitic imidazolate framework-8 (ZIF-8) with preferentially crystal-exposed (110) facets. The coordinatively unsaturated Zn centers on this surface serve as Lewis acid sites that selectively anchor bis(trifluoromethanesulfonyl)imide anions (TFSI − ), inducing directional Li + flux and suppressing dendritic growth. Concurrently, the microporous framework facilitates spatial lithium confinement, mitigating local current density and enhancing interfacial stability. As a result, the engineered separator enables ultra-stable cycling of Li||Cu cells for over 1400 cycles at 2 mA cm −2 and 1 mAh cm −2 , delivering an average Coulombic efficiency of 98.7%. In full-cell configurations, LiFePO 4 (LFP) cells exhibit 99.9% Coulombic efficiency over 3000 cycles at 5 C, while high-loading Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811, 12.30 mg cm −2 ) cell retains 84.4% of its capacity after 135 cycles. Furthermore, a Li||LFP pouch cell with a high cathode loading of 19.92 mg cm −2 demonstrates robust cycling over 170 cycles. These findings establish facet-engineered separators based on framework materials as a versatile and scalable strategy for advancing stable and fast-charging metal batteries.

The hydrometallurgical electrodeposition process has become a hot research field for metallic lead recovery from spent lead paste due to its energy-efficient and eco-friendly features. However, traditional electrodeposition process is usually carried out under strong acid or alkaline systems, accompanied by the side reaction of lead dioxide. This study proposed a closed-loop ammonium acetate leaching-electrodeposition route for metallic lead recovery from spent lead paste. The spent lead paste was firstly leached by a neutral leaching solution of NH4Ac, HAc and H2O2. After filtration, the leaching solution was electrodeposited to produce metallic lead. Anion exchange membrane was introduced to avoid anodic lead dioxide generation in the electrodeposition process. Under the optimal conditions, the cathode current efficiency and energy consumption were 91.62 % and 625 kWh/t Pb, respectively. The NH4Ac leachant was regenerated from the eletrolyte by removing soluble SO4 2- with addition of Ba(Ac)2 to generate BaSO4 by-product. The regenerated NH4Ac leachant was then reused in the nextround leaching process, thus realizing a closed-loop process. In five leachant recirculation processes, the leaching ratio, electrodeposition ratio and total recovery ratio of lead remained relatively stable, within the ranges of 95.7-97.3 wt %, 98.6-99.6 wt % and 94.4-96.4 wt %, respectively. By upgrading of the metallic Pb product, the purity could finally reach 99.998 %. This study proposes an environmentally and economically friendly process for lead recovery from spent lead paste and other lead-containing wastes.

Direct regeneration of spent lithium-ion batteries offers economic benefits and a reduced CO2 footprint. Surface prelithiation, particularly through the molten salt method, is critical in enhancing spent cathode repair during high-temperature annealing. However, the sluggish Li+ transport kinetics, which predominantly relies on thermally driven processes in the traditional molten salt methods, limit the prelithiation efficiency and regeneration of spent cathodes. Here, we introduce a special molecular configuration (benzoate) into molten salts that facilitates rapid Li+ transport to the surface of LiNi0.5Co0.2Mn0.3O2 (NCM) via a quasi-Grotthuss topochemistry mechanism. This approach effectively avoids the phase transitions that could adversely degrade the electrochemical performance due to insufficient lithiation during the repair process. Computational and experimental analyses reveal that the system enables fast Li+ migration through the topological hopping of benzoate in organic lithium salt, rather than relying solely on thermally driven diffusion, thereby significantly improving the prelithiation and repair efficiency of spent NCM cathodes. Benefiting from the quasi-Grotthuss Li+ topochemistry transport, the degraded structure and Li vacancies in the spent cathode are effectively eliminated, yieding the regenerated cathode with good cycling stability comparable to commercial counterparts. The proposed Li+ transport mechanism presents a promising route for the efficient and sustainable regeneration of spent cathodes.

Recycling spent lithium-ion batteries is essential for alleviating resource shortages and environmental pollution, with cathode material recovery being especially significant due to its high content of valuable elements. Relithiation is crucial for the direct regeneration of spent cathodes, and defective structures (Li vacancies, spinel/rock salt) in layered cathodes can only be completely repaired in an environment with adequate Li. However, cathode materials recycled by relithiation suffer the formation of dense spinel/rock salt structure, induced by the migration of transition metals (TMs) to the Li layer and resulting in the creation of TMO6 octahedron, which hinders Li+ transport between adjacent LiO4 tetrahedra, and further greatly impedes the relithiation of the spent cathodes. Here, we regulated lattice stress at the defect structures to break the lattice symmetry of the unfavorable TMO6 octahedron and consequently form a quasi LiO6 octahedral sites with a low Li+ transport energy barrier. This approach ensures a Li-sufficient environment, facilitating the effective relithiation and structural repair of spent cathodes. The combination of theoretical calculations and experimental approaches proves the advantage of symmetry breaking over the traditional relithiation process in repairing the structure of spent cathodes. The proposed repair strategy paves the way for the exploration of more efficient repair methods for spent cathode materials.

Novel high-energy, binder-free, and solvent-free carbon–silicon layered composite anodes were manufactured using an industrially scalable Virtual Cathode Deposition (VCD) technique. The deposition process transforms commercial graphite target material into carbon polymorph (CALIB) layers, interposed with silicon layers deposited in situ from a silicon source, thereby forming high-capacity anodes for Li ion batteries. Composite CALIB-C/Si4 anodes with a layered architecture exhibited a first-cycle specific capacity of over 1550 mAh g−1 at 0.1 A g−1 and retained a capacity of ~1080 mAh g−1 at a 1 A g−1 rate after 200 cycles. Detailed structural characterisation revealed a disordered carbon matrix encompassing nanosized sp2-bonded carbon clusters (average size ~20 nm), cross-linked by a network of sp3-bonded atomic sites, with predominant mesoporosity and high surface area. The silicon layers were found to consist of an amorphous Si matrix with embedded nanocrystalline components, emulating the growth mode of the CALIB buffer. The presence of the mesoporous carbon matrix accommodated the stress caused by the alloying/de-alloying of silicon nanolayers, thereby alleviating the pulverisation effect and preserving the structural integrity of the composite. The initial performance and capacity decay of the anodes were found to depend on the thickness of the CALIB-C buffer interlayers.

Aqueous organic redox-flow batteries (AORFBs) are promising candidates for the low-cost grid-level energy storage. However, their widescale deployment is limited by crossover of redox-active material through the separator membrane, which causes capacity decay. Traditional membrane permeability measurements do not capture all contributions to crossover in working batteries, including migration and changes to ion size and charge. Here we present a new method for characterising crossover in operating AORFBs, using on-line 1H NMR spectroscopy. By introducing a separate pump to decouple NMR and battery flow rates, this method opens a route to quantitative time-resolved monitoring of redox-flow batteries under real operating conditions. In this proof-of-concept study of a 2,6-dihydroxyantharquinone(2,6-DHAQ)/ferrocyanide model system, we observed a doubling of 2,6-DHAQ crossover during battery charging, which we attribute to migration effects. This new membrane testing methodology will advance our understanding of crossover and accelerate the development of improved redox-flow batteries.

Two-dimensional (2D) XIV-group nanosheets (germanene, silicene, and stannene) possess unique physical and chemical features promising in fields of electronics, energy storage, and conversions. However, preparing these nanosheets is challenging owing to their non van der Waals structure with strong chemical bonds inside. Herein, a bubbling chemical-vapor growth method is proposed to synthesize these XIV-group nanosheets by bubbling XIV-group-element chlorides in molten sodium. During the synthetic process, XIV-group materials are formed by the reaction of XIV-group element chlorides with strong reducing sodium, then nucleated, and finally isolated to 2D nanosheets in the gas-liquid interface. With the collapse of vapor bubbles and subsequent injection, 2D nanosheets are continuously produced. The nanosheets (Ge) possess a thickness of ∼3.8 nm and a lateral size of ∼2.0 μm. Combining with graphene, the hybrid and flexible films are obtained, delivering a volumetric specific capacity of 4785 mAh cm-3 and superior cycling stability (over 4000 cycles) in lithium-ion batteries.

Selenium (Se), as an important quasi-metal element, has attracted much attention in the fields of thin-film solar cells, electrocatalysts and energy storage applications, due to its unique physical and chemical properties. However, the electrochemical behavior of Se in different systems from electrolytic cell to battery are complex and not fully understood. In this article, we focus on the electrochemical processes of Se in aqueous solutions, molten salts and ionic liquid electrolytes, as well as the application of Se-containing materials in energy storage. Initially, the electrochemical behaviors of Se-containing species in different systems are comprehensively summarized to understand the complexity of the kinetic processes and guide the Se electrodeposition. Then, the relationship between the deposition conditions and resulting structure and morphology of electrodeposited Se is discussed, so as to regulate the morphology and composition of the products. Finally, the advanced energy storage applications of Se in thin-film solar cells and secondary batteries are reviewed, and the electrochemical reaction processes of Se are systematically comprehended in monovalent and multivalent metal-ion batteries. Based on understanding the fundamental electrochemistry mechanism, the future development directions of Se-containing materials are considered in view of the in-depth review of reaction kinetics and energy storage applications.

Solid-state batteries (SSBs) have garnered significant attention in the critical field of sustainable energy storage due to their potential benefits in safety, energy density, and cycle life. The large-scale, cost-effective production of SSBs necessitates the development of high-performance solid-state electrolytes. However, the manufacturing of SSBs relies heavily on the advancement of suitable solid-state electrolytes. Composite polymer electrolytes (CPEs), which combine the advantages of ordered microporous materials (OMMs) and polymer electrolytes, meet the requirements for high ionic conductivity/transference number, stability with respect to electrodes, compatibility with established manufacturing processes, and cost-effectiveness, making them particularly well-suited for mass production of SSBs. This review delineates how structural ordering dictates the fundamental physicochemical properties of OMMs, including ion transport, thermal transfer, and mechanical stability. The applications of prominent OMMs are critically examined, such as metal-organic frameworks, covalent organic frameworks, and zeolites, in CPEs, highlighting how structural ordering facilitates the fulfillment of property requirements. Finally, an outlook on the field is provided, exploring how the properties of CPEs can be enhanced through the dimensional design of OMMs, and the importance of uncovering the underlying "feature-function" mechanisms of various CPE types is underscored.

Garnet-type Li7La3Zr2O12 (LLZO) Li-ion solid electrolytes are promising candidates for safe, nextgeneration solid-state batteries. In this study, we synthesize Ga-doped LLZO (Ga-LLZO) electrolytes using a microwave-assisted solvothermal method followed by low-temperature heat treatment. The nanostructured precursor (<50 nm) produced by the microwave-assisted solvothermal process has a high surface energy, facilitating the reaction for preparing garnet-type Ga-LLZO powders (<800 nm) within a short time (<5 h) at a low calcination temperature (<700 degrees C). Additionally, the calcined nanostructured Ga-LLZO powder can be sintered to produce a highdensity pellet with minimized grain boundaries under moderate sintering conditions (temperature: 1150 degrees C, duration: 10 h). The optimal doping concentration was determined to be 0.4 mol% Ga, which resulted significantly increased the ionic conductivity (1.04 x 10(-3) S cm(-1) at 25 degrees C) and stabilized the cycling performance over 1700 h at 0.4 mA cm(-2). This approach demonstrates the potential to synthesize oxide-type solid electrolyte materials with improved properties for solid-state batteries.