Zinc‐based flow batteries (ZFBs) have demonstrated significant potential for large‐scale energy storage owing to their low cost, high safety, and environmental friendliness. However, there still exist two major challenges about ZFBs: (i) the limited energy density resulting from the low solubility of active ions and (ii) dendrite growth, hydrogen evolution reaction (HER), corrosion, and passivation of the zinc metal anode during long‐term cycling, which severely constrain the battery's cycle life and areal capacity (typically below 80 mAh cm −2 ). Fundamentally, these challenges are closely tied to the interfacial properties of the zinc electrode. Therefore, interface engineering has become crucial for enhancing the performance of zinc anodes. This review systematically summarizes recent advanced strategies developed to stabilize the zinc anode interface, encompassing electrode modification (e.g., constructing three‐dimensional hosts, introducing zincophilic coatings, and nanomaterial functionalization), electrolyte optimization (e.g., incorporating functional additives to tailor solvation structures, interfacial adsorption, and pH adjusting), and separator modification (e.g., membrane designs for physical blocking, ion flux homogenization, chemical stabilization, and ion‐selective sieving). The aim is to synergistically induce uniform zinc deposition, suppress side reactions, and stabilize interfacial properties. Ultimately, this review delineates future research directions for high‐performance ZFBs, with the aim of promoting the large‐scale practical application.

A multifunctional cationic electrolyte additive-Li+ was incorporated into the Zn‖V-MOF battery, which could enhance the electrolyte's ionic conductivity and accelerate the Zn2+ diffusion rate, facilitate reversible de-intercalation into the V-MOF cathode, and suppress zinc dendrite formation.

Abstract Lithium-ion batteries exhibit complex multi-species, multi-reaction (MSMR) kinetics, making rapid yet physically consistent inference of internal states a major challenge. We propose a physics-informed neural network (PINN) surrogate for an MSMR electrochemical model. The surrogate resolves ten competing reaction pathways across the two electrodes, enabling high-precision parameter inference. A custom 1 Ah NCM622/graphite pouch cell was fabricated, and an MSMR model reproduced its responses to ensure consistency. To accelerate computation, we embedded piecewise-approximate function representations into the PINN. They capture three key internal states: lithiation, interfacial current density, and particle-surface concentration. We then designed stage-aware network architectures that adaptively learn the distinct nonlinear behaviors of each operating condition. Under standard conditions, the PINN achieves an average R 2 above 0.98 while reducing total runtime by 14 % compared with the conventional MSMR solver. The framework offers an accurate and physics-consistent route for battery state estimation with strong engineering potential.

Redox flow batteries (RFBs) are pivotal for large-scale energy storage, with membranes serving as critical components for ion conduction and active species separation. This review systematically explores the mechanisms, rational design strategies, and applications of advanced RFB membranes. First, fundamental mechanisms of ion transport including proton conduction, size/charge sieving, and degradation pathways (acid/oxidation-induced failure) are dissected. Rational design strategies encompass material innovations (e.g., amphoteric ion-exchange membranes, 2D material-based membranes), structural engineering (microphase separation regulation, gradient pore structure design) to optimize selectivity, conductivity, and chemical/mechanical stability. Applications in RFB systems, including vanadium, zinc-based, and multivalent metal flow batteries are discussed, highlighting membrane-performance correlations and practical challenges. Current bottlenecks, such as the selectivity-conductivity trade-off, cost, and scalability, are identified, alongside future directions including biomimetic ion channels, sustainable materials, and integrated system-level optimization. This review aims to guide the development of high-performance, cost-effective membranes for next-generation RFBs toward commercial deployment.

Achieving long-term stable Zn metal anodes with iso-plating/stripping remains a great challenge for practical rechargeable Zn-ion batteries. Herein, we propose a surface engineering strategy utilizing ultrafine Cu4Zn@Zn core-shell powders fabricated via powder metallurgy. The zincophilic Cu4Zn@Zn interlayer functions as a spatially confined reactor, orchestrating uniform Zn deposition at preferential nucleation sites while facilitating rapid Zn2+ transport via selective dissolution of the metallurgical active Zn core, thereby eliminating current localization and achieving highly reversible stripping/plating behavior. Consequently, the modified electrode delivers remarkable performance: a low polarization (15.32 mV at 1 mA cm- 2, 35.30 mV at 10 mA cm- 2), a high Coulombic efficiency (99.81% at 5 mA cm- 2 for 4000 cycles), and a long-term stability over 2370 h under harsh conditions (10 mA cm- 2). When paired with an NH4V4O10 cathode, the full cell maintains 79.83% of its capacity after 1500 cycles at 5 A g-1. This work provides an effective surface-engineering strategy for Zn anodes and opens a new avenue for stabilizing metal electrodes in aqueous battery systems.

Layered Bi2Se3 has been designed as a promising anode material for aqueous batteries due to its large interlayer spacing and high specific capacity. However, Bi2Se3 is a topological insulator, its interior presents an insulating state, which results in a slow reaction dynamics. Moreover, it is found that unmodified Bi2Se3 has a poor structural stability during charging/discharging. Hence, we design conductive polypyrrole coated hollow Bi2Se3 particles (Bi2Se3@PPy) to solve these problems. Various experiments show that the PPy possesses bifunctional features and enhance the electrical conductivity and structural stability of Bi2Se3. The hollow structure of Bi2Se3 exposes abundant active sites and shortens the diffusion paths of Mg2+. As a result, at current density of 0.2 A g-1, Bi2Se3@PPy offers high discharge capacity of 134 mA h g-1 in aqueous magnesium ion battery. More importantly, Bi2Se3@PPy//Mn3O4 full cell presents discharge capacity of 66 mA h g-1 at 0.5 A g-1. Furthermore, Bi2Se3@PPy exhibits good electrochemical performance in ammonium ion battery. This paper provides a feasible strategy to enhance the structural stability and ionic/electronic conductivity of topological insulator.

P2-type layered Na0.7MnO2 is regarded as a promising cathode material for sodium-ion batteries due to its high specific capacity. However, Mn3+-induced Jahn-Teller distortion and Mn2+ dissolution result in the structural instability of Na0.7MnO2, thereby restricting its large-scale application. In this study, a K0.5MnO2@Na0.7MnO2 composite is prepared by a molten salt method and used as a cathode. In particular, partial K+ in K0.5MnO2 substitutes for the Na+ sites in Na0.7MnO2 during the charge-discharge process, which decreases the Mn3+/Mn4+ ratio and provides wide Na+ channels, achieving fast reaction kinetics and long-term cycling stability. The persistent K0.5MnO2 throughout the entire testing process works as a robust K+ supply source and compensates for the K+ loss of K-doped Na0.7MnO2 during cyclic tests. Consequently, the cathode shows a high discharge capacity of 148 mA h g−1 at 0.04 A g−1 and outstanding cycling stability, with a capacity retention of 69% after 800 cycles at 0.5 A g−1. This research provides important references for designing high-performance layered cathode materials in sodium-ion batteries.

Quasi-solid-state composite electrolytes (QSSEs) represent a promising approach to fabricating high-energy rechargeable batteries, but their practical implementation is hindered by structural instability and interfacial incompatibility. In this study, a QSSE was prepared with the aid of a molecular reinforcer, thioctic acid, which induces a polymer conformational change to a high-dielectric phase for improved ion transport and strengthens the structural durability, even with rich porosity, due to the strong and dynamic complexing bonds. As a result, the ionic conductivity and electrochemical stability of the QSSE are significantly enhanced to 5.0 × 10- 4 S cm-1 and 5.1 V. Moreover, the greatly reduced activation energy (0.11 eV) and the electrolyte-derived inorganic-rich interphases facilitate ion migration across the electrolyte-electrode interfaces and enable simultaneous stabilization of both cathode and anode with thin and stable protection layers. Accordingly, Na|Na3V2(PO4)3F3 cells assembled with the designed QSSE exhibit excellent rate capability and cycling stability at a high cut-off voltage of 4.4 V (vs. Na+/Na), delivering a capacity of 94.1 mA h g- 1 with 93.4% retention after 600 cycles at 1 C. This work offers a viable strategy for developing high-energy-density batteries.

As a chlorinated cationic surfactant, benzyltrimethylammonium chloride (BTMAC) is capable of reducing electrolyte viscosity, improving ionic conductivity, and selectively binding to VO(OH)3 monomers within the electrolyte matrix. This inhibits the dimerization of VO(OH)3 and the subsequent formation of V2O5 precipitation, significantly improving the high-temperature stability of the electrolyte. For a 1.7 M V(IV) electrolyte, visible precipitation begins after just 3 h at 50 degrees C and 2.5 h at 60 degrees C in the absence of BTMAC. The addition of 400 ppm of BTMAC extends this stabilization period to 5.5 h at 50 degrees C and 3 h at 60 degrees C. After 9 h at 60 degrees C, the precipitation rate decreases from 33.27% to 25.99%, and it effectively slows down the capacity decay rate of the battery at 45 degrees C. This finding offers an effective approach for developing low-cost and high-performance vanadium electrolytes.

The rational design of solid-state electrolytes (SSEs) with high ionic conductivity, interfacial robustness, and thermal stability remains a critical challenge for lithium metal batteries (LMBs). Herein, we established the crystal-transformed hydrogen-bonded organic framework/trinuclear Cu cluster organic framework heterostructures (HOFa/TrCuMOF8) as thermally stable SSEs for LMBs. The crystal-transformed HOF/MOF heterostructure constructs continuous low-energy Li+ transport pathways, while the pendant -CH3 with strong steric hindrance induces anion adsorption to effectively suppress TFSI- migration. Meanwhile, coordination-confined TrCu synergizes with imine (C = N) groups to create a dynamically polarized local electronic environment through Li+-induced charge redistribution, thereby promoting selective Li+ transport. Consequently, the HOFa/TrCuMOF8 SSEs deliver a high Li+ transference number (0.94) and ionic conductivity (2.7 mS cm-1 at 30°C). Compared with polypropylene (PP) separators, the flexible HOFa/TrCuMOF8 SSEs maintain structural integrity at high temperatures (180°C), effectively suppressing electrolyte shrinkage and thermal short-circuit propagation. The assembled Li|HOFa/TrCuMOF8 SSEs|LiFePO4 LMBs achieve 97.8% capacity retention after 1000 cycles at 2 C and maintain stable cycling even at 100°C. Remarkably, the Li|HOFa/TrCuMOF8 SSEs|NCM811 pouch cell exhibits an impressive energy density of 259.4 Wh kg-1 with enhanced thermal safety. This work provides a crystal-transformation strategy for engineering HOF/MOF heterostructures toward thermally stable solid-state lithium batteries.

In virtue of the wide electrochemical window and superior flame-retarded ability, phosphate electrolytes are widely employed as transport media in high-voltage lithium metal batteries. Unfortunately, the strong interaction of Li+-phosphates leads to inefficient Li+ transport. Furthermore, the uncontrollable electrode-electrolyte interphase originated from the labile interfacial species retards the stable cycling of lithium metal batteries during operation. Herein, in-built high dielectric dissociated reservoir and functional interfacial regulation additive were designed to boost the dissociation ability of Li+ and stabilize the bidirectional electrode-electrolyte interfaces. Benefitting from the strong desolvated kinetic of nanowires and excellent interfacial regulation function of lithium nitrate, the continuous Li+ transport pathway and homogeneous bidirectional electrode-electrolyte interfaces were constructed, preventing the lithium metal anode and high-nickel cathode from persistent reactive with phosphate electrolytes, revealed by theoretical calculation and ex-situ characterization. Attributed to the guided ion transfer pathway and oriented artificial solid electrolyte interface, the Li||Li symmetrical batteries exhibit excellent cycling stability of above 1000 h at 2 mA cm-2 and 2 mAh cm-2. The Li|| LiNi0.8Co0.1Mn0.1O2 (NCM811) battery shows more than 90 % capacity retention after 200 cycles at 1C. This strategy holds great promising for developing advanced electrolytes in other advanced electrochemical storage devices.

Vanadium redox flow batteries (VRFBs) have attracted much attention in the field of large-scale energy storage due to the advantages of large energy storage capacity, stable performance, high safety and long cycle life. However, traditional graphite felt (GF) electrodes suffer from poor hydrophilicity and insufficient electrocatalytic activity, which limit the energy efficiency and rate performance of VRFBs. Here, the SnO2 nanoparticles derived from disodium stannous citrate (DSSC) is applied to modify the GF (SnO2@GF). Owing to the Sn-O-C bonds between SnO2 particles and carbon lattice, it not only enhances the specific surface area to facilitate interfacial ion transport, but also improves electrocatalytic activity for vanadium ions redox reactions. As a result, at the optimal DSSC concentration of 300 g/L, SnO2@GF-based VRFBs demonstrate a significant reduction of the overpotential by 110 mV and an increase in the energy efficiency by 15 % at 200 mA cm-2 compared with pristine GF.

The vanadium redox flow battery (VRFB) is a promising technology for large-scale energy storage, but the sluggish kinetics and poor catalytic activity of carbon felt electrodes limit high-current-density operation. Herein, a simple sulfuric acid impregnation and segmented thermal treatment strategy is developed to achieve synergistic mild etching and sulfur doping. The 300 degrees C stage induces surface etching and defect formation, while the subsequent 600 degrees C treatment promotes C-S bond formation. The optimized electrode exhibits improved redox reversibility, reduced charge transfer resistance, and an increase in the diffusion coefficient for the vanadium ion reduction process. In full-cell tests, it delivers an energy efficiency of 78.6 % at 300 mA cm-2, 8.1 % higher than pristine carbon felt, and remains stable over 800 cycles. This work provides a facile route for constructing highperformance sulfur-doped carbon felt electrodes for VRFBs.

The rich valence states (-2 to +6) make elemental Te become a high-capacity electrode in aqueous batteries. The conversion process (Te to TeO2) generates soluble Te4+ species in aqueous electrolyte. The suppression of conversion process enables a long-term Te electrode at the cost of a partial storage capacity. Herein, a polyethylene glycol additive is introduced to regulate the electrolyte environment. The low H2O activity hinders Te4+ species formation and therefore leads to the insertion-type Te electrode. The reshaped NH4+ solvation structure facilitates the fast H2O removal and firm PEG adsorption on the electrode surface, also improving water-induced side reactions. This, coupled with the introduction of carbon host, contributes to a high-stability Te electrode. Theoretical and experiment studies reveal the reshaped NH4+ solvation structure/hydrogen-bond network, the strong adsorption capability of B-doped carbon, and the inhibited Te dissolution. Additionally, a series of in/exsitu characterizations prove the intercalation-type mechanism and the enhanced cycling stability. As a result, this elaborate electrode delivers a high reversible capacities of 376 mA h g- 1 at 0.05 A g- 1 and a long-term cycling stability with 73.8 % capacity retention at 5 A g- 1 after 4500 cycles. This work provides a reference for the storage mechanism regulation in aqueous battery.

Hybrid supercapacitor (HSC) delivers high power and energy densities for energy storage applications, but its pronounced temperature dependence and fluctuating capacity fade severely impede accurate state of health (SOH) estimation. Current algorithms focus solely on SOH and do not provide mechanistic understanding of degradation, which limits the effectiveness of hybrid supercapacitor health management. This study proposes a P2D-convolutional neural network (CNN) framework for online SOH monitoring and degradation mechanism analysis of HSC. A P2D model modified with the double-layer equation was employed to generate datasets via Latin hypercube sampling. This model was then coupled with a CNN to extract degradation-related features from incremental capacity curves through physics-data fusion, enabling reliable SOH prediction and quantitative assessment of electrochemical parameter degradation. Experimental results demonstrate that the proposed framework accurately captures the degradation mechanisms of HSC under fluctuating conditions, with the SOH prediction achieving an R2 of 0.9387 and a mean absolute percentage error (MAPE) of 1.57% across 13,898 cycles. These findings provide useful guidance for the design and health monitoring of HSC.

Due to uncontrollable interfacial reactions in aqueous electrolytes, zinc metal anodes typically suffer from severe dendrite growth and side reactions, significantly hindering the practical application of aqueous zinc metal batteries. Herein, a nitrogen-rich interphase is in situ constructed on the surface of the zinc anode by incorporating tetraethylenepentamine (TEPA) into the electrolyte. The nitrogen-rich interphase regulates interfacial charge via electrostatic shielding effect, enabling Zn2+ to be guided by uniform electric fields during deposition. Meanwhile, the nitrogen-rich groups coordinate with or electrostatically adsorb Zn2+, driving preferential deposition on the low-surface-energy (002) plane rather than high-energy crystal planes (e.g., (100), (101)) and thereby suppressing the occurrence of disordered dendrites and side reactions. As a result, the Zn symmetric batteries with the nitrogen-rich interphase exhibit excellent stability for over 340 h under a depth of discharge of 65.3%, and still achieve stable cycling for over 450 h at an ultrahigh current density of 63.0 mA cm-2. Furthermore, the assembled Zn||NH4V4O10 full batteries can retain 91.2% of initial capacity after 1000 cycles at 5 A g-1. Such a finding provides valuable guidance for rationally designing interphases to address interfacial issues in long-life zinc metal batteries.

Dendrites and water-induced side reactions impose greatly challenge on the implementation of aqueous zinc ion batteries. To tackle these problems, an artificial rectified layer (ARL) with hydrophobic, zincophilic and insulating features was in situ synthesized on Zn surface rapidly to prevent the electron leakage from Zn anode to aqueous electrolyte, which is the underlying logic for uneven Zn deposition and parasitic side reactions. The ARL also displays a high Zn 2+ transference number of 0.71 and can build fast Zn 2+ transport channels to homogenize the interfacial ion flux and electric field according to the calculated work function and multi-physics phase simulation results. Therefore, the Zn anode with ARL shows preferred plating along with (002) crystal facet and an admirable Coulombic efficiency of 99.86 % over 3200 cycles. Zn symmetric cells can withstand large current density up to 40 mA cm −2 and operate stably at 44.2 % depth of discharge for 250 hours, surpassing most of published reports. The ARL also enables the Zn||MnO 2 full batteries to circulate over 2600 cycles with a high-capacity retention of 80.1 % and low self-discharge at 1 A g −1 . This work provides a different perspective to comprehend and design satisfactory solid electrolyte interphase for Zn metal anodes.

Aqueous zinc-iodine batteries are considered as promising energy storage device, but the severe shuttle effect of polyiodide species limits their cycling life. The conventional physical adsorption has a limited effect in preventing polyiodide shuttling. Herein, a dual strategy of physical adsorption and chemical confinement is performed through nitrogen/boron dual-doped carbon nanofiber-encapsulated bismuth nanoparticles. In situ characterizations and theoretical calculations confirm that the nitrogen and boron co-doping endows carbon nanofibers with strong physical adsorption for iodine species, hindering polyiodide shuttling. A robust chemical confinement is realized by Bi/BiOI conversion, proved by ex situ tests and suppressing the formation of polyiodide. Moreover, Bi nanoparticles are restricted to carbon nanofibers, the charge transfer and structural stability of electrode are improved with the help of 3D conductive network. Therefore, the elaborate dual-mechanism aqueous batteries deliver a high reversible capacity of 275 mA h g-1 at 0.5 A g-1, an excellent rate performance with 207 mA h g-1 at 10 A g-1, and a long-term cycle life over 2000 cycles. Remarkably, high mass loading electrode (10 mg cm-2) and flexible pouch cell still display satisfactory performances. This work provides a new idea to design host with strong physicochemical confinement for iodine species.