The development of materials that simultaneously offer broadband electromagnetic protection, optical transparency, mechanical flexibility, and intelligent responsiveness remains a formidable challenge in the advancement of next-generation smart windows. In this study, a synergistic design strategy that integrates multi-component molecular engineering with in-situ microphase separation was introduced, leading to the successful fabrication of a novel multifunctional ionogel. This approach enables the spatial decoupling of the mechanical framework from ion transport and polarization domains within a nanoscale bicontinuous structure, effectively addressing the trade-off between mechanical strength and ionic conductivity. The optimized ionogel demonstrates an ultra-wide effective absorption bandwidth of 8.08 GHz at a remarkably thin thickness of 1.72 mm, along with high visible-light transmittance exceeding 93% and excellent mechanical properties, including a fracture strain of 406%. Furthermore, by incorporating photochromic molecules, the material exhibits light-gated microwave absorption characteristics with reversible bandwidth tuning and achieves passive radiative cooling exceeding 22.83 degrees C under simulated sunlight. Differential charge density calculations further confirm electron accumulation at the hard/soft phase interfaces, providing atomic-scale evidence for interfacial polarization. This work establishes a new paradigm of microstructure-driven molecular design, opening a new avenue for the development of next-generation electromagnetic protection and thermal management systems.

Zinc anodes offer several compelling advantages, including elevated theoretical capacity, favorable redox potential, and plentiful natural reserves, which have made aqueous zinc-ion hybrid capacitors a focal point of intensive research. However, uncontrolled dendrite growth and the hydrogen evolution reaction remain critical issues limiting their stability and reliability. In this study, an indium-based In-BDC MOF was constructed as a protective layer on the surface of zinc foil. Benefiting from the zincophilic nature of In3+, the abundant porous channels in the MOF structure, and the physical shielding effect of the artificial protective coating, this interfacial layer exhibited excellent cycling stability. The In-BDC@Zn symmetric cell exhibited exceptional cycling durability, operating steadily for 1200 h under conditions of 2 mA cm-2 and 1 mA h cm-2, while retaining stability beyond 1000 h at an elevated current density of 20 mA cm-2. When paired with activated carbon in a full zinc-ion hybrid capacitor, the device retained 40.8 mA h g-1 after 15 000 cycles at 1 A g-1, corresponding to 93.93% capacity retention.

Against the backdrop of advances in intelligent sensing, information protection, and electronic device integration, the performance bottleneck of electromagnetic wave (EMW) absorption has gradually shifted from the intrinsic properties to the limitations of structural control strategies. Multiscale engineering, as a key approach to overcoming this bottleneck, integrates atomic/molecular, nanoscale, microscale, and macroscale levels, thereby endowing EMW absorption materials with enhanced controllability, efficiency, and intelligent tunability. Nevertheless, current multiscale studies still face significant challenges, including the unclear mechanisms of structural synergy and the reliance on empiricism in structural design. This review provides a systematic overview of the multiscale structural design and first elucidates the influence of structures ranging from atomic to macroscopic scales on the electromagnetic responses. Subsequently, the progress on EMW absorption materials in three typical synergistic strategies at atomic/molecular, nanometer, micrometer, and macroscopic scales was summarized, revealing the regulatory effect of structural evolution on EMW absorption performance. This review particularly emphasized the cross-scale structure-function coupling mechanism, such as dipole polarization, interface loss, multiple scattering, and impedance matching. Finally, the main challenges currently facing multiscale structural engineering in the field of EMW absorption are summarized, and future development directions are outlined from the perspective of material design and performance optimization.

MXene-based proton pseudocapacitors are promising candidates for microscale electronic devices due to their superior portability and high-power density, yet their advancement is constrained by the scarcity of efficient electrode materials. Herein, a nitrogen-directed Ti3C2Tx MXene with substitution of terminal functional groups by nitrogen is proposed as a high-efficiency electrode material for proton pseudocapacitors. This strategy introduces multiple surface-active sites and a new pathway for fast proton storage for achieving high specific capacitance. Impressively, a nitrogen-directed proton storage mechanism is unraveled in the terminal N groups can preferentially interact with protons and lower the diffusion energy barrier toward adjacent active-sites, substantially facilitating the storage of protons. As a result, the N300-Ti3C2Tx delivers excellent capacitance retention of 84.48% after 30,000 cycles at 2 A g-1. Furthermore, in-plane proton pseudocapacitors are fabricated via direct ink writing, which shows great compatibility with various connection configurations, validating the superior potential in application feasibility of the N-directed Ti3C2Tx on proton storage.

Ni-rich layered oxides stand as pivotal cathode candidates for high-energy lithium-ion batteries, yet their elevated nickel content (Ni ≥ 0.9) exacerbates structural instability through interfacial degradation and lattice stress accumulation during cycling, leading to accelerated capacity decay. Here, we propose a dual-gradient architecture for Ni-rich cathodes that synergistically integrates germanium concentration gradients with controlled phase evolution. By engineering radial Ge doping gradients within spherical particles, we achieve coherent phase progression from disordered rock-salt through spinel to layered configurations. This structural design not only markedly enhances Li+ diffusion kinetics but also efficaciously suppresses interfacial parasitic reactions by modulating the oxidation state of Ni. Moreover, the coherent transition from disordered to ordered structures minimizes the crystallographic mismatch, stabilizes the internal layered framework, and alleviates anisotropic stress accumulation, ultimately achieving extraordinary cycling stability. Under high-rate conditions (4.3 V, 10 C), the material exhibits a discharge capacity of 171.4 mAh g-1, with a capacity retention of 97.0% after 200 cycles at 1 C. This dual-gradient strategy offers a promising approach to developing advanced cathode materials that meet the demanding requirements of high-rate and long-life lithium-ion batteries.

Phase transitions in sodium layered transition metal (TM) oxides often induce microstrain and TM ion migration, leading to structural degradation and poor cycling stability. However, a rational design approach for optimizing phase transitions is still lacking. Here we introduce phase transition potential (Φphase) as a rational descriptor to predict and control phase evolution in these cathodes. A lower Φphase enables smoother Na+ migration and slower slab sliding during Na extraction, thereby facilitating a continuous phase transformation rather than abrupt phase changes. Guided by this concept, we design a calcium-substituted layered oxide, Na0.96Ca0.02Ni0.33Fe0.33Mn0.33O2 (NCNFMO), which delivers a specific capacity of 140 mAh g-1 at 0.1 C and retains 84.2% of its initial capacity after 500 cycles at 1 C, compared to only 26.4% retention for NaNi0.33Fe0.33Mn0.33O2. Moreover, the NCNFMO||Al@C full cell maintains a high-capacity retention of 82.5% after 100 cycles, and 6.1 Ah full cell demonstrates an energy density of 192 Wh kg-1 entire cell. These findings offer fundamental insights into phase behavior-induced microstrain and a promising path toward high-energy, long-life sodium-ion batteries.

With the rapid development of the low-altitude economy (e.g., drones, eVTOL aircraft), high-performance lithium-ion batteries have become a core enabling technology. Ni-rich single crystal LiNixCoyMnzO2 (NCM) cathodes are promising due to their high specific capacity and structural stability, but suffer from "storage failure" during long-term storage. This study systematically investigates the restoration of storage-failed NCM single crystal cathodes with Ni contents of 60%, 88%, and 94% using water washing and heat treatment at different temperatures (300-800°C) under different atmospheres (O2, air, Ar). Water washing efficiently removes surface residual lithium compounds (RLCs) but causes lithium loss and increased Li/Ni mixing, failing to restore rate capability. The heat treatment atmosphere plays a decisive role: oxygen effectively replenishes lattice oxygen and reduces Li/Ni mixing. The optimal method-heat treatment at 800°C under O2 atmosphere-recovers >99% of the original rate capability and nearly full cycling performance, with broad applicability across different Ni contents. Structural analysis reveals that storage failure is primarily caused by rock-salt NiO formation due to lattice Li/O loss, rather than surface RLCs. High-temperature O2 treatment decomposes surface RLCs, replenishes Li+ and lattice oxygen, and transforms the cubic rock-salt phase back to the hexagonal layered structure. This study provides a scientific basis for understanding the storage failure mechanism and thermal restoration strategy of Ni-rich single crystal NCM cathodes.

MXene‐based proton pseudocapacitors are promising candidates for microscale electronic devices due to their superior portability and high‐power density, yet their advancement is constrained by the scarcity of efficient electrode materials. Herein, a nitrogen‐directed Ti 3 C 2 T x MXene with substitution of terminal functional groups by nitrogen is proposed as a high‐efficiency electrode material for proton pseudocapacitors. This strategy introduces multiple surface‐active sites and a new pathway for fast proton storage for achieving high specific capacitance. Impressively, a nitrogen‐directed proton storage mechanism is unraveled in the terminal N groups can preferentially interact with protons and lower the diffusion energy barrier toward adjacent active‐sites, substantially facilitating the storage of protons. As a result, the N300‐Ti 3 C 2 T x delivers excellent capacitance retention of 84.48% after 30,000 cycles at 2 A g −1 . Furthermore, in‐plane proton pseudocapacitors are fabricated via direct ink writing, which shows great compatibility with various connection configurations, validating the superior potential in application feasibility of the N‐directed Ti 3 C 2 T x on proton storage.

Fundamental limitations in structural reversibility and electrochemical performance have rendered anode materials a critical bottleneck for proton batteries and capacitors. While the rational design of intrinsic properties for metal oxides offers a promising route for advanced proton storage, the simultaneous realization of high-power and low-temperature operability remains a grand challenge. We show that topochemical preintercalation of protons and confined lattice water in hydrated molybdenum bronze modifies host lattice rearrangement and enables ultrafast proton-coupled electron transfer. Ion-fluid cointercalation mediates electrochemical reaction pathways to an unconventional three-proton insertion mechanism, enabling a state-of-the-art specific capacity of 407 mAh g-1, ultrahigh-rate capability exceeding 1000 C (500 A g-1), and ultralow-temperature adaptability (194.2 mAh g-1 at -80 °C). Comprehensive in situ crystal and interface evolution methods and theoretical calculations reveal a highly reversible and homogeneous protonation mechanism and enhanced interfacial transport, suppressing heterogeneous and unstable reaction kinetics of pristine MoO3. The hybrid proton capacitor with such a molybdenum bronze anode shows an unprecedented ultrahigh-power and ultralow-temperature performance, with excellent stability for over 2000 cycles at -80 °C. This work highlights physicochemical insights on preintercalation topochemistry in modulating charge carrier-host interactions and provides electrode design principles for high-rate and low-temperature nonmetallic ion storage.

Heteroatom doping is an effective defect-engineering strategy to improve the electrochemical activity of carbon materials. However, the influence of specific heteroatom configurations on Na-storage behavior remains inadequately understood. Herein, N/P co-doped soft carbon is prepared from low-cost needle coke through a facile aqueous mixing and high-temperature pyrolysis approach. The obtained carbon exhibits enlarged interlayer spacing, abundant structural defects, and optimized surface heteroatom configurations including N-5, N-6, P-C, and P-O. Among all samples, 800-0.2-NPC delivers the best performance, with a reversible capacity of 365 mAh g-1 in the second cycle and an ICE of 63.2% at 0.02 A g-1. It also maintains 102.8 mAh g-1 at 5.0 A g-1 and retains 118.7 mAh g-1 after 1000 cycles. Combined DFT, XPS, and electrochemical analyses confirm that favorable configurations provide reversible Na-storage sites, enhancing sloping capacity and ICE. Kinetic analysis reveals that N/P co-doping increases the surface-capacitive contribution, explaining the superior rate capability. Pyrolysis temperature critically regulates configurations, defects, and graphitization, thereby determining Na-storage performance. This work highlights the importance of heteroatom-configuration engineering for high-performance soft carbon anodes in sodium-ion batteries.

Aqueous zinc-ion capacitors have garnered tremendous attention owing to their prominent merits of high safety, superior energy density, and environmental benignity. Nevertheless, the adoption of aqueous electrolytes triggers a series of side reactions during operation, which significantly compromises the cyclic stability. To tackle this critical issue, this paper employs a facile soaking strategy, where zinc foil is immersed into a pre-prepared perfluorobutanesulfonyl fluoride (PBSF) solution. Leveraging the reaction between reactive PBSF and reducible metallic zinc, an organic protective layer dominated by zinc perfluorobutanesulfonate is in-situ constructed on the zinc surface. This layer not only reduces direct Zn-electrolyte contact to suppress dendrite formation, but also blocks SO42- ingress and accelerates Zn2+ migration, homogenizing the electric and Zn2+ concentration fields on the Zn surface for corrosion-resistant Zn plating/stripping with effective dendrite inhibition. The assembled PBSF@Zn & Vert;PBSF@Zn symmetric cell achieves stable cycling over 3500 h at 2 mA cm- 2 and 1 mAh cm- 2. The zinc-ion capacitor retains nearly 100% capacity after 10,000 cycles at 10 A g- 1, with a maximum energy density of 47.2 Wh kg- 1 and peak power density of 800 W kg- 1. Additionally, density functional theory (DFT) calculations confirm strong PBSF-Zn adsorption enables uniform Zn deposition, providing solid theoretical support for ultra-long cycle life.

The commercial viability of aqueous zinc-ion capacitors (AZICs) is currently constrained by the intrinsic instability of zinc anodes, manifested as erratic dendrite proliferation and deleterious parasitic reactions. To circumvent these impediments, we engineered a dense, manganese oxide-based artificial interphase in-situ on Zn foil utilizing a facile permanganate oxidation protocol. Distinct from conventional ex-situ coatings, this robust architecture functions as a dual-mechanism shield: it physically segregates the electrolyte to arrest corrosion while simultaneously homogenizing the interfacial ionic flux to eradicate the "tip effect." Mechanistic investigations reveal that this protective layer significantly ameliorates desolvation kinetics and elevates the Zn2+ transference number. Consequently, the modified anode sustains stable cycling for over 1500 h at 10 mA cm-2. Moreover, the assembled Zn@KMnO4//activated carbon capacitors exhibit exceptional durability, maintaining near 100% capacity over 65,000 cycles at 10 A g-1. This study delineates a scalable and effective trajectory for stabilizing zinc anodes in next-generation energy storage systems.

The rapid expansion of the low-altitude economy-particularly the development of unmanned aerial vehicles (UAVs) and electric aircraft-has intensified the trade-off between flight endurance and payload capacity. Carbon fiber structural supercapacitors (CF-SSCs) offer a promising solution by integrating energy storage into load-bearing components; however, the inherent chemical inertness of carbon fibers restricts device capacitance, and their low-temperature electrochemical behavior remains largely unexplored. Here, we construct an H2V3O8@PPy composite electrode via in situ low-temperature oxidative polymerization. The uniform PPy coating facilitates rapid interfacial kinetics, provides reversible pseudocapacitance, and buffers the volume expansion of the H2V3O8 nanorods. The assembled H2V3O8@PPy@CF-SSC achieves a high specific capacitance of 1082.4 mF g-1 and an energy density of 573.6 mWh kg-1. Crucially, the device maintains 42.1% capacitance retention at -10 degrees C, delivering an energy density of 165 mWh kg-1 surpasses the performance of most previously reported CF-SSCs. Furthermore, the device demonstrates robust mechanical properties, featuring a tensile strength of 126.5 MPa and a tensile modulus of 6.92 GPa. This work fills the gap in low-temperature CF-SSC research and provides guidance for the design of high-energy-density structural energy-storage devices for extreme environments.

High-nickel single-crystal NCM cathodes are essential for high-energy-density power batteries in the electric vehicles (EVs), but they suffer from severe surface residual lithium compounds (RLCs) that degrade electrochemical performance. Conventional modification methods can only remove RLCs once and fail to prevent their re-formation upon air exposure. Here, we report a WO3 treatment strategy that simultaneously eliminates surface LCs and constructs an in situ Li2WO4 protective layer on single-crystal NCM613 and NCM8866 cathodes. An optimal WO3 addition of 0.5 wt % achieves the best balance between RLCs removal and electrochemical performance restoration. The Li2WO4 layer acts as a fast-ion conductor to facilitate Li+ transport and as a chemically stable barrier to block moisture and CO2, thereby suppressing RLCs regeneration during air storage. After 6 days of humid air exposure, the total RLCs content of the WO3-treated 8-NCM increases by only 18%, compared with 57.6% for the pristine material. The optimized 8-NCM@0.5W delivers an initial discharge capacity of 207 mAh g-1 (vs 137 mAh g-1 for pristine) with significantly improved cycling stability and rate capability. Galvanostatic intermittent titration technique (GITT) confirms enhanced Li+ diffusion kinetics. Moreover, the Li2WO4 layer passivates the cathode surface, mitigating electrolyte side reactions and microcrack formation during long-term cycling. This work provides a simple, scalable, and effective surface modification approach to overcome the critical bottleneck of RLCs re-formation, which is particularly relevant for long-life, high-safety power batteries in EVs applications.

The development of lithium-ion batteries (LIBs) that integrate high-voltage stability with ultra-low-temperature operational capability remains a critical bottleneck for industrializing next-generation energy storage technologies. Conventional electrolytes cannot simultaneously ensure interfacial stability at high-voltage and efficient ion transport at ultra-low-temperatures due to inherent limitations in their molecular structures. In this study, tetrahydropyran (THP) is employed as the main solvent, capitalizing on its low viscosity and weak solvation ability to optimize low-temperature ion transport kinetics. Meanwhile, fluoroethylene carbonate (FEC) and LiTFSI are introduced as functional additives, which undergo selective redox reactions on the surfaces of the cathode and anode. This enables the directional construction of compositionally uniform and structurally dense CEI and SEI, thereby synergistically suppressing interfacial degradation of high-voltage cathodes and solvent co-intercalation into graphite anodes. Based on this strategy, the formulated THP-FEC (5%) electrolyte allows an NCM811||Gr full-cell to retain 80% of its capacity after 300 cycles at 4.5 V while also delivering 90 mAh & centerdot;g-1 at -50 degrees C. Furthermore, a 1 Ah pouch cell using this electrolyte maintains 0.96 Ah after 170 cycles at 25 degrees C and provides 0.6 Ah when transferred to -20 degrees C after cycling. This work presents a universal strategy for designing high-voltage and ultra-low-temperature LIB electrolytes through precise component modulation.

Manganese exhibits remarkable chemical versatility,arising from its multiple valence states and diverse coordination environments.This unique redox flexibility underpins a rich spectrum of electrochemical processes,making man-ganese-based compounds central to the development of advanced energy storage systems.However,it also gives rise to intrinsic instability,involving disproportiona-tion reactions,dissolution of Mn species,and irreversible structural evolution.An in-depth understanding of these coupled chemical-structural dynamics is essential to unlocking the full potential not only of Mn-based electrodes but,more importantly,of aqueous Mn-ion batteries(AMIBs).In this review,we critically summarize the recent progress of AMIBs,with an emphasis on the development and engineering strategies of electrodes and electrolytes.Finally,we propose future perspectives for constructing robust,energetic,and sustainable AMIBs.

Electrochemical energy storage technology has emerged as a crucial research focus in the development of advanced energy storage systems, owing to its high energy conversion efficiency, flexible modular design, and environmental benignity. In recent years, the growing demand for large-scale energy storage in renewable energy integration and smart grids has further accelerated research in this field. Compared with conventional lithium-ion batteries, which are constrained by high production costs, limited lithium resources, and potential safety risks associated with flammable organic electrolytes, aqueous zinc-ion capacitors (ZICs) have attracted considerable attention as promising alternatives for large-scale energy storage applications. This advantage mainly stems from the intrinsic merits of zinc metal anodes, including high theoretical capacity, low redox potential, natural abundance, low cost, and excellent safety when operated in aqueous electrolytes. Despite these advantages, the practical application of zinc ion batteries (ZIBs) is still severely restricted by the intrinsic challenges associated with zinc metal anodes. During repeated zinc plating/stripping processes, non-uniform Zn deposition tends to occur, leading to the formation of zinc dendrites. Meanwhile, unavoidable side reactions such as hydrogen evolution, corrosion, and by-product formation further deteriorate the anode surface and electrolyte environment. These issues collectively result in rapid capacity decay, poor cycling stability, and low Coulombic efficiency, ultimately impacting the long-term reliability and commercial viability of aqueous zinc-ion batteries. In order to solve the above problems, this study proposed a zinc electrode (APS@Zn) strategy to construct a compact three-dimensional ZnO layer by ammonium persulfate (APS) treatment. The method is simple and controllable, and the dense ZnO layer formed can not only effectively regulate the nucleation behavior of Zn2+, inhibit dendrite growth and side reactions, but also significantly improve ion transport kinetics and cycle reversibility, and realize uniform electroplating and stripping of zinc. Therefore, APS@Zn electrode shows better electrochemical performance than bare zinc electrode. The assembled symmetrical battery can be stably cycled for 4500 h under the conditions of 5 mA center dot cm(-2 )and 1 mAh center dot cm(-2), and can still run stably for 1800 h even under the high current density of 20 mA center dot cm(-2) and 0.5 mAh center dot cm(-2). The zinc ion capacitor paired with active carbon anode can be stably cycled for more than 40000 cycles under the condition of 2 A center dot g(-1). It can be seen that the three-dimensional porous compact ZnO layer formed by APS treatment not only effectively improves the stability and reversibility of the electrode, but also makes the battery show higher and more stable specific capacity.

Aqueous ammonium-ion (NH4 +) batteries/capacitors, recognized for inherent high safety and fast diffusion kinetics, are a promising alternative for sustainable energy storage. However, the development of ammonium-ion energy storage devices has been hindered by the poor compatibility between the distinctive solvation structure of NH4 + ions and conventional organic electrode materials, especially under low-temperature conditions. Here, a redox-active conjugated polymer with self-selective coordination mechanism is designed for achieving high-rate and low-temperature performance. The electron delocalization induced by the conjugated backbone facilitates rapid electronic transport in electrodes, delivering an ultrahigh-rate capacity of 107 mAh g-1 at 20 A g-1 under 25 °C and stable cycling performance with 99% capacity retention under -50 °C. Theoretical calculations and experimental investigations reveal that the inherent structural self-selectivity renders symmetrically arranged carbonyl groups as active binding sites for NH4 + storage, leading to a reversible 4-electron coordination process. Hence, the assembled all-organic hybrid ammonium-ion capacitor enables a long cycle life for over 3,000 cycles at -50 °C, which surpasses the lowest operating temperature reported for ammonium-ion devices, thus propelling the advancement of ammonium-ion energy storage technologies at low temperatures.

Ni-rich oxides have emerged as leading cathode candidates for lithium-ion batteries because of high specific energy, lower cost, and improved sustainability compared to cobalt-based materials. However, Ni-rich cathodes suffer from voltage and capacity degradation driven by anisotropic lattice strain and interfacial reconstruction. Here, we report a high-performance Ni-rich cathode featuring a robust outside-in architecture, achieved via machine learning-assisted identification of Al3+ and Sn4+ dopants. Through a competitive doping mechanism, these dopants form a Sn-rich rock-salt surface layer and a uniformly Al-doped bulk. This high-quality outside-in structure enhances interfacial stability and structural reversibility by mitigating cathode/electrolyte interfacial degradation and alleviating anisotropic lattice strain associated with H2/H3 phase coexistence. Moreover, nonmagnetic Al3+ and Sn4+ weaken superexchange interactions and suppress Li─Ni disorder. As a result, the cathode retains 96.9% of its capacity after 200 cycles with minimal voltage fade. These findings provide insights into the development of high-performance Ni-rich cathodes.