The high-voltage spinel LiNi0.5 Mn1.5 O4 (LNMO) is a promising cobalt-free cathode with high specific energy, attributed to its high operating voltage (approximately 4.7 V). However, its practical durability is limited by irreversible transition-metal migration, spinel-to-rock-salt phase reconstruction, highvoltage interfacial side reactions, and transition-metal dissolution. Herein, we report a multi-elementdoped, cation-disordered spinel LiNi0.4 Mn1.4 Fe0.05 Cr0.05 Cu0.05 Nb0.05 O4 (HELNMO) synthesized via a solidstate method. Rietveld refinement confirms a single-phase Fd 3 m structure with a slightly expanded lattice parameter (8.1857 A & ring; for HELNMO versus 8.1776 A & ring; for LNMO), and energy-dispersive X-ray spectroscopy mapping reveals a homogeneous distribution of the dopant elements. Structural and spectroscopic characterizations consistently confirm enhanced cation disorder in HELNMO, which contributes to favorable electrochemical performance by delivering approximately 130 mAh g-1 at 0.1 C and exhibiting markedly improved cycling stability, retaining 92 % of its initial capacity after 10 0 0 cycles at 2 C between 3.5 and 4.9 V. In-situ X-ray diffraction reveals smoother, more continuous lattice evolution of HELNMO than LNMO during (de)lithiation, consistent with a more homogeneous reaction pathway. Post-cycling analyses corroborate suppressed surface rock-salt reconstruction, reduced impedance growth, and alleviated Mn/Ni dissolution. Collectively, multi-element doping coupled with disorder engineering can effectively mitigate transition-metal migration and high-voltage interfacial degradation, providing a practical strategy for durable, high-energy spinel cathodes. (c) 2026 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.

Aqueous zinc-ion batteries (ZIBs) have emerged as promising candidates for large-scale grid energy storage due to their inherent safety, low cost, and environmental friendliness. Among the various cathode materials, vanadium-based oxides are particularly attractive because of their high theoretical capacity and robust crystal frameworks. However, achieving a combination of high capacity and long-term cycling stability in vanadium-based ZIBs remains a significant challenge. While conventional pre-intercalation approaches can effectively widen the interlayer spacing, they offer only limited improvements in overall energy density. To overcome this limitation, advanced multi-level synergistic strategies are being developed, encompassing optimized cation pre-intercalation, structural water regulation, defect engineering, and hybridization with carbon-based or non-carbon materials. This review begins with the evolution of ZIBs and highlights the inherent advantages of vanadium-based cathodes. Subsequently, it delves into the fundamental charge storage mechanisms of ZIBs. Finally, it presents a comparative analysis of how multi-level design tactics—such as the intercalation of mono-valent (e.g., Na+, K+) and multi-valent (e.g., La3+, Cr3+, Zn2+) metal ions, as well as dual-ion co-intercalation—affect the structure and electrochemical behavior of vanadium oxides. Additional performance-enhancing modification strategies are also discussed. Ultimately, this work aims to establish a theoretical foundation and provide practical design principles for the development of high-performance cathode materials for next-generation ZIBs.

Commercial LiCoO2 (LCO) cathodes are hindered by interfacial side reactions and structural degradation at high voltages, limiting their energy density and raising safety concerns. To address this, we develop a surface engineering strategy that employs nanoscale LATP (Li1+xAlxTi2-x(PO4)3) precursors to form, via high-temperature sintering, an amorphous/nanocrystalline LATP composite coating on LCO (denoted tp@LCO). This coating not only heals machining-induced surface defects but also enables thermal diffusion of Al3+/Ti4+ into the near-surface lattice of LCO, creating an integrated “coating-plus-doping” architecture. Owing to its Li⁺-conducting nature, the LATP interlayer helps maintain favorable interfacial Li⁺ transport and reduces charge-transfer resistance. In practical graphite||tp@LCO full cells cycled between 3.0 V and 4.5 V, the modified cathode delivers exceptional stability, retaining 81.9 % of its capacity after 2000 cycles with negligible median voltage decay, indicating minimal polarization buildup. Critically, the LATP layer passivates the cathode-electrolyte interface and suppresses exothermic parasitic reactions, allowing a 0.75 Ah pouch cell to withstand nail penetration without thermal runaway and substantially raising the onset temperature of thermal runaway in hot-box tests. This work demonstrates that multifunctional LATP interfacial layers can synergistically enhance both high-voltage performance and intrinsic safety of LCO-based batteries.

The development of electrolytes with effective anion-trapping functionality is pivotal for safe, high-rate lithium metal batteries, yet remains a formidable challenge. While electron-deficient alpha-hydrogen sites intrinsically attract anions, their concurrent high reactivity toward lithium metal leads to detrimental side reactions. Herein, we unlock a universal molecular design principle-the ortho alpha-hydrogen (O-alpha-H) motif-that breaks this paradox by simultaneously enhancing anion anchoring and passivating the reactive sites. This is achieved through the strategic placement of electron-withdrawing groups to forge adjacent alpha-H sites, which orchestrates a triple synergistic mechanism: (1) a Spatial Effect from multisite hydrogen bonding (O-alpha-H delta'& centerdot;& centerdot;& centerdot;F delta-/O delta-) that firmly binds anions, facilitating rapid Li' conduction and forming a dynamic shield to protect the alpha-H sites; (2) an Electronic Effect that delocalizes electron density to lower the reduction potential of alpha-H, intrinsically inhibiting reduction; and (3) Interfacial Regulation via molecular-level anion enrichment near the electrode surface, guiding the formation of a robust, anion-derived solid electrolyte interphase. Consequently, O-alpha-H-based electrolytes achieve superior Li' transference numbers and critical current densities, enabling remarkable high-rate cycling stability in Li||NCM811 cells. This work establishes the O-alpha-H motif as a versatile and foundational paradigm for designing high-performance electrolytes.

The main problems holding back inverted perovskite solar cells (PSCs) are poor crystal formation and too many defects inside the perovskite layer. We address both issues by introducing 4-aminobutylphosphonic acid, which effectively releases residual tensile stress and passivates film defects, leading to enhanced efficiency and stability. We report 4-aminobutylphosphonic acid as a multifunctional additive where the phosphonic acid (-PO3H2) and amine (-NH2) groups coordinatively passivate undercoordinated Pb2+ and I- vacancies, as supported by GIXRD measurements showing 64% reduction in residual tensile stress, and time-resolved photoluminescence shows enhanced carrier lifetime. The optimized devices achieve a champion power conversion efficiency (PCE) of 24.1% and retain 85% of its initial PCEs after 840 h under 1-sun illumination at 65 degrees C. This molecular engineering approach provides a facile route to concurrently boost efficiency and stability in inverted PSCs.

Efficient Li+ transport is crucial for ensuring the stability of Li metal anodes in Li metal batteries (LMBs). However, conventional vehicular transport in non-aqueous electrolytes, where Li+ migrates with an intact solvation shell, results in sluggish ion transport kinetics, thereby exaggerating Li+ flux heterogeneity and promoting dendritic deposition. Here, we propose a dipole-mediated solid-liquid interfacial solvation regulation strategy that leverages the abundant interface provided by a nano-ceramic electrolyte coating on the separator to accelerate and homogenize the Li+ transport. The high-dipole molecule 2,5-difluoro-4-nitrobenzoic acid (DNA) was employed to functionalize the ceramic coating, inducing strong ion-dipole interactions with Li+ and lowering the transport energy barrier at the interfacial region. Its low LUMO level further enables preferential reduction to generate a Li3N/LiF-enriched interphase, stabilizing the Li surface and suppressing electrolyte decomposition. As a result, the dipole-regulated interface delivers a high ionic conductivity (0.517 mS cm-1, compared with the pristine separator at 0.308 mS cm-1) and a Li+ transference number of 0.646, enabling dendrite-free Li deposition. Li‖LiFePO4 and Li‖NMC811 full cells exhibit markedly improved long-term cycling stability under high areal-capacity loadings, demonstrating the effectiveness and practical viability of this dipole-mediated interfacial solvation strategy for enhancing ion transport in LMBs.

Developing high-performance solid-state electrolytes with both fast Li* transport and stable interfaces remains a critical challenge for next-generation batteries. Herein, we report an innovative molecularlevel interfacial engineering strategy by covalently grafting amino-silane [3-(2-Aminoethylamino)pro pyl]trimethoxysilane (AEAPTMS) onto the surface of Li1.4Al0.2Ti1.8Si0.2P2.8O12 (LATSP) ceramic fillers within polyethylene oxide (PEO)-based composite solid-state electrolytes. Specifically, AEAPTMS not only alleviates filler agglomeration and reduces PEO crystallinity, but also provides unique interfacial functions. The -NH2 groups strongly anchor TFSI-anions via hydrogen-bonding interactions, while the weak coordination between Li* and AEAPTMS reduces the migration energy barrier, thereby regulating the Li* coordination environment and enabling accelerated interfacial Li* transport. Moreover, the engineered interface induces the formation of astable, LiF-rich SEI to suppress side reactions and enhance interfacial stability. Consequently, the optimized PEO-LATSP@AEAPTMS composite electrolyte exhibits superior electrochemical performance, including high ionic conductivity of 8.47 & times; 10-4 S cm-1, enhanced Li* transference number of 0.5, and improved compatibility with high-voltage cathodes. This work clearly distinguishes the dominant contribution of molecular-level interfacial engineering from the general filler effect, highlighting multifunctional molecular bridges as a promising strategy for high-performance composite solid electrolytes, and providing guidance for the rational design of practical solid-state battery systems. (c) 2026 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

The commercialization of Li metal anodes in all-solid-state lithium batteries (ASSLBs) is hindered by uncontrollable dendritic growth and nonuniform deposition during cycling. Here, we report a facile metal displacement strategy to construct a Li-Ga alloy anodic interlayer to suppress Li dendrite growth and stabilize the anode-solid-state electrolyte interface. The significantly enhanced performance originates from the dramatically improved Li diffusion kinetics, with the Li-Ga alloy modified Li (Li-Ga@Li) anode exhibiting a Li atomic diffusion coefficient twice as high as that of pristine Li metal. Consequently, the Li-Ga@Li|LPSCl|Li-Ga@Li symmetric cells deliver stable lithium stripping/plating behavior over 800 h with minimal polarization and a significantly increased critical current density. When paired with a high-loading LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode active material, Li-Ga@Li|LPSCl|NCM811 ASSLBs demonstrate enhanced rate capability and prolonged cycling stability. This work provides a practical interfacial engineering strategy through diffusivity improvement toward high-performance ASSLBs.

ZrO 2 /SiO 2 composite film was prepared on the surface of zirconium hydride by anodic oxidation + sol-gel sealing composite process to solve the problem of insufficient hydrogen resistance caused by defects such as micropores and microcracks in the anodic oxidation film of zirconium hydride. Using tetraethoxysilane (TEOS) as precursor, polyvinyl alcohol (PVA), silane coupling agent KH570 and A171 were introduced to regulate the sol structure, and the film was densified and stabilized by stepwise heat treatment. The microstructure, composition, phase, thermal behavior and molecular structure of the composite film were systematically analyzed by means of SEM, EDS, XRD, TGDSC and FTIR. The thickness, adhesion, microhardness and hydrogen resistance of the film were tested to reveal the defect repair mechanism and hydrogen resistance mechanism. The results show that PVA and silane coupling agent can significantly refine the sol particle size, improve the film density and interfacial bonding strength. The optimized composite film has a thickness of 27.15µm, a binding force of 70.74 N, a microhardness of 457HV, and an initial dehydrogenation temperature of 710°C, showing excellent mechanical properties and high-temperature hydrogen resistance. The composite membrane forms a double-layer protective structure through anodic oxide layer support + sol-gel layer sealing, which blocks cracks and pores macroscopically. At the micro level, O-H and C-H chemical bonds are used to capture hydrogen atoms and inhibit diffusion, so as to achieve high-efficiency hydrogen resistance modification of zirconium hydride. This process can provide theoretical basis and technical reference for the surface strengthening of zirconium hydride based hydrogen barrier materials in nuclear industry and space energy field.

Oxygen vacancies are often considered the active sites for CO2 conversion, but their engineering to enhance activity and stability has been scarcely investigated, especially at high reaction tempeture (≥600 °C) or under severe stressing conditions (i.e., in presence of H2S). We demonstrate that oxygen vacancies in defective MgO nanocrystals (less than 20 nanometres) can be significantly promoted by the addition of atomically dispersed Ce atoms anchored at these defective MgO sites. These catalysts combine high performance in CO2 conversion with exceptional stability even in the presence of 300 ppm H2S. For a loading <2 wt%, the Ce atoms are exclusively present as isolated species coordinated to oxygen-defective sites of MgO nanocrystals. These Ce single atoms promote the formation of these defects and facilitate the adsorption of CO2, enhancing the activation of H2 molecules, but do not play a role alone as single-atom catalysts. Extensive mechanistic studies, chemical kinetics and theoretical modelling prove that the single-atom-assisted oxygen vacancies (SA-Ov) enables the high catalytic performance and stability, thereby opening new avenues for catalyst design.

Interfacial degradation is a major bottleneck for LiFe1-x Mn x PO4 (LMFP) cathodes. Conventional surface modifications, such as inert coatings or doped layers, can mitigate interfacial metal dissolution but often at the cost of Li+ transport, leading to a long-standing trade-off between interfacial stability and interfacial electrochemical kinetics. Here, we reconciles this conflict by constructing a surface-confined Li-Fe antisite defect layer via a simple ferrocene-assisted thermal treatment. A moderate antisite concentration (similar to 3.2%) simultaneously densifies the surface lattice, significantly suppressing Mn and Fe dissolution while enabling a transition of Li+ diffusion from one-dimensional (1D) to three-dimensional (3D) at the surface. This dual-function surface significantly improves both cycling stability and kinetics of the LMFP. Beyond practical improvements, these results overturn the conventional view of antisite defects as purely detrimental, establishing controlled antisite engineering as a versatile paradigm for reconciling interfacial stability with fast ion transport in phosphate cathodes.

Poly(ethylene oxide) (PEO)-based solid polymer electrolytes exhibit low ionic conductivity and susceptibility to lithium dendrite-induced short circuits. To overcome these issues, we propose a facile and cost-effective strategy of incorporating KH550-modified montmorillonite (KMMT) as a multifunctional filler to reinforce PEO-based solid polymer electrolytes. The incorporation of KMMT not only reduces the crystallinity of the PEO matrix, but its negatively charged surface also attracts Li+ through electrostatic interactions, creating an oriented migration pathway for Li+ transport. Meanwhile, the hydrogen bonding interactions derived from the amino functional groups of KMMT improve the mechanical properties of the solid electrolyte. Benefiting from these synergistic effects, the as-prepared composite electrolyte exhibits remarkable ionic conductivity (4.99 x 10-4 S cm-1) and a wide electrochemical stability window (4.59 V) at 60 degrees C, while maintaining excellent mechanical strength (1.28 MPa). Leveraging these advantages, the Li||Li symmetric cell possesses ultra-stability by maintaining over 2000 h without short circuit. The LFP||Li solid-state cell demonstrates exceptional rate capability and cycling stability, underscoring the practical potential of the composite electrolyte. This study provides an effective material design strategy for the development of high-performance solid-state lithium batteries.

Gel polymer electrolytes combine the advantages of solid and liquid electrolytes, making them promising electrolyte candidates for lithium-metal batteries. However, low-temperature performance is hindered by sluggish ion transport and unstable electrolyte–electrode interfaces. Herein, a topology-driven solvation-decoupling strategy is proposed by designing a topological ester-based polymer electrolyte with dynamically polar side chains, enabling high-voltage lithium-metal batteries to operate reliably at low temperatures. This strategy dynamically reconstructs the local solvation environment within ester electrolytes, which simultaneously enhances lithium salt dissociation and lowers the desolvation energy barrier. The electrolyte exhibits ionic conductivities of 2.39 × 10−3 and 2.1 × 10−4 S cm−1 at 25 ℃ and −30 ℃, respectively, with a Li+ transference number of 0.76. Moreover, the tailored electrolyte composition stabilizes both lithium metal anodes and high-voltage cathodes (LiNi0.6Co0.2Mn0.2O2 and LiCoO2), enabling polymer-based cells to operate below −30 ℃. At −20 ℃ and 0.1 C, Li||LiNi0.6Co0.2Mn0.2O2 cells deliver a high discharge capacity of 151.3 mA h g−1 (>85% of that at 25 ℃). Notably, a Li||LiNi0.6Co0.2Mn0.2O2 pouch cell with a mass loading of 11.7 mg cm−2 can be stably cycled at −30 ℃. The Li||LiNi0.6Co0.2Mn0.2O2 cells demonstrate outstanding stability over a broad temperature range. This study provides a feasible strategy for designing high-performance gel polymer electrolytes for high-voltage lithium-metal batteries at extreme temperatures.

Interfacial degradation is a major bottleneck for LiFe1-xMnxPO4 (LMFP) cathodes. Conventional surface modifications, such as inert coatings or doped layers, can mitigate interfacial metal dissolution but often at the cost of Li+ transport, leading to a long-standing trade-off between interfacial stability and interfacial electrochemical kinetics. Here, we reconciles this conflict by constructing a surface-confined Li-Fe antisite defect layer via a simple ferrocene-assisted thermal treatment. A moderate antisite concentration (∼3.2%) simultaneously densifies the surface lattice, significantly suppressing Mn and Fe dissolution while enabling a transition of Li+ diffusion from one-dimensional (1D) to three-dimensional (3D) at the surface. This dual-function surface significantly improves both cycling stability and kinetics of the LMFP. Beyond practical improvements, these results overturn the conventional view of antisite defects as purely detrimental, establishing controlled antisite engineering as a versatile paradigm for reconciling interfacial stability with fast ion transport in phosphate cathodes.

Metal oxides have emerged as the dominant choice of matrix for the design and synthesis of supported catalysts with high-performance, because of the tunable surface properties, low cost, and strong interactions with active components. Herein, the nanoflower-like titanium dioxide (TiO2) is achieved through solvothermal approach. Then, boron (B) doped black TiO2 loaded with Ru (Ru/B-TiO2) is achieved through rapid (40 s) microwave quasi-solid approach. The incorporation of B modulates the energy band structure of the electrocatalyst, creating additional active sites, and then favors the water dissociation and following hydrogen desorption. The presence of oxygen vacancy defects and metal-support interactions (MSI) lead to satisfactory stabilization of the catalysts. These effects collectively contributed to the superior performance in 1 M KOH and alkaline seawater for the hydrogen evolution reaction (HER) with small overpotentials of 39 and 61 mV, respectively, which also demonstrates excellent activity and stability. This work presents a novel microwave-assisted strategy for constructing metal oxide supported low-content noble metals for energy conversion and storage applications.

Cathode prelithiation can compensate first-cycle irreversible lithium loss and increase the energy density of high–specific-energy Li-ion batteries. Li5FeO4 (LFO) is a promising prelithiation additive owing to its ultrahigh theoretical capacity and suitable delithiation potential; however, its severe air sensitivity limits practical implementation. Here we report a simple molecular-layer interface strategy using perfluorodecyltrimethoxysilane to in situ form an ultrathin composite protective layer on LFO (PT-LFO), enabling simultaneous improvements in air stability and electrochemical performance. After 7 days of exposure at 40 % relative humidity, PT-LFO retains 552.8 mAh/g available capacity, 67.1 % higher than pristine LFO. The coating reduces interfacial polarization and accelerates Li⁺ transport, delivering 690.5 mAh/g at 1 C. In a Ni-rich cathode || graphite–SiOₓ (9.5 wt%) full cell, PT-LFO increases the initial discharge capacity to 207.5 mAh/g, a 10.3 % improvement over the reference (188.1 mAh/g). This scalable interfacial regulation provides a practical pathway toward air-stable, high-capacity prelithiation additives.

Layered sodium oxide cathodes form electrochemically unstable Na2CO3 in humid air, causing capacity fade. This work redefines its role in cathode-electrolyte interphase (CEI) evolution. While a thick, loose Na2CO3 layer promotes detrimental side reactions, a controlled layer can be transformed beneficially. Introducing fluoroethylene carbonate (FEC) enables this Na2CO3 to react in situ, forming a NaF-rich CEI with a dual-layer structure: a dense, insulating NaF inner layer and a Na2CO3 outer layer. This effectively suppresses interfacial decomposition, enhancing cycling stability. To minimize initial Na loss, a hydrophobic self-assembled monolayer (SAM) was employed to precisely regulate the Na2CO3 thickness. The resulting composite "NaF/SAM-Na2CO3" CEI synergistically delivers high initial capacity and exceptional long-term cyclability, achieving 88.7% capacity retention after 500 cycles. This study reveals Na2CO3's positive function and proposes a "preconstruction in situ transformation" strategy for designing advanced battery interfaces.