Polymer electrolytes for lithium metal batteries face a fundamental trade-off between mechanical strength and ionic conductivity. Herein, the ethylene-vinyl acetate (EVA) acts as a molecular "expander" to widen the interlayer spacing of organically modified montmorillonite (OMMT) from 2.20 nm to 3.17 nm, as verified by Xray diffraction. This expansion bridges isolated ion channels and reduces polymer crystallinity, facilitating fast Li+ transport visualized by molecular dynamics simulations. Simultaneously, EVA induces physical cross-linking with the polymer matrix and improves OMMT dispersion, resulting in a high tensile strength of 5.56 MPa. The resulting open-framework architecture further promotes three-dimensional Li nucleation and the formation of a LiF-and Li3N-rich solid electrolyte interphase. Consequently, the EVA/LOPPM (LiTFSI/PVDF/P(VDF-HFP)/ PMMA/OMMT, where LOPPM denotes a hybrid composition consisting of lithium bis(trifluoromethanesulfonyl) imide (LiTFSI), PVDF, poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDF-HFP), poly(methyl methacrylate) (PMMA), and organically modified montmorillonite (OMMT)) composite achieves a Li+ transference number of 0.72 and a room-temperature ionic conductivity of 2.01 & times; 10-3 S cm-1. In Li||LiFePO4 cells, it delivers a discharge capacity of 138 mAh g-1 at 5C and retains 106 mAh g-1 after 100 cycles. This work provides a nanostructure-guided strategy to decouple the conductivity-strength dilemma in polymer electrolytes.

The interfacial defects induced by halide ion migration critically limit the performance scalability of solution-processed perovskite solar cells (PSCs). Here, we demonstrate an engineering strategy using zwitterionic potassium hydrogen phthalate (KHP). This approach synergistically regulates crystallization dynamics and passivates multidimensional defects via atomic-scale interface anchoring. Time-resolved AFM characterization reveals that the amphiphilic KHP, with C═O/Pb2+ coordination capability, induces self-assembled boundary confinement during perovskite crystallization, generating ultrasmooth films with 68% reduced surface roughness (average roughness (Ra) = 62 nm vs control 112 nm). Multinuclear (1H/207Pb) NMR analyses decipher the dual-anchoring mechanism, where KHP coordinates Pb2+ via carboxyl oxygen (207Pb upfield shift Δδ = 1020 ppm, [PbI6]4- → [PbI5(OOCR)]3-) while forming NH3···HOOC- hydrogen bonds with the hydrogen phthalate anion (HP-) (2D COSY J-coupling at 7.95 ppm), synergistically immobilizing halides through this molecular vise effect as corroborated by XPS-derived Pb2+ reduction (Pb 4f7/2 peak shift of 1.25 eV). The dual passivation mechanism involving both Pb defects and halide vacancies enables a record PCE of 6.17% for air-processed low-cost PSCs, achieving absolute efficiency enhancement over the baseline. Herein, ambient-air fabricated perovskite solar cells via zwitterion-mediated interface anchoring achieve 6.17% efficiency and 71.12% stability (360 h), with enhanced moisture resistance (contact angle: 31° → 59°), enabling scalable low-cost production under noninert conditions.

Heteronuclear Ni-Co dual-atom catalysts anchored on nitrogen-doped carbon (NiCo DACs/NC) are constructed to clarify the relationship between intermetallic d-d orbital coupling and bidirectional sulfur redox kinetics in lithium-sulfur batteries. Combining spin-resolved density functional theory, spin-density mapping, and potential-dependent magnetic measurements, we demonstrate that d-oupling reconstructs the local 3d electronic structure, induces interfacial spin-related electronic redistribution, and undergoes reversible dynamic evolution during sulfur reduction and Li2S oxidation. This regulation enhances polysulfide conversion, Li & horbar;S bond activation, and Li2S nucleation/deposition as well as oxidation/decomposition. Consequently, the NiCo DACs/NC-based Li-S battery delivers a discharge capacity of 1129.6 mAh g-1 at 1C and retains 864.6 mAh g-1 after 500 cycles (0.034% decay per cycle). Under a high sulfur loading of 9.12 mg cm-2 and lean electrolyte (3.5 & micro;L mg-1 an areal capacity of 7.69 mAh cm-2 is achieved. A pouch cell delivers a component-level energy density of 321.2 Wh kg-1 with 88.7% retention after 50 cycles. This work provides mechanistic insight into spin-related electronic dynamics for designing high-performance dual-atom catalysts in Li-S batteries.

ABSTRACT Despite the exceptionally high theoretical energy density of all‐solid‐state lithium–sulfur batteries (ASSLSBs), their practical performance is severely limited by discontinuous interfacial contact and sluggish transport of electrons and lithium ions. These issues cause accumulation of locally electrochemically inactive sulfur, resulting in electrode passivation and uneven reaction distribution, which are critical bottlenecks to performance improvement. In recent years, redox mediators (RMs) have garnered significant attention due to their ability to effectively regulate complex multiphase reaction processes in liquid‐phase lithium–sulfur (Li–S) systems. However, whether RMs can enable efficient and closed‐loop redox cycling under solid–state conditions remains a central challenge. To address this issue, this review systematically summarizes and compares sulfur conversion pathways across different electrolyte systems, with a particular focus on the mechanistic roles of RMs in regulating the transformation of sulfur species in ASSLSBs. It further discusses the relationship between the molecular structures of representative RMs and their electrochemical performance. The key scientific problems and engineering challenges currently facing the field are identified. The review outlines future directions for molecular designs of tunable RMs and a deeper understanding of redox mechanisms in solid–state environments to provide theoretical guidance and design strategies for high–performance ASSLSBs.

High-entropy materials enable entropy-stabilized structures and tunable active sites to suppress polysulfide shuttling and accelerate sulfur redox kinetics in Li–S batteries.

Herein, we demonstrate that ethylene-vinyl acetate (EVA) serves as a molecular "expander" to significantly increase the interlayer spacing of organic-modified montmorillonite (OMMT). This structural expansion, driven by the physical binding of vinyl acetate groups within the polymer electrolyte (PE) matrix, bridges isolated conduction channels and reduces crystallinity, thereby facilitating rapid lithium-ion transport as visualized by molecular dynamics (MD) simulations. The resulting open-framework architecture triggers a three-dimensional nucleation process, promoting the formation of a robust solid electrolyte interphase (SEI) rich in LiF and Li3N. Consequently, the EVA/LOPPM composite achieves a high tensile strength of 5.56 MPa and a markedly enhanced lithium-ion transference number (tLi+) of 0.72. When paired with LiFePO4 (LFP) cathodes, the solid-state batteries deliver a high discharge capacity of 138 mAh g-1 at 5 C and maintain 106 mAh g-1 after 100 cycles at room temperature, demonstrating superior electrochemical performance and dendrite suppression.

Solid-state polymer lithium–sulfur batteries have attracted considerable attention because they combine high energy density with good safety. However, their performance is still limited by sluggish Li+ transport and insufficient effective Li+ supply on the sulfur cathode side. Conventional modification strategies are often constrained by the inhomogeneous dispersion of modifying components and localized interfacial contact, making it difficult to achieve uniform regulation of ion transport. Therefore, in this work, a silicone polyurethane (SiPu)-modified poly(vinylidene fluoride) (PVDF)-based composite polymer electrolyte was designed to regulate Li+ coordination and transport through the intrinsic molecular structure of the polymer. The carbamate, polyether, and siloxane segments in SiPu provide differentiated Li+ coordination strengths, constructing a strong-medium-weak multilevel coordination network that promotes LiTFSI dissociation and enables continuous Li+ migration. Benefiting from this molecular regulation, the PVDF/SiPu/LiTFSI electrolyte exhibits a low ion-transport activation energy of 11.04 kJ mol-1 and a high Li+ transference number of 0.74. The assembled solid-state lithium-sulfur battery delivers a discharge capacity of 895.7 mAh g-1 at 0.1 C and retains 414.1 mAh g-1 after 200 cycles at 0.2 C. This study provides a new design strategy for synergistically regulating lithium salt dissociation, segmental motion, and Li+ transport through the intrinsic molecular structure of polymers, offering guidance for constructing high-performance solid-state lithium–sulfur batteries.

The development of next-generation solid-state batteries for extreme applications, such as aerospace, electric vehicles, and wearable electronics, requires polymer electrolytes (PEs) capable of operating under high voltage, wide temperature ranges, and mechanical deformation; however, conventional PEs are fundamentally constrained by an intrinsic "mechano-electro-thermal" (MET) trilemma, in which ionic conductivity, electrochemical stability, and mechanical robustness cannot be simultaneously optimized. This limitation originates from the molecular structure and topological characteristics of polymer systems, leading to interfacial oxidative decomposition at high voltages, sluggish ion transport at low temperatures, and mechanical instability under deformation. To overcome these challenges, this review proposes a mechanism-driven, multi-scale synergistic design framework: electronic structure regulation (e.g., fluorination engineering) lowers the highest occupied molecular orbital (HOMO) to enhance oxidative stability; phase behavior optimization enables stable ion transport over a wide temperature range (-40 to 150 degrees C); and network topology engineering via dynamic bonding and interpenetrating structures reconciles mechanical flexibility with ionic conductivity. By establishing correlations between multi-scale structural design and macroscopic electrochemical performance, this review provides a unified pathway to decouple the MET trilemma and outlines future directions toward adaptive polymer electrolytes for high-performance solid-state batteries.

Lithium-metal batteries (LMBs) face critical challenges in interfacial instability and dendritic growth, despite their high theoretical capacity. To address these issues, we designed an interface layer containing LiNbO3 crystals to modify the polymer electrolyte, achieving uniform deposition of lithium ions. This design innovatively integrates electrostatic screening and field-guided ion transport mechanisms─unique to LiNbO3 dielectric polarization materials─achieving unprecedented homogeneous Li+ flux distribution while catalytically mediating the formation of a dual-functional LiF/Li3N-rich solid electrolyte interphase (SEI). Notably, the Li3N component synergistically enhances ion diffusion, while LiF mechanically suppresses dendrites, synergizing physicochemical stabilization where conventional SPEs fail. The optimized LN-SPE demonstrates exceptional ionic conductivity of 4.92 × 10-4 S cm-1 and Li+ transference number of 0.67 at RT, enabling an assembled SSLMB to deliver 138.1 mAh g-1 at 0.5 C with ultrahigh capacity retention of 94.42% after 100 cycles, while maintaining 142.4 mAh g-1 at 1 C. Crucially, the sustained dielectric polarization activity ensures long-term interfacial integrity, positioning this work as a paradigm-shifting approach for electroceramic-polymer hybrids with scalable manufacturing pathways, thus offering transformative solutions for next-generation high-energy-density batteries.

Anode-free lithium metal batteries (AFLMBs) enhance energy density by using bare copper (Cu) foils as the anode. However, they face challenges due to irreversible lithium (Li) plating caused by the inherent lithiophobicity of the materials. In this study, we present an ultraviolet-assisted in-situ polymerization strategy to create a poly(tannic acid) film embedded with silver (Ag) nanospheres (PTA@Ag-Cu) in just 15 min. The PTA film improves the wettability of the electrolyte, reducing the contact angle by 50.6 %, and accelerates Li+ desolvation. The Ag nanoparticles (21 nm) lower the nucleation overpotential to 10 mV compared to 150 mV for bare Cu, through the formation of a lithiophilic LiAg alloy. The charge-transfer dynamics and embedded electric fields, which are verified by density functional theory (DFT), contribute to the uniform deposition of Li, as evidenced by in situ optical microscopy. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) indicates a synergistic regulation of Li+ flux at the atomic level by the combination of Ag and molecular-level interactions from PTA. The PTA@Ag-Cu||LiFePO4 configuration achieves 61.2 % capacity retention after 100 cycles at a rate of 1 C-rate without pre-lithiation. The preparation of PTA@Ag-Cu using UV-assisted polymerization is economical, time-saving, and suitable for large-scale production. This work introduces a photo-induced dualfunctional interface that addresses AFLMB degradation through integrated electric field engineering, making it compatible with roll-to-roll battery manufacturing.

Perovskite solar cells (PSCs) have emerged as promising candidates to profoundly impact the photovoltaic industry due to their high efficiency and low-cost manufacturing advantages. Nickel oxide (NiOX)-based inverted PSCs are promising candidates for advancing perovskite photovoltaics toward commercialization, leveraging their remarkable stability, scalability, and cost-effectiveness. However, the low conductivity of NiOX limits PSCs performance. Incorporating cobalt oxide (Co3O4) as a dopant enhances stability and minimizes charge loss, significantly improving hole transport properties. Co3O4 incorporation shifts the valence band of NiOX films, achieving better alignment with the valence band of the perovskite layer. The optimized device achieves a peak power conversion efficiency (PCE) of 9.51

In the pursuit of sustainable energy, lithium-ion batteries (LIBs) have revolutionized storage solutions and advanced the development of electric vehicles. However, as LIBs near their energy density limits and face...

The deepening electrification of society and the wide application of electric vehicles have raised the demand for high-energy-density batteries. The anode-free lithium-metal battery (AFLMB), which relies on a simple internal structure of the battery to bring about high energy density, has a broad application prospect. The lack of surplus Li metal at the anode restricts the active material in AFLMB to only the cathode and electrolyte, resulting in a more concentrated distribution within the batteries. Thus, most AFLMBs encounter a rapid decline in capacity after 100 cycles, presenting a significant challenge. Maximizing the effectiveness of the limited active substances is the breakthrough to improve the cycling performance of AFLMB. Based on the latest research findings, this paper presents a comprehensive analysis of the factors for the capacity decline in the AFLMB cycling process, specifically focusing on the behavior of Li deposition on the anode. We explore the relationship between the lithophilic nature of the substrate and Li deposition morphology, along with methods for characterization, and propose optimal spherical deposition. Furthermore, it discusses strategies for optimizing Li deposition behavior through current collector modification, electrolyte modification, and improvement of test conditions. Ultimately, this evaluation of optimization strategies for Li deposition morphology aims to offer insights for advancing AFLMB development and enhancing its long-cycle stability.

Lithium-sulfur batteries that utilize polymer electrolytes can significantly reduce polysulfide shuttling, offer high safety, and represent a promising energy storage solution. However, constructing efficient ion transport pathways at the electrode/electrolyte interface and within the cathode of solid-state lithium-sulfur batteries remains challenging. In this study, we proposed a polymer electrolyte made from a poly (vinylidene fluoride cohexafluoropropylene) (PVDF-HFP) matrix with neodymium trioxide (Nd2O3) nanorods as fillers. This polymer electrolyte slurry was incorporated into the cathode to establish a lithium-ion pathway between the electrode and the electrolyte. The potential difference between Nd2O3 and the carbon layer generates an internal electric field, facilitating the formation of a smooth lithium-ion transport channel in a solid-state environment. We visualized these lithium-ion transport channels across the cathode interface using Molecular Dynamics (MD) simulations in an electric field. Simultaneously, the abundant oxygen vacancies in Nd2O3 can interact with carbon groups in N,N-Dimethylformamide (DMF), promoting the formation of [Li(DMF)x]+ complexes. This interaction effectively reduces the radicalized DMF and enhances lithium-ion (Li+) conduction. As a result, the solid-state lithium-sulfur battery demonstrated excellent cycling performance at room temperature, achieving a specific capacity of 940.8 mAh g- 1 at a rate of 0.1C. This work contributes valuable insights for developing solidstate lithium-sulfur batteries with improved compatibility at electrode/electrolyte interfaces.

Solid polymer electrolytes (SPEs) are considered a key enabler for high-safety and high-energy-density solid-state lithium-metal batteries. However, challenges such as low ionic conductivity, poor interfacial compatibility, and limited thermal stability continue to hinder their practical application. This review explores the interaction mechanisms in SPEs in detail from four aspects—Lewis acid-base theory, anion vacancies, hydrogen-bond networks, and phase-separated structures—and introduces three functionalized design strategies: channel design, high-entropy design, and flame-retardant design. We also comprehensively discuss the latest advancements and development potential in artificial interface design and in situ interface design. This article outlines strategies to overcome existing bottlenecks and emphasizes the importance of functional design. By modulating these microinteractions and optimizing design strategies, it will help accelerate the commercialization of high-safety, high-energy-density solid-state batteries.

Polymer electrolytes (PEs) are essential for high-energy-density, safe, and durable lithium metal batteries (LMBs). However, their widespread adoption is hindered by inherent challenges such as low ionic conductivity and uneven lithium deposition. Here, we present an innovative strategy to engineer a novel polyvinylidene fluoride (PVDF)-based polymer electrolyte by incorporating lithium-ion nonconductive fillers and polymer additives. The optimized electrolyte exhibits remarkable ionic conductivity (approximate to 0.31 mS.cm-1) and mechanical toughness (approximate to 393 %), attributed to the synergistic interaction between lanthanum oxide (La2O3) and polyvinylpyrrolidone (PVP). Specifically, oxygen vacancies in La2O3 strongly adsorb bis(trifluoromethane sulfonyl) imide anions (TFSI-), promoting free lithium-ion mobility, while the C--O groups in PVP engage in ion-dipole interactions with lithium ions, ensuring uniform ion flux. This dual mechanism facilitates rapid and stable lithium-ion transport, resulting in an expanded electrochemical stability window (4.61 V) and an elevated lithium-ion transfer number (tLi+ = 0.54). In practical applications, LMBs employing this electrolyte demonstrated exceptional cycling stability, achieving 200 cycles with a capacity retention of 75.3 % at 1.5C. This work presents a novel strategy for the construction of high-performance polymer electrolytes and establishes a basis for nextgeneration LMBs with improved safety and efficiency.

The polysulfide shuttling and sluggish sulfur redox kinetics hinder the commercialization of lithium-sulfur (Li-S) batteries. Herein, the fabrication of phosphorus (P)-doped iron telluride (FeTe2) nanoparticles with engineered Te vacancies anchored on nitrogen (N)-doped carbon (C) (P-FeTe2-x@NC) is presented as a multifunctional sulfur host. Theoretical and experimental analyses show that Te vacancies create electron-deficient Fe sites, which chemically anchor polysulfides through enhanced Fe─S covalent interactions. Additionally, P doping shifts the Fe d-band center toward the Fermi level, increasing the affinity for polysulfide intermediates through d-p orbital hybridization. This dual modulation strengthens the built-in electric field at the P-FeTe2-x/NC interface, effectively suppressing the shuttle effect and accelerating redox kinetics. The optimized P-FeTe2-x@NC host enables Li-S batteries to achieve an initial capacity of 1475.6 mAh g-1 at 0.1 C and remarkable cycling stability, exhibiting only a 0.031% capacity decay per cycle over 1000 cycles at 1 C. High sulfur utilization is evidenced by attaining 6.51 mAh cm-2 areal capacity under a loading of 7.80 mg cm-2, while a 2.67 Ah pouch cell delivers an energy density of 326.6 Wh kg-1. This work establishes a vacancy-doping synergy strategy for coordinating adsorption and conversion processes in sulfur electrochemistry, offering new insights into the design of high-energy-density batteries.

In electrochemical energy storage (EES), lithium-sulfur (Li-S) batteries have recently gained recognition for their exceptional theoretical specific capacity, making them stand out among a wide range of cutting-edge energy storage technologies. While Li-S batteries demonstrate a long cycle life under regular conditions, expanding their application scenarios is crucial for their future development. Specifically, ensuring stable battery operation in extreme temperature environments, such as below 0 degrees C and above 60 degrees C, becomes paramount. Thus, this review aims to summarize the recent progress of Li-S batteries in extreme temperature ranges and analyse the processability of critical materials within these batteries at extreme temperatures. Ultimately, this review presents insights and potential prospects for Li-S battery systems operating within a wide temperature range, contributing to advancing energy storage devices capable of functioning across various temperatures. Despite the inherent long cycle life of Li-S batteries under normal operating conditions, ensuring their stable performance in extreme temperatures, particularly below 0 degrees C and above 60 degrees C, is imperative for expanding their application range. This review aims to comprehensively summarize recent advancements in the field of Li-S batteries, with a primary focus on their electrochemical performance and longevity under extreme temperature conditions. image