Lithium metal batteries (LMBs) are promising for high-energy–density electrochemical storage, yet their industrial deployment is severely hindered by Li dendrite growth and unstable electrode–electrolyte interfaces caused by inhomogeneous ion flux and sluggish interfacial kinetics. Herein, a green, scalable PP@Me-PVDF/mSiO2 composite separator was fabricated via non-solvent-induced phase separation (NIPS), an industrially compatible process, using earth-abundant mesoporous silica (mSiO2) to replace high-cost rare fillers for spatiotemporal Li⁺ transport regulation. Spatially, mSiO2 immobilizes PF6− anions and modulates the local electric field to homogenize Li⁺ flux. Temporally, its hierarchical porous structure optimizes Li⁺ desolvation and diffusion kinetics, shifting Li⁺ nucleation from uncontrolled 3D instantaneous to controllable progressive mode, inducing a dense LiF-rich solid electrolyte interphase (SEI), and effectively suppressing dendrite growth. Electrochemical tests confirm superior engineering performance: Li||Li symmetric cells cycle stably for over 1300 h at 0.2 mA cm−2 and 1000 h at 2 mA cm−2. LiFePO4||Li full cells deliver excellent rate capability (87.1 mAh g−1 at 7C) and long-term cycling stability (93.7% capacity retention after 1200 cycles at 5C). In-situ/ex-situ characterizations validate the dendrite inhibition and stable SEI formation mechanisms. Notably, a facile low-energy regeneration strategy (cosolvent cleaning + vacuum drying) enables closed-loop utilization of spent separators, realizing material circularity for industrial battery systems. This work provides a sustainable engineering strategy for high-performance LMB separators and offers valuable insights for interfacial engineering of other high-energy battery systems toward eco-friendly industrial development.

A novel fluorinated diamine monomer, 4,4'-((bicyclo[2.2.1]hept- 5-ene-2,3-diylbis (methylene)) bis(oxy))bis(3- (trifluoromethyl) aniline) (NFDA), featuring a tailored alicyclic norbornane core, flexible ether linkages, and pendant trifluoromethyl groups, was successfully synthesized. This monomer was polymerized with six commercial dianhydrides to produce a series of poly(amic acid) precursors, which were subsequently converted into high-performance polyimide (PI) films via a thermal imidization process. The strategic integration of the alicyclic, ether, and fluorinated motifs within the polymer backbone resulted in materials with an exceptional combination of properties. These PI films display outstanding solubility in a wide range of organic solvents, including low-boiling options like chloroform and tetrahydrofuran, highlighting their superior solution processability. The films are amorphous and exhibit remarkable hydrophobicity, evidenced by high water contact angles (up to 109.4°) and minimal water absorption (as low as 0.26%). Furthermore, they possess excellent optical transparency, with a maximum transmittance of 86.7% in the visible region. The materials also maintain robust thermal stability, with 5% mass loss temperatures exceeding 416 °C, and offer a desirable balance of mechanical strength and flexibility. This unique set of attributes, stemming from a rational molecular design, positions these polyimides as highly promising candidates for next-generation flexible electronics and advanced photovoltaics.

In situ-polymerized 1,3-dioxolane (DOL) electrolytes offer a promising route to quasi-solid-state lithium metal batteries (QSSLMBs), yet their limited oxidative tolerance and unstable electrode interfaces restrict high-voltage operation. Here, a simulation-guided dual-track regulation strategy uses MoCl5 as a multifunctional initiator to couple DOL ring-opening polymerization with Li-salt dissociation and inorganic interphase construction. MoCl5 promotes formation of a high-molecular-weight poly(1,3-dioxolane) (PDOL) matrix and LiF/LiCl/LixMoy-enriched solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), improving bulk stability, Li+ transport, and interfacial robustness. The resulting MoCl5-regulated PDOL electrolyte achieves a Li+ transference number of 0.71 and an electrochemical stability window of 4.7 V. Li||Li symmetric cells cycle for over 1000 hours at 5 mA cm-2, while high-voltage Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) cells retain over 95% capacity after 50 cycles at 2 C. This work establishes a design principle for multifunctional initiators and unlocks the high-voltage potential of ether-based electrolytes, advancing the practical application of QSSLMBs.

Solid-state batteries hold great promise for energy storage but remain constrained by the inherent trade-off between high ionic conductivity and interfacial stability in polymer electrolytes. Here, we introduce a natural, biocompatible beta-cyclodextrin-based MOF (beta-CD-MOF) as a multifunctional filler in a poly(ethylene oxide)/polyacrylonitrile composite. The inherent hydroxyl groups of the beta-CD-MOF create a pervasive hydrogen-bonding network that actively bridges the polymer phases, constructing continuous three-dimensional ion transport highways. This bio-derived framework simultaneously disrupts polymer crystallinity, anchors anions, and regulates the lithium-ion coordination environment. The resulting solid electrolyte exhibits a high ionic conductivity of 3.97 x 10-4 S cm-1 at 30 degrees C and an elevated Li+ transference number of 0.54. This synergistic mechanism enables exceptional interfacial stability, allowing a Li parallel to Li symmetric cell to cycle steadily for over 1000 hours and a LiFePO4 parallel to Li full cell to retain 87.2% of its capacity after 1000 cycles at 1C. Our work demonstrates that natural MOFs can be engineered to create sophisticated ion-conducting networks, moving beyond the conventional role of passive fillers. This approach establishes a new strategy for sustainable material design in next-generation energy storage, unifying performance with environmental considerations.

Solid polymer electrolytes face a fundamental trade-off between ionic conductivity and interfacial stability, particularly when incorporating the plasticizer succinonitrile (SN): specifically, SN boosts Li+ conductivity by tailoring the Li+ coordination environment and facilitating Li+ transport; However, the uncontrolled diffusion and electrochemical degradation of SN undermine the stability of Li metal anode interface. We address this challenge by constructing coordination-engineered ion highways within a hierarchical iron-based metal-organic framework (MOF) architecture, through rationally designing Fe3+-cyano (CN-) coordination bonds as molecular anchors to permanently immobilize SN within the MOF nanopores while simultaneously regulating the competitive coordination of Li+ among MOF-immobilized SN, poly(ethylene oxide) (PEO), and TFSI-anions. This dual-regulation strategy simultaneously constructs continuous 3D Li+ transport pathways and suppresses parasitic reactions, delivering a high room-temperature ionic conductivity (1.16 mS cm-1), a high Li+ transference number (0.80), and a extended electrochemical window of 5.2 V. The dual-regulation strategy enables dendrite-free Li plating/stripping for 1600 h in Li/Li symmetric cells, while a LiFePO4 (LFP) full cell retains 85.6% of its initial capacity after 1200 cycles at 2 C. Multiscale characterizations and modeling reveal how the Fe3+-CN "molecular lock" impedes SN degradation, while optimized Li+ flux homogenization facilitates the formation of an inorganic-rich interphase that suppresses dendrite growth. This work provides a versatile strategy for decoupling ion conduction from interfacial degradation in solid-state batteries.

The strategic selection of electrolytes critically governs charge storage behavior in supercapacitors, with ionic liquid mixtures demonstrating particular promise for achieving high energy densities. This study pioneers a heterosized ion synergy approach, where rationally paired large/small anions dynamically adapt to hierarchical carbon pore architectures in the micropores region, compressing free volume through dense ion packing. This confinement effect critically restricts ionic degrees of freedom, enhancing adsorption stability at electrode interfaces. The heterosized ion-pore structure matching system achieves significantly enhanced energy density, remarkably suppressed self-discharge kinetics, and maintains robust capacitance retention across a wide temperature range (-20 to 80 degrees C), establishing a new electrolyte design principle for high-stability energy storage under thermal extremes.

ABSTRACT Lithium sulfide (Li 2 S) is a critical cathode material for high‐energy‐density lithium sulfur batteries and an indispensable precursor for sulfide solid electrolytes. Traditional high‐temperature carbothermal reduction remains energy‐intensive and carbon‐heavy, creating a significant mismatch with industrial sustainability targets. This review focuses on engineering‐oriented green synthesis routes, systematically analyzing low‐temperature solid‐state reactions, magnesiothermal reduction, and solution‐based metathesis pathways. It highlights process intensification, scale‐up feasibility, techno‐economic analysis, and by‐product valorization. Current challenges in industrial amplification, including mass transfer limitations and cost competitiveness, are critically evaluated. Future directions emphasize continuous‐flow manufacturing, closed‐loop solvent recovery, and hybrid process integration, providing actionable technical pathways to enable cost‐effective, low‐carbon Li 2 S production for industrial applications.

A bone-inspired PP@Li-HAP/PAN separator integrates mechanical reinforcement and ion regulation to suppress Li dendrites and enable long-life lithium metal batteries.

Lithium-sulfur (Li-S) batteries are promising candidates for high-energy-density storage but face challenges such as polysulfide-shuttling and safety concerns associated with liquid electrolytes. While solid-state electrolytes offer potential solutions, they often suffer from low ionic conductivity at room temperature and poor interfacial contact. In this work, we present a composite solid electrolyte (CSE) engineered using F127 triblock copolymer via a scalable solution-casting approach. F127 serves a triple role: its micelles template the assembly of PVDF-HFP to suppress crystallinity (reducing the relative crystallinity from 47.1

The global transition to sustainable energy demands energy storage systems balancing ultrahigh energy density, intrinsic safety, and long cycle life. Lithium‑sulfur (LiS) batteries, with a theoretical energy density of 2600 Wh kg−1, represent a transformative alternative to lithium-ion batteries, yet their commercialization is constrained by polysulfide shuttling, poor solid-solid interfacial compatibility, and lithium dendrite growth. Herein, we report a 1-butyl-3-methylimidazolium thiocyanate (BMIM-SCN)-mediated bulk-interface co-tuning strategy for poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/F127-based composite solid-state electrolytes (CSEs), addressing these challenges via a four-fold synergistic effect. This tuning modulates polymer crystallinity, promotes lithium salt dissociation, optimizes interfacial wettability, and induces a stable solid electrolyte interphase (SEI). The resultant CSE-BS exhibits a room-temperature ionic conductivity of 1.20 × 10−3 S cm−1, Li+ transference number of 0.70, tensile strength of 33.4 MPa, and electrochemical stability window >4.78 V. Integrated into solid-state LiS batteries, CSE-BS delivers an initial discharge capacity of 1499 mAh g−1 at 0.1C, retains average capacity 840 mAh g−1 after 200 cycles at 0.2C (0.13% per-cycle decay), and maintains average capacity 667 mAh g−1 after 200 cycles at 1C. Mechanistic studies confirm BMIM-SCN induces a low-crystallinity (8.9%) polymer bulk and a LiF-rich SEI, collectively suppressing dendrite growth and stabilizing the electrode-electrolyte interface. This work establishes a scalable bulk-interface co-optimization strategy for CSEs, advancing practical high-energy solid-state LiS batteries and empowering next-generation energy storage technologies.

Poly(ethylene oxide) (PEO) solid electrolytes offer processability, flexibility and low-cost, yet their poor ionic conductivity and limited dendrite suppression capability impedes practical applications. Despite advances in Li+ transport kinetics, performance degradation persists due to space-charge polarization induced by uncontrolled anion migration. Here, we present a covalent organic framework (COF) for synchronous cation and anion regulation. By integrating lithiophilic methoxy groups and anionophilic imidazolium species into a single framework, this ionic COF (ICOF) enables synergistic ion management in PEO electrolytes. Ordered channels with fast-hopping sites facilitate rapid Li+ conduction, while cationic sites immobilize TFSI- anions, preventing anion depletion and subsequent space-charge polarization. This dual-ion regulation leads to an Li+ transference number of ∼0.72 and effective dendrite mitigation in symmetric-cells as well as full-cells with LiFePO4 and high-voltage NCM811 cathodes. By engineering COFs with spatially segregated yet functionally complementary motifs, selective anion immobilization alongside fast cation transport is achievable, potentially breaking the conventional trade-offs that have limited PEO-based lithium metal batteries.

The practical application of lithium-sulfur batteries (LSBs) is hindered by critical challenges such as the dissolution-induced shuttle effect of lithium polysulfides (LiPSs) and sluggish electrochemical kinetics. Therefore, the rational design of high-performance sulfur cathode materials has emerged as an effective strategy to enhance sulfur utilization and improve redox kinetics. In this study, we report a defect-rich bimetallic sulfide catalyst (CoNi2S4@NC), derived from zeolitic imidazolate framework-67(ZIF-67) and grown in situ on its surface, as a multifunctional sulfur host. Benefiting from its dual catalytic functions-strong chemical adsorption of LiPSs and efficient catalytic conversion of LiPSs intermediates-CoNi2S4@NC effectively suppresses the shuttle effect and accelerates redox kinetics. Additionally, the synergistic effect of its hollow structure and nitrogen-doped carbon matrix enhances electronic conductivity and alleviates volume expansion during cycling. First-principles calculations further verify the strong LiPSs binding energy and catalytic activity of CoNi2S4@NC. Electrochemical tests demonstrate that lithium-sulfur batteries employing CoNi2S4@NC as the sulfur host deliver outstanding lithium storage capacity and cycling stability. A high initial discharge capacity of 1379.7 mAh g-1 was achieved at 0.1C, and after 800 cycles at 1C, the battery maintained excellent capacity retention with an average capacity fading rate of only 0.065 % per cycle. Even under harsh conditions of high sulfur loading and lean electrolyte, the system still delivered impressive electrochemical performance. In summary, the designed dual-functional sulfur cathode material offers new insights and significant guidance for the development of highperformance lithium-sulfur batteries.

This work introduces nickel (II) tetraphenylporphyrin (NiTPP) as a multifunctional electrolyte additive to simultaneously address polysulfide shuttle and uncontrolled lithium dendrite growth in lithium-sulfur (Li-S) batteries. Mobile NiTPP species act as homogeneous catalysts with Ni-N4 centers for rapid polysulfide redox mediation to suppress migration, while planar molecules featuring lithium-affinity capability migrate to the lithium metal surfaces, enabling uniform lithium flux and anode protection. NiTPP-modified electrolytes significantly enhance Li-S battery performance, demonstrated by 634.9 mAh g-1 at 4C, 758.3 mAh g-1 after 100 cycles at 0.2 C (83.4% retention), and 757.5 mAh g-1 under high sulfur loading (2.9 mg cm-2) with lean electrolyte (E/S = 5 mu L mg-1), all with high Coulombic efficiency. Crucially, NiTPP, acting as a soluble dual-functional mediator enabling homogeneous operation in electrolytes, simplifies Li-S battery fabrication while demonstrating the commercial viability of molecularly engineered mobile active sites for stabilizing both electrodes in high-energy-density Li-S batteries.

Lithium metal batteries (LMBs) face critical challenges due to uncontrolled lithium dendrite growth and inhomogeneous Li+ flux, largely attributed to conventional separators' poor interfacial compatibility. To address this, we propose a hydrogen bond-driven layer-by-layer (LbL) assembly strategy for engineering functional separators using poly(vinyl alcohol) (PVA) and tannic acid (TA). The optimized PP/(TA/PVA)15 separator leverages the synergistic interplay between PVA's hydroxyl groups and TA's carbonyl moieties, forming a robust hydrogen-bonded network that simultaneously enhances lithiophilicity, regulates Li+ flux uniformity, and immobilizes anions. The interfacial design achieves exceptional electrochemical performance: Li//Li symmetric cells maintain stable operation for 800 h at 0.5 mA cm-2/0.5 mAh cm-2, while Li//LiFePO4 half cells retain 73.8% capacity after 1000 cycles at 5C (decay rate: 0.026% per cycle). The separator further exhibits high ionic conductivity (0.94 mS cm-1) and Li+ transference number (0.63), outperforming conventional polyolefin counterparts. By integrating simplicity, scalability, and eco-friendliness, this work pioneers a universal interface chemistry paradigm for next-generation LMBs, offering transformative insights into separator engineering through molecular-level hydrogen-bonding control.

In this work, an electrochemical sensing platform based on graphene@phosphotungstic acid nanocomposite (GR@PWA) was constructed for sensitive determination of acetaminophen (AP). The electrochemical performance of the obtained sensor (GR@PWA/GCE) was investigated by cyclic voltammetry, differential pulse voltammetry and electrochemical impedance spectroscopy. The calculated effective active area of GR@PWA/GCE was 2.22 times than that of bare glassy carbon electrode. Under the optimal conditions, a good linear relationship with AP concentration ranging from 1 μM to 100 μM and a lower limit of detection (0.305 μM) were obtained. The proposed sensing platform exhibited excellent anti-interference capability, repeatability, reproducibility and stability. Furthermore, the beef and lamb samples were employed to perform recovery test with a satisfactory recovery rate (88.0 %-107.6 %). The content of AP in pork and chicken samples was detected by the proposed sensor and high performance liquid chromatography. The results of the two methods were compared, and no significant difference was found (P > 0.05). This analysis strategy provides a basis for further expanding the application of electrochemical sensors in food safety detection.

To expand the application of zinc-air batteries (ZABs) and improve their efficiency, the development of highly active bifunctional oxygen electrocatalysts is of significant practical importance. An efficient bifunctional oxygen electrocatalyst (Fe/dZ8@Co/PDA) for the ORR/OER reaction is successfully prepared by an epitaxial growth method and a modulated bilayer ZIF8 strategy. Compared with the conventional catalyst with a monolayer ZIF8 structure, Fe/dZ8@Co/PDA contains an additional nitrogen source, forming and exposing more active centers. The Fe/dZ8@Co/PDA catalyst exhibits a half-wave potential of 0.85 V and an overpotential of 1.57 V under alkaline conditions. This high catalytic activity is attributed to the synergistic effect between the CoFe alloy and the M-NX active sites. Additionally, excellent methanol resistance and cycling stability are demonstrated. A high power density of up to 136.6 mW cm-2 and a specific capacity of 775.6 mA h gZn-1 were achieved by the assembled ZAB, which also maintained excellent cycling stability for over 170 h. Hierarchical porous hollow bilayer ZIF8-structured bifunctional oxygen electrocatalysts are constructed in this study, providing a new approach for the development of highly active electrocatalysts for the ORR/OER.

Lithium-sulfur (Li-S) batteries, with their high theoretical specific capacity and energy density, hold the promise of transforming energy storage. However, challenges such as polysulfide shuttling and lithium anode instability hinder their commercialization. This study introduces an innovative electrolyte additive, iron bromide dimethoxyethane (FeBr2DME), which catalyzes polysulfide conversion, enhances reaction kinetics, and stabilizes lithium deposition. In Li-Li symmetric cells, FeBr2DME enabled stable cycling for 1000 h at 1 mA cm(-2). Li-Cu cells maintained high coulombic efficiencies (similar to 99 %) over 200 cycles. Adding 0.5 mM FeBr2DME to the electrolyte resulted in a specific discharge capacity of 519.3 mAh g(-1) at 4C, with 90.3 % capacity retention after 100 cycles at 0.2C. Even with high sulfur loading (3.1 mg cm(-2)) and a low electrolyte/sulfur ratio (5 mu L mg(-1)), the batteries achieved a discharge specific capacity of 425.8 mAh g(-1) after 100 cycles at 0.2C, showcasing exceptional cycling stability. These findings highlight FeBr2DME's potential as a dual-function electrolyte additive, offering a viable solution to key challenges in Li-S batteries and paving the way for their commercial viability.

Key obstacles to commercializing lithium-rich manganese-based cathodes (LRMs) include voltage decline and capacity loss due to irreversible structural damage. The integration of structural design with surface modification to enhance structural stability represents the optimal choice for addressing these challenges. Here, an H+/Li+ exchange interface treatment and subsequent thermally driven process achieves external LiMgPO4 coating and internal gradient Mg doping of LRMs. The "pillars effect" achieved through Mg doping reduce the irreversible oxygen release and inhibits the migration of transition metals, and the LiMgPO4 coating layer mitigates interfacial reactions. As a result, the dual-form incorporation of Mg components, synergistically enhances the electrochemical performance of LRMs for Li-ion batteries. The modified sample exhibits an improved capacity retention from 68.8 % to 85.3 % after 250 cycles compared to the pristine LRMs, and demonstrates a high specific discharge capacity of 155.8mAh g-1 at 5C. This work provides a valuable new idea for improving the comprehensive electrochemical performance of LRMs through a synergistic integration strategy that encompasses both internal doping and external coating factors of Mg components.

The commercialization of lithium-sulfur (Li-S) batteries is hindered by challenges such as the polysulfide shuttle effect, sluggish conversion kinetics, and loss of active materials. Regarding the above issues, through a precisely controlled coprecipitation-hydrothermal-thermal treatment synthesis strategy, this study reports the first successful construction of ZnS-SnO2 (ZSSO) heterojunction cubes with well-defined porous surfaces and internal hollow structures, which were specifically employed as sulfur host materials. This structure not only integrates the advantages of the individual components but also generates a synergistic enhancement effect through the interfacial built-in electric field. Both theoretical calculations and operando spectroscopic analyses confirm that the heterointerface significantly outperforms every single component in mediating polysulfide conversion, achieving clear cooperative effects. By combining systematic operando characterizations with first-principles calculations, we establish a complete evidence chain linking microscopic electronic structures to macroscopic electrochemical behaviors, offering deep insights and theoretical guidance for the rational design of heterostructure materials. Based on this innovative design, the S@ZSSO cathode exhibits breakthroughs in key electrochemical performance metrics compared with relevant literature reports from the past year, especially in high-rate capability and cycling stability, highlighting its strong potential for practical applications. Experimental results show that the S@ZSSO cathode delivers an initial discharge capacity of 1343.7 mAh g-1 at 0.1C and maintains 603.9 mAh g-1 even at a high rate of 5C. It also demonstrates outstanding cycling stability, retaining 405.8 mAh g-1 after 800 cycles at 0.5C with an extremely low-capacity decay of only 0.063% per cycle. This work provides a simple yet effective host-material design strategy for high-performance Li-S batteries.

The conversion of biomass into high-value carbon materials presents significant opportunities for sustainable development in energy storage, catalysis, and environmental applications. Biomass, with its renewability and abundant carbon content, offers a valuable raw material source. This review focuses on the innovative use of molten salt-mediated thermochemical conversion (MSMTC) techniques, coupled with electrochemical approaches, to transform biomass into functional carbon materials. Molten salts serve as heat carriers, catalysts, and solvents, providing multiple benefits: high thermal efficiency, catalytic promotion, and customizable compositions for specific reactions. They also enable electro-deoxygenation and graphitization, improving the conductivity of biomass-derived carbon, while offering a sustainable and cleaner conversion process. Recent advances in MSMTC for producing graphite, carbon nanotubes, carbon nanosheets, graphene, carbon black, and porous carbon materials from biomass are comprehensively discussed. This review delves into the mechanisms, synthetic routes, and potential applications of MSMTC, highlighting its industrialization prospects and contribution to achieving a circular economy. By addressing the challenges and innovations in this field, the review aims to provide a thorough understanding of MSMTC's role in biomass valorization and its future potential.