Li-CO2 batteries utilizing greenhouse gas CO2 as feedstock offer high energy density and environmental benefits. However, the sluggish CO2 redox kinetics at cathodes lead to high overpotentials and low Coulombic efficiency, severely limiting practical applications. Here, the potential of Li-CO2 batteries is unlocked through a high-entropy alloy (HEA)-driven synergistic coupling strategy using a PtPdFeCoCuZn (PPFCCZ) catalyst (similar to 2.2 nm). The unique multi-element composition of the PPFCCZ catalyst creates an interfacial environment that enables ternary synergistic coupling among the interface metal, Li2CO3, and Li2C2O4, collectively stabilizing the amorphous Li2C2O4 formation pathway. This design achieves a record discharge voltage of 3.1 V with an ultralow overpotential (0.48 V) in Li-CO2 batteries. Additionally, it achieves a cycling lifespan exceeding 1000 h at a current density of 20 mu A cm-2, overcoming the conventional trade-off between voltage and reversibility. This work provides a paradigm for designing multi-functional HEA catalysts to manipulate reaction pathways in Li-CO2 batteries.

Lithium-lithium nitrate batteries are regarded as a promising high-capacity alternative to lithium-ion batteries due to their superior specific capacity, which is enabled by the unique dual role of LiNO3 as both lithium salt and active cathode material. However, their practical application is hindered by the unstable lithium anode interface and sluggish cathode kinetics, resulting in limited cycle life and safety concerns. Herein, this work presents a remote interfacial regulation engineering via nanoscale ZnPtFeCuNiCo High-entropy alloy (ZPFCNC-HEA) cathode catalyst. During the initial resting phase, this catalyst effectively decomposes LiNO3 in the electrolyte to directionally generate active nitrogen intermediates (LiNO2/LiNO). These intermediates spontaneously migrate to the anode interface, where they induce the in-situ formation of a Li3N-rich solid electrolyte interphase (SEI) during subsequent electrochemical cycling, achieving remote interfacial regulation. The resulting SEI significantly enhances interfacial stability and charge transfer efficiency. Combined with the exceptional catalytic activity of ZPFCNC-HEA toward the NO3-/NO2- redox reaction, the assembled Li-LiNO3 battery employing this cathode catalyst delivers a remarkable specific capacity of 15019 mAh g-1 and maintains stable operation for over 700 cycles. Furthermore, an Ah-level pouch cell (1.522 Ah) is demonstrated, validating a novel remote interfacial regulation of SEI strategy for practical high-energy batteries.

The development of aqueous zinc-ion batteries (AZIBs) is constrained by challenges including cathode dissolution, structural instability, and sluggish Zn2* diffusion. Vanadium oxides (VO), though promising due to their layered structure and high specific capacity, suffer from low conductivity and interfacial instability. This work introduces a rational surface-coating strategy using poly(3,4-ethylenedioxythiophene) (PEDOT) to overcome these limitations. DFT calculations reveal that PEDOT lowers Zn2* adsorption energy, mitigates electrostatic interactions, and induces an interfacial built-in electric field that enhances carrier density and mobility. Guided by these insights, VO was synthesized hydrothermally and uniformly coated with PEDOT via in situ polymerization, yielding VO-PEDOT composites (PVOs) with tunable coating levels. Structural characterizations confirm the formation of a continuous conductive network, while electrochemical tests reveal significantly improved performance. The optimized PVO-200 delivers an initial discharge capacity of 327.3 mAh g-1 with 92 % retention after 70 cycles at 0.2 A g-1 , and maintains 207.7 mAh g-1 after 2000 cycles at 5 A g-1 , demonstrating excellent rate capability and long-term stability. These findings underscore that PEDOT coating enhances conductivity, structural integrity while accelerating Zn2* transport via interfacial modulation. This work strategy a scalable route to high-performance vanadium-based cathodes and provides valuable guidance for interfacial engineering in future AZIBs.

Hydrophobic silica aerogels are widely used as thermal-insulation materials, but the thermal decomposition of their organic surface groups may affect their stability and safety during high-temperature service. In this study, ambient-pressure-dried silica aerogels modified with trimethylsilyl, dimethylsilyl, and methylsilyl groups were prepared and denoted as TSA, DSA, and MSA, respectively, to clarify how the degree of methyl substitution in the surface modifier controls the pyrolysis behavior of hydrophobic silica aerogels. Thermogravimetric analysis at different heating rates was combined with TG-FTIR, a model-free kinetic analysis, a model-fitting analysis and thermodynamic calculation. With decreasing methyl substitution from TSA to MSA, the aerogel framework became denser, the specific surface area decreased, and the contribution of solid-phase heat transfer increased slightly. The main pyrolysis process occurred at 250-800 °C and involved multiple overlapping reactions. The average activation energies of TSA, DSA, and MSA were 241.4, 246.6, and 285.5 kJ/mol according to the Kissinger-Akahira-Sunose (KAS) method and 243.0, 248.2, and 289.0 kJ/mol according to the Flynn-Wall-Ozawa (FWO) method, respectively. The higher activation energy of MSA indicates that the more condensed silica-rich framework and lower organic methyl content improves its resistance to the main degradation process. The model-fitting analysis further suggested an A1/2 mechanism for TSA and A2/5 mechanisms for DSA and MSA. TG-FTIR further confirmed the evolution of CO2, H2O, CH4, and C2H4 and revealed distinct gas-release behaviors among the three samples. These results demonstrate that the surface methyl-substitution structure governs the balance between hydrophobic modification, pore-structure preservation, pyrolysis resistance, and volatile-product release, providing a basis for selecting surface modifiers for thermally stable silica-aerogel insulation materials under oxygen-limited high-temperature conditions.

Amid the global transition toward clean and sustainable energy systems, the development of cost-effective and resource-abundant energy storage technologies has become increasingly critical. Sodium-ion batteries have emerged as a highly promising candidate due to their material availability and competitive performance. Nevertheless, the practical application of layered oxide cathode materials in these batteries is hindered by mechanical stress accumulation during cycling, which leads to structural degradation, capacity fade, and ultimately battery failure. This review systematically summarizes recent advances in stress engineering strategies aimed at mitigating these challenges. It begins by elucidating the fundamental mechanisms of stress generation associated with sodium ion intercalation and deintercalation processes. The article then provides a comprehensive analysis of various innovative approaches designed to manage stress, including microstructural optimization, surface and interface engineering, and composite material design. Furthermore, it discusses the correlation between atomic-scale lattice strain and macroscopic electrochemical behavior, offering deep insights into failure mechanisms. By integrating theoretical understanding with experimental progress, this review aims to provide valuable guidance for the rational design of durable and high-performance cathode materials, thereby supporting the broader effort to develop reliable sodium-based energy storage systems.

Aqueous zinc‑iodine batteries (AZIBs) utilizing the four-electron (4e-) redox reaction (I-/I0/I+) offer impressive theoretical capacities; however, their practical application is severely impeded by the rapid hydrolysis of electrophilic I+ species and uncontrolled Zn dendrite growth. Herein, a novel hybrid electrolyte is engineered by integrating 1-ethyl-3-methylimidazolium chloride (EMIMCl) and ethylene glycol (EG) into the ZnSO₄ aqueous system (denoted as ZEM 1-40) to fundamentally address these challenges. The combination of EMIMCl and EG in the system creates a new structure which blocks water molecules from entering the Zn2+ ion environment thus preventing I+ from breaking down into I₃- byproducts. The EMIM+ cations at the Zn interface create an electrostatic shield which protects the interface by controlling Zn2+ ion movement to achieve uniform deposition and prevent dendrite formation. The ZEM 1-40-based cell enables a 4e- transfer reaction which becomes reversible to achieve 455.76 mAh g-1 at 1 A g-1. Furthermore, the system demonstrates exceptional long-term durability, sustaining over 14,300 cycles at 10 A g-1 with an ultralow capacity decay rate of 0.0047% per cycle and a near-unity Coulombic efficiency (99.79%). The research establishes a deep comprehension of solvation chemistry mechanisms which enable the stabilization of high-valence iodine species for developing high-energy-density aqueous batteries.

Aqueous zinc–iodine (Zn–I2) batteries are promising for safe and cost-effective energy storage, but their durability is limited by nonuniform Zn deposition at the anode and polyiodide shuttling from the cathode. Here, mycelium-leather alternative waste (MLAW) was converted by chitinase-assisted hydrolysis into a chitin-oligosaccharide-rich (COS-rich) hydrolysate and immobilized on a commercial glass-fiber (GF) scaffold to form an organic–inorganic hybrid separator. The resulting CMLW-500/GF interphase combines a densified transport pathway with abundant hydroxyl, amino, and acetamido groups. Spectroscopic and morphological analyses indicate that these functionalities promote polyiodide retention and provide coordination sites for regulating hydrated Zn2+ transport. Accordingly, the modified separator suppresses rough Zn deposition and decreases the interfacial charge-transfer resistance from 135.1 to 50.9 Ω. Kinetic analysis indicates rapid interfacial Faradaic conversion of confined polyiodide species. Zn–I2 cells using CMLW-500/GF retain 99.0% of their capacity after 3000 cycles at 1 A g−1 and operate for 11,000 cycles at 5 A g−1 while maintaining a capacity of approximately 160 mAh g−1 and nearly 100% Coulombic efficiency. This work demonstrates a practical route for converting fungal-material waste into a multifunctional separator interphase that concurrently mitigates Zn-anode instability and polyiodide crossover.

Lithium iron phosphate (LiFePO4) is a promising cathode material for lithium-ion batteries (LIBs), but its low conductivity and poor rate performance limit its application in high-power devices. In this study, we employed a particle size grading strategy to enhance the electrochemical performance of LiFePO4. By mixing small and large particles in different ratios (3:1, 2:1, 1:1, 1:2, and 1:3), we synthesized graded iron phosphate precursors, which were then used to prepare LiFePO4 cathode materials. The effects of particle size distribution on the material’s structural properties and electrochemical performance were systematically investigated. SEM images revealed that the morphology of LiFePO4 changed with varying precursor ratios, with the 3:1 ratio resulting in a more uniform particle distribution. The results showed that the 3:1 ratio exhibited the highest discharge capacity of 159.4 mAh/g, while larger particle ratios (2:1 and 1:1) led to decreased capacity due to the increased proportion of larger particles. Additionally, the LiFePO4 materials prepared from non-in situ mixed precursors exhibited higher tap densities, with the 2:1 ratio achieving the highest tap density of 2.545 g/cm3. This study demonstrates the effectiveness of the particle size grading approach in improving the electrochemical properties of LiFePO4 and provides insights into the design of high-performance cathode materials for advanced lithium-ion batteries.

This study investigates the effects of different titanium doping concentrations on the properties of iron phosphate precursors and the final lithium iron phosphate (LiFePO4) materials, aiming to optimize the structural and electrochemical performance of LiFePO4 by introducing titanium during the precursor synthesis stage. Titanium was introduced using titanate as a titanium source to prepare iron phosphate precursors with varying titanium concentrations. The materials were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), and other techniques. The results showed that titanium incorporation significantly influenced the Fe and P content in the precursors, with a decrease in both Fe and P levels as the titanium doping concentration increased. Moreover, as the titanium content increased, the particle size of the precursor decreased, and the particle distribution became more uniform. Additionally, titanium doping improved the tap density of the precursors, with a significant increase in tap density observed when the titanium content reached 4000 ppm. Electrochemical measurements revealed that titanium doping had a certain impact on the discharge capacity of LiFePO4, with the discharge capacity gradually decreasing as the titanium content increased. Overall, this study effectively improved the physical properties of LiFePO4 materials by introducing titanium during the precursor synthesis stage, providing a theoretical foundation for further optimization of titanium-doped LiFePO4.

The effective recovery of valuable materials from spent LiFePO4 batteries is crucial for resource sustainability and environmental protection. This study investigates the recovery of phosphorus iron slag from waste LiFePO4 batteries, focusing on dissolution and impurity removal processes to produce battery-grade iron phosphate. Using high-temperature-activated dissolution, followed by precipitation/dissolution for impurity removal, we optimize conditions to ensure high recovery rates (up to 98.8% for FePO4 under optimized conditions) and product purity. Our findings demonstrate that the proposed method effectively transforms waste slag into valuable iron phosphate, significantly reducing raw material costs and contributing to sustainable battery recycling practices. The regenerated LiFePO4 cathode exhibits excellent electrochemical performance, achieving a discharge capacity of 160.7 mAh g−1 at 0.1 C, which meets market standard levels. This research provides a solid foundation for enhancing resource utilization and advancing circular economy principles in the battery industry.

Despite the advantages of aqueous zinc-ion batteries (AZIBs), such as high specific capacity and inherent safety, zinc metal as the anode undergoes dendrite growth and severe corrosion during battery cycling. This study reports the use of glutarimide (Glu) as an electrolyte additive, which occupies the dense region of the Zn-electrolyte electric double layer (EDL), protecting the Zn surface from parasitic corrosion in aqueous electrolytes. Spectroscopic, theoretical calculations, and electrochemical analyses collectively demonstrate that the preferential adsorption of the additive at the zinc interface results in the restructuring of the EDL. This restructuring creates an H2O-poor inner Helmholtz surface that inhibits parasitic reactions, accelerates interfacial dynamics, and promotes uniform zinc deposition. As a result, the Coulombic efficiency (CE) improves from 98.74% in ZnSO4 (ZSO) electrolyte to 99.53% in ZSO/Glu electrolyte. The Zn symmetric cell achieves stable cycling performance of 6275 h at 1 mA cm-2 and 3460 h at 5 mA cm-2, surpassing the performance of ZSO (290 h, 240 h). Additionally, Glu demonstrates excellent long-term cycling stability and rate performance in Zn//CaVO full cells, confirming its feasibility. This work highlights the innovative application of Glu as a protective additive to enhance the stability and performance of AZIBs.

The development of efficient and reliable acidic oxygen evolution reaction (OER) electrocatalysts represents a crucial step in the process of water electrolysis. RuO2, a benchmark OER catalyst, suffers from limited large-scale applicability due to its tendency toward the less stable lattice oxygen mechanism (LOM). This work reports the synthesis of Co-doped RuO2 nanosheets with a unique porous morphology composed of interconnected grains via a facile molten salt method. Co doping modulates the grain size, effectively increasing the specific surface area and introducing oxygen vacancies. These oxygen vacancies, coupled with the Co dopants, form Co-O(V) motifs that tune the electronic configuration of Ru. This structural engineering promotes a shift in the OER mechanism from the detrimental LOM pathway to the more efficient adsorbate evolution mechanism (AEM), significantly enhancing the stability of the RuO2 matrix in acidic environments. The optimized Co0.108-RuO2 catalyst exhibits a low overpotential of 214 mV at 10 mA cm-2 and remarkable stability over commercial RuO2 and undoped counterparts, owing to the synergistic effect of the increased surface area, Co-O(V) motifs, and favored AEM pathway. This strategy of utilizing Co doping to engineer morphology, electronic structure, and reaction mechanism offers a promising avenue for developing high-performance OER electrocatalysts.

Manganese oxides are widely recognized as promising cathode materials for aqueous zinc-ion batteries (AZIBs) due to their low cost and high theoretical capacity. However, their practical performance is often limited by challenges such as poor conductivity and manganese dissolution during charge/discharge cycles, leading to structural degradation. In this study, a novel strategy is proposed to enhance the electrochemical performance of NiMn2O4 by incorporating additional Mn2 + into its structure. This modification expands the lattice spacing, improves the conductivity, and stabilizes the overall structure. The increased Mn2+ concentration also generates additional redox-active sites, thereby significantly enhancing the electrochemical performance of the material. The modified NiMn2O4 (NMO-1) cathode demonstrates a high specific capacity of 260 mAh g- 1 at a current density of 0.5 A g-1, excellent rate capability, and long-term cycling stability, retaining 120.7 mAh g- 1 after 1800 cycles at 1 A g-1. This approach provides valuable insights into optimizing manganese-based cathodes for AZIBs and offers a promising strategy for improving their electrochemical performance.

The exploration of nanoscale high-entropy intermetallic compounds (HEICs) represents a transformative frontier in materials science, particularly in catalysis. The unique combination of multi-element composition, long-range atomic ordering, and nanoscale dimensions endows HEICs with superior electronic, structural, and catalytic properties that surpass those of traditional metal catalysts. However, achieving both uniform multi-element mixing and long-range ordered structures at the nanoscale is challenging. Building on this, this review highlights the key role of configurational entropy, mixing enthalpy, elemental composition, and size effects in the stable formation of nanoscale HEICs through thermodynamic and kinetic analysis. The latest advancements and existing challenges in the design, synthesis, structure, and applications of HEIC catalysts are discussed, with a focus on exploring their synthesis–structure–performance relationships from multiple perspectives. We hope that this review will offer valuable insights for further exploration and development of HEICs in catalytic applications.

Polyaniline (PANI) is currently one of the most extensively studied conductive polymers in the field of flexible gas sensors. However, sensors based on pure PANI generally suffer from problems such as low sensitivity and poor stability. To address these issues, in this work, a room-temperature hydrogen sulfide gas sensor of polyaniline/tungsten oxide/copper oxide (PANI/WO3/CuO) was synthesized using in situ polymerization technology. This gas sensor displays a response value of 31.3% to 1 ppm hydrogen sulfide at room temperature, with a response/recovery time of 353/4958 s and a detection limit of 100 ppb. Such an excellent performance is attributed to the high surface area and large adsorption capacity of the ternary composite, as well as the multi-phase interface synergistic effect.

Iridium oxides (IrOx) are benchmark catalysts for the acidic oxygen evolution reaction, but their performance is often constrained by a trade-off between catalytic activity and long-term stability. Herein, we utilize an amorphous IrOx matrix as a robust scaffold for synergistic ruthenium (Ru) doping, a strategy designed to enhance catalytic activity while maintaining an exceptional stability. A simple nitrate-assisted synthesis produces ultrathin Ru-doped amorphous IrOx nanosheets (2.36 nm thick) with a significantly enhanced specific surface area. Combined spectroscopic analysis and density functional theory calculations reveal that atomically dispersed Ru dopants induce charge transfer to adjacent Ir sites, which optimizes the Ir d-band electronic structure. This electronic modulation not only lowers the energy barrier for the rate-determining *O to *OOH transformation but also critically ensures the reaction proceeds via the stable adsorbate evolution mechanism while suppressing the degradative lattice oxygen mechanism. Benefiting from the above advantages, the optimized Ru0.0738-IrOx catalyst exhibits excellent catalytic activity, achieving 10 mA cm-2 at a low overpotential of 225 mV with outstanding stability for over 100 h, far surpassing commercial IrO2 and RuO2. This study highlights a synergistic doping strategy within an amorphous matrix to overcome the intrinsic performance limitations of iridium-based oxides for robust oxygen evolution.

This study investigates the impact of Ca2+ and phytic acid (PA) pre-insertion on the performance of vanadium oxide (V6O13) as a cathode material for aqueous zinc-ion batteries. Ab initio molecular dynamics (AIMD) simulations reveal that the diffusion coefficient of Ca2⁺ is higher than that of Zn2+, leading to the preferential extraction of Ca2⁺. The extracted Ca2⁺ readily forms a dense cathode-electrolyte interphase (CEI) with SO₄2 - on the electrode surface, effectively mitigating electrode dissolution. Furthermore, density functional theory (DFT) calculations indicate that the incorporation of Ca2⁺ lowers the diffusion energy barrier for Zn2⁺, facilitating its diffusion. Additionally, PA insertion stabilizes the interlayer spacing of V6O13, and its strong chelating ability stabilizes the structure by preventing collapse during cycling. Experimental validation through a one-step solvothermal method confirms these theoretical predictions. The CaVO-PA composite exhibits excellent cycling stability, with a capacity retention rate increasing from 60% to 102% after 3000 cycles at 10 A g-¹. Even at 20 A g-¹, it delivers a specific capacity of 170.2 mAh g-¹ with stable Coulombic efficiency. After 10 000 cycles, the capacity shows no significant degradation, demonstrating superior cycling stability and high current tolerance, thereby confirming the effectiveness of the CEI and PA in enhancing electrochemical performance.

Developing cost‐effective and highly efficient oxygen evolution reaction (OER) electrocatalysts that operate in both acidic and alkaline media is crucial for industrial electrocatalytic water splitting. However, achieving high performance under dual pH conditions remains a significant challenge. Herein, we report the synthesis of multi‐sized RuO 2 sub‐nanoclusters on Co 3 O 4 nanoarrays via a facile method, which demonstrates exceptional OER activity in both acidic and alkaline environments. The optimized catalyst exhibits remarkably low overpotentials of 165 mV in 0.5 M H 2 SO 4 and 223 mV in 1 M KOH at a current density of 10 mA cm −2 , respectively. Additionally, it exhibits outstanding stability, maintaining performance over a 10‐h continuous operation, which is attributed to the robust structural stability of the dispersed RuO 2 sub‐nanocluster morphology. Atomic‐scale investigations reveal a layer‐by‐layer growth mechanism of Ru on the Co 3 O 4 substrate, transitioning from single atoms to monolayer clusters and ultimately to sub‐nanoclusters as Ru loading increases. This growth mechanism provides a rational strategy for the precise design and synthesis of advanced cluster‐based catalysts. Density functional theory (DFT) calculations further elucidate the strong oxide‐support interactions between RuO 2 clusters and the Co 3 O 4 matrix, facilitating electron transfer from RuO 2 to Co 3 O 4 and generating an electron‐deficient region. This electronic modulation enhances –OH adsorption and accelerates OER kinetics. These findings underscore the potential of metal sub‐nanoclusters for designing highly efficient and durable electrocatalysts for water electrolysis. image

Endogenous T cell activation relies on recognizing tumor-specific antigens. However, tumor cells often alter phenotypes to evade immune surveillance, resulting in immune escape and drug resistance. Photodynamic therapy (PDT) activates anti-tumor immune responses by generating reactive oxygen species, which induce endoplasmic reticulum stress and immunogenic cell death. The clinical application of PDT is limited by immunosuppressive tumor microenvironment. Notably, enhancer of zeste homolog 2 (EZH2) regulates expression of immune-related genes in tumor and immune cells through H3K27 methylation. Consequently, targeting EZH2-mediated epigenetic silence provides an effective strategy to enhance the anti-tumor immune effect of PDT. In this study, a nano-delivery system (NP2) is designed to demonstrate PDT and epigenetic reprogramming effects. NP2 can reverse epigenetic silence, enhance MHC-I expression, and induce release of CXCL9-10 via EZH2i. Meanwhile, NP2 has a significant effect on PDT, inducing endoplasmic reticulum stress that resulted in immunogenic cell death and subsequent activation of the immune cascade. In a mouse model of in situ breast cancer, the combination of PDT activation and epigenetic reprogramming through EZH2i showed synergistic effects on remolding, and triggering a robust anti-tumor immune response in vivo. This study provides a novel idea for improving the immunosuppressive environment in clinical individualized immunotherapy. Oxidative stimuli in tumor environment caused P1 and tazemetostat (TAZ) to be released from NP2. TAZ reduced methylation of histones by inhibiting enhancer of zeste homolog 2 (EZH2), which reverse epigenetic silence and upon an 808 nm laser irradiation, P1 generates reactive oxygen species to eradicate tumor cells and activates effector T cells, thereby triggering synergistic antitumor immunity. image