The oxygen evolution reaction (OER) is crucial for renewable energy systems, such as water splitting and metal air batteries. However, the slow kinetics of OER significantly limits the overall energy conversion efficiency, necessitating effective catalysts. The multielement transition metal oxides offer a promising alternative compared to precious metal oxides, yet their composition optimization remains challenging due to the vastness of the combinatorial space. Traditional trial-and-error approaches are labor-intensive and inefficient. To address this challenge, we develop an innovative automated platform integrating machine learning (ML) with Bayesian optimization for rapid and cost-effective synthesis and evaluation of electrocatalysts. This platform allows the automation of the entire experimental process, from synthesis to evaluation, enabling real-time feedback and guiding subsequent experiments. In a continuous operation of 32 h, the platform conducted 96 experiments to optimize the composition of (Ni-Fe-Co-Mn-Mo)Ox , resulting in an electrocatalyst with an overpotential of 231 mV at 10 mA/cm 2. This automated approach significantly reduces manual intervention and enhances efficiency, proving to be a valuable tool for optimizing materials in complex, multidimensional spaces. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

Lithium-rich layered oxide cathodes, Li1.2Ni0.13Co0.13Mn0.54O2 (LNCM), owing to their ultrahigh capacity (>250 mAh/g), have emerged as prime candidates for the next-generation high-energy-density lithium-ion batteries. However, severe interfacial side reactions and structural degradation result in pronounced capacity fading and voltage decay, substantially hindering their practical deployment. Here, we prepare nanosized single-crystal LNCM via the molten salt method, which delivers high capacity and enhanced electrochemical activity owing to its exposed high-energy surfaces, but suffers from rapid performance degradation. To address this issue, an ultrathin TiO₂ layer is controllably deposited on the nanosized LNCM by atomic layer deposition (ALD), effectively passivating the unstable high-energy surface and mitigating interfacial degradation. The modified LNCM exhibits improved electrochemical performance, with the initial coulombic efficiency increased from 78 % to 88 % and the capacity retentions raised from 57 % to 82 % at 0.5 C and 47 % to 83 % at 1 C after 200 cycles. This work not only offers an effective remedy for LNCM interfacial failure but also elucidates the pivotal role of high-energy interfacial engineering in the electrode material.

Rechargeable hydrogen gas batteries show a great promise for large-scale energy storage due to their high safety, environmental friendliness, high efficiency and long-cycle life. However, the costly catalysts at the anode for hydrogen oxidation/evolution reactions (HOR/HER) hinder the practicability. Here, we report a pseudo-single-crystal mesoporous (PSCM) PtPd catalyst with high HOR/HER bifunctional activities for high-performance hydrogen gas batteries. It exhibits an outstanding HOR activity with a kinetic current density of 3.10 A mg-1 and an HER overpotential of 34.8 mV at 10 mA cm-2, outperforming commercial Pt/C (0.42 A mg-1, 79.3 mV). When assembling Ni-H2 battery with a low PSCM-PtPd catalyst loading of ∼45 µg cm-2, it displays a high energy efficiency of ∼85% and cycling stability of >1000 cycles. Even at an ultra-low catalyst loading of ∼10 µg cm-2, the Ni-H2 (PSCM-PtPd) battery still exhibits an energy density of ~135 Wh kg-1 and durability of >1000 cycles with a cell cost of ~105 $ kWh-1, much better than that of Pt/C-based battery (>700 $ kWh-1). We demonstrate that the superior activity of the PSCM-PtPd catalyst originates from the charge transfer from Pd to Pt and lattice distortion caused by Pd incorporation, and the enhanced stability is attributed to its fewer grain boundaries and stable attachment to the electrode. This work offers a promising pathway toward designing cost-effective and scalable energy storage systems.

Developing highly efficient catalysts is crucial for Li-CO2 batteries to achieve superior performance, offering significant benefits of CO2 utilization and energy conversion. However, accurately elucidating the structure-activity relationships of catalysts under operating conditions remains a major challenge. The limited understanding derived solely from catalysts' pristine states hinders the rational optimization of catalytic systems. Here, by monitoring the structural reconstruction and the evolving Co ligand environments in CoX (X = O, S, and Se) precatalysts during operation, we establish the structure-activity relationship and reveal the regulatory role of precatalyst covalency in governing the catalytic activity and stability of Li-CO2 batteries. We found that the reconstruction behavior of the catalysts is fundamentally determined by the catalysts' covalency, which governs the oxidation thermodynamics that ultimately drive the structural evolution. CoS, with the weakest covalency, suffers from detrimental complete reconstruction, transforming into a fully oxidized phase CoO during cycling, ultimately resulting in the rapid failure of polarization voltage exceeding 2 V after 200 h of cycling. In contrast, CoSe, with stronger covalency, undergoes confined partial reconstruction to form a CoSe/CoO heterophase interface on the local surface, which protects active sites and facilitates electron transfer. This partial reconstruction strategy successfully breaks the activity-stability trade-off. The CoSe-based battery demonstrates both high activity and stability, maintaining a polarization voltage of 0.96 V with an energy efficiency exceeding 80% after 736 h of continuous cycling. This work reveals the structure-activity correlations dominated by covalency in Li-CO2 batteries and provides insights into designing durable and high-efficiency catalysts by inducing partial reconstruction.

Li-rich layered oxides (LLOs) cathodes exhibit high specific capacities (>250 mAhg(-1)), yet their practical application is hindered by inherent structural instability and low ionic conductivity. This study proposes a trace dual-metal doping strategy (0.2 wt% Zr and 0.1 wt% Al) to enhance the structural stability and Li (+) transport efficiency of Li1.2Ni0.16Co0.16Mn0.48O2. Combined in-situ X-ray diffractions and density functional theory calculations reveal that Zr4+ and Al3+ doping at 3b sites suppresses lattice expansion along the c-axis (Delta c reduced by 6.9 %) and strengthens the metal-oxygen bond, thereby mitigating Li/Ni cation mixing and oxygen loss during cycling. The optimized Al@0.10 sample achieves a capacity retention of 80.8 % after 500 cycles at 9.5 mg cm(-2) loading, with a total discharge voltage decay of 0.78 V after 500 cycles. Additionally, it delivers a high-rate capacity of 136 mAhg(-1) at 5C. This work provides new insights into synergistically optimizing structural stability while maintaining electrochemical performance through dual-metal doping.

Breakthroughs in high-capacity anodes represent a critical frontier in the development of next-generation high-specific-energy storage systems. However, the current high-capacity anodes of lithium batteries are confronted with numerous challenges, including uncontrolled volume expansion, lithium dendrite growth, dead lithium, and unstable solid electrolyte interphase (SEI) films. Herein, we firstly employ laser engraving technology to fabricate an ultra-light freestanding graphene film with through-hole array and defect-rich edges, which serves as a lithium-free anode that integrates lithium-ion intercalation and metallic lithium deposition. During discharge, the defect structures at the pore edges facilitate the adsorption of lithium ions and their rapid intercalation between graphene layers, forming the LiCx framework. This enables the conversion of quasi-dead lithium through the solid-state pathway of Li-LiCx-Li+. Simultaneously, the vertically aligned through-holes homogenize ion flux and promote metallic lithium storage within the pores, thereby achieving high areal capacity, excellent reversibility, dendrite-free growth, and minimal volume change. As a result, this ultra-light freestanding lithium-free graphene anode (FLFGA) achieves highly reversible Li storage with 99.9% Coulombic efficiency (CE) over 1300 cycles and dendrite-free plating/stripping at a high areal capacity of 4 mAh & centerdot;cm-2 (1350 mAh & centerdot;g-1 anode). When paired with a high-loading LiFePO4 (LFP) cathode (11.5 mg & centerdot;cm-2), the FLFGA||LFP full cell exhibits significantly enhanced cycling stability (500 cycles), outperforming most conventional Li metal battery, lean-Li battery, and anode-free Li battery systems. This work demonstrates a viable lithium-free anode strategy via laser-engraved graphene engineering, paving the way for durable, safe, and high-energy-density Li batteries.

ABSTRACT Solid polymer electrolytes (SPEs) show great promise for solid‐state lithium metal batteries but face challenges due to inherently slow ion transport and interfacial instability. In this work, we propose a dipole‐matching strategy to engineer an SPE with a compact microstructure and stabilized interfaces. Through combined theoretical and experimental studies, we identify a molecular additive, such as 3,5‐bis(trifluoromethyl)benzoic acid (N‐CFF), that promotes rapid and uniform nucleation and directs phase alignment via dipole interactions with polymer chains, resulting in a compact microstructure conducive to rapid lithium‐ion transport and homogeneous deposition. Simultaneously, the dipole‐matched N‐CFF creates an electron‐rich environment that facilitates the formation of a LiF‐rich solid electrolyte interphase, effectively suppressing lithium dendrite growth. Employing this strategy, we fabricate Li||LiFePO 4 solid‐state batteries that deliver ultra‐long cycle life (90% capacity retention after 3000 cycles), exceptional low‐temperature and rate performance, as well as improved thermal safety. This work offers a comprehensive interface and microstructure co‐design approach to promote the development and application of high‐performance solid‐state batteries.

Solid polymer electrolytes (SPEs) are promising for use in high-energy-density solid-state Li metal batteries. However, their practical application is hindered by challenges including poor mechanical strength, inadequate thermal stability, electrode-interface instability, and sluggish ionic transport, which collectively fall short of the required safety and performance standards. Here, we develop an organic-inorganic interwoven architecture using PBO nanofiber and MXene nanosheets as a multifunctional host for SPE. This interwoven framework enhances the mechanical strength and toughness of the solid electrolyte by 12.5- and 7-fold, respectively, and reduces thermal shrinkage below 10% at 200°C. More importantly, we demonstrate that the interwoven structure promotes Li salt dissociation through strong local electric-field polarization, accelerates Li-ion transport (0.75 mS cm-1), and enhances the stability (8000 h without short-circuiting) of the Li metal interface during battery operation while suppressing exothermic side reactions under extreme thermal runaway conditions. Using this strategy, solid-state Li metal pouch cells operate stably under mechanical and thermal abuse conditions, delivering 91.7% capacity retention after 300 cycles at 10C and 90°C. This work effectively addresses the interrelated challenges of mechanical strength, ion transport, and interface/thermal stability of SPE, offering a promising strategy for safe and high-performance solid-state Li metal batteries.

Infected wounds are difficult to treat due to biofilm formation, drug-resistant bacteria, and inefficient localized therapy. To address these challenges, we developed a core-shell microneedle (MN) patch that enables sequential delivery of copper peroxide (CuO2) nanoparticles and vascular endothelial growth factor (VEGF) for synergistic healing. CuO2 was encapsulated in zeolitic imidazolate framework-8 (CuO2@ZIF-8) to improve the aqueous stability and regulate reactive oxygen species (ROS) generation. The antibacterial nanocomposite was loaded into a pH-sensitive hyaluronic acid (HA) core layer for rapid release under a weakly acidic wound microenvironment, while VEGF was incorporated into a gelatin methacryloyl (GelMA) shell for sustained delivery. Upon application, the core dissolves to release Cu2+, Zn2+, and ROS, disrupting biofilms and killing bacteria. Subsequently, the shell swells and degrades to release VEGF, promoting angiogenesis and tissue regeneration. In a Staphylococcus aureus-infected wound model, the MN patch demonstrated potent antibacterial activity, enhanced neovascularization, and accelerated healing. This programmable, dual-functional MN platform offers an effective strategy for treating infected wounds by integrating infection control with tissue regeneration in a temporally coordinated manner.

Lithium-sulfur (Li-S) batteries have attracted significant attention due to their high energy density and low cost of raw materials. Although the SPAN cathode has better electrochemical performance than the traditional S8/C composite, it is far from meeting the needs of commercialization, and its energy density, cycle stability, and rate performance need to be further improved. In this study, the swelling and dispersion of SPAN in different solvents are investigated for the first time by using different binders to optimize the electrode structure. The selection of water as a solvent can reduce the swelling of SPAN and inhibit cracking in the electrode preparation process, which effectively improves the structural stability of the electrode during the long-time charging and discharging process. The combination of CMC&SBR binder can reduce the agglomeration of active material and conductive carbon and contribute to the capacity of SPAN at a high current rate. As a result, the non-swelling SPAN with CMC&SBR binder exhibits a stable long cycling performance (83% capacity retention for 200 cycles at 1 C) and high rate performance (1192 mAh g-1 at 5 C). In particular, the Li-S pouch cell is able to cycle stably for more than 50 cycles at 0.2 C under high loading (SPAN loading level of 7.2 mg cm-2 and area capacity over 4 mAh cm-2) with the specific capacity maintained at 1306 mAh g-1. This work has the potential to promote the commercialization of Li-SPAN batteries.

Mechanical metamaterials (MMs) have garnered significant attention in recent years owing to their extraordinary mechanical properties that cannot be found in natural materials. As a distinctive class of MMs, graphene origami-enabled auxetic metamaterials (GOEAMs) offer unique advantages over traditional MMs and possess materials properties that are independent of complicated architecture or topology. Since its concept was first proposed in 2021, this emerging field has quickly attracted the attention from many researchers who have carried out extensive studies on the design and analysis of various GOEAM structures. This paper aims to provide a comprehensive review and systematic discussion on the state-of-the-art in this emerging field, beginning with a brief introduction of origami as well as the mechanical and physical properties of graphene and graphene origami (GOri). Subsequently, the modelling framework of GOEAMs and the commonly employed approaches for predicting their effective material properties are reviewed. This is followed by detailed discussions on the structural responses, including bending, buckling, postbuckling and free vibration of various GOEAM structures under different loading conditions. The article also identifies current challenges and future research directions, offering valuable insights into the future development and practical engineering applications of GOEAM based structures.

Cobalt-free LiNi0.5Mn1.5O4 (LNMO) is a highly competitive spinel cathode material due to the Ni2+/4+ redox couple, which alleviates Jahn-Teller distortion and offers a high redox potential near 5 V. However, its limited cycling life remains a major obstacle to large-scale application, primarily due to severe interfacial instability. Here, we identify chemical inhomogeneity as a limiting factor contributing to this instability, which leads to increased oxygen vacancies and rock-salt phase formation on the particle surface, resulting in poor cycling stability. In contrast, we demonstrate that chemically homogeneous LNMO (CH-LNMO), synthesized via a polyvinylpyrrolidone (PVP)-assisted solid-state method, exhibits a uniform Ni/Mn distribution and improved interfacial stability, which achieves excellent cycling performance, with a capacity retention of 90.32 % after 1000 cycles at 2C. We further reveal that chemical homogeneity enhances Ni/Mn ordering in the structure and decreases the Jahn-Teller effect of Mn3+, thereby mitigating interfacial reactions and transition metal ion dissolution. This work underscores the critical role of chemical homogeneity in large-scale synthesis and provides a viable approach for improving the long-term cycling stability of cathode materials.

Lithium-carbon dioxide (Li-CO2) batteries provide an extremely feasible strategy for sustainable development and carbon neutrality. However, due to the sluggish kinetics and complex interfacial reactions, Li-CO2 batteries are limited by low output voltage and poor cycling stability. Developing efficient and durable catalysts remains an urgent challenge. Transition metal oxides have gained significant attention owing to their availability and stability for electrocatalytic reactions, but their catalytic activity remains unsatisfactory toward Li-CO2 batteries. Herein, this work proposes an asymmetric Fe/Cu-incorporated Co3O4 tactic system to tune charge distribution for motivating efficient electrocatalysis and decipher the mechanism of asymmetric structure modulation on the promotion of catalytic activity and stability. It is unraveled that d-orbital spin splitting induces the modification of nondegenerate state, which enhances catalyst durability, while simultaneously increasing electron occupancy in dxz / yz orbitals. This higher electron occupancy facilitates the hybridization with the p orbitals of reactants and intermediates via π bonding, thereby strengthening the adsorption activity. In consequence, the Li-CO2 battery with Cu-Co3O4 cathode demonstrates a low overpotential of 0.73 V and high Coulombic efficiency of 96%, outperforming batteries with Co3O4 and Fe-Co3O4. This work offers a unique insight for electronic structure regulation strategy and displays a high-performance catalyst for Li-CO2 batteries.

Achieving Coulombic efficiency values greater than 99.9% for Li metal cells is considered one of the most important requirements for the technology development of long cycle life in energy-dense Li metal batteries. However, owing to the volume changes in Li metal electrodes and Li reservoir loss during battery operation, this requirement has not yet been realized in Li metal cells. Here, to overcome these issues, we propose a zero-volume-change, complete-sealing design for a nanoengineered composite material consisting of multilayer reduced graphene oxide and zinc oxide. This composite electrode material can accommodate Li metal without showing negligible volume changes while promoting the formation of an inorganic-rich solid-electrolyte interphase. When the nanoengineered Li/reduced graphene oxide/zinc oxide electrode is tested in combination with a Li metal electrode in a coin cell configuration using non-aqueous electrolyte solutions, Li plating/stripping Coulombic efficiency values ranging from 99.9900% to 99.9999%, for almost 2,000 cycles at a current density of 1 mA cm-2, can be calculated. Testing of the nanoengineered Li/reduced graphene oxide/zinc oxide electrode in combination with high-potential electrodes (for example, LiNi0.8Co0.1Mn0.1O2 or LiFePO4) in non-aqueous coin cell configuration also demonstrates improved performance compared with the high-potential coin cells utilizing pristine Li metal electrodes.

Solid polymer electrolytes are emerging as a key component for solid‐state lithium metal batteries, offering a promising combination of large‐scale processability and high safety. However, challenges remain, including limited ion transport and the unstable solid electrolyte interphase, which result in unsatisfactory ionic conductivity and uncontrollable lithium dendrite growth. To address these issues, a high‐throughput Li‐ion transport pathway is developed by incorporating tungsten sulfide enriched with sulfur vacancies (SVs) into a poly(vinylidene fluoride‐co‐hexafluoropropylene)‐based composite polymer electrolytes (CPEs). The SVs strong interaction in the CPEs facilitates homogeneous high‐throughput Li‐ion transport 1.9 × 10 −3 S cm −1 at 25 °C) by enhancing the dissociation of lithium salts and effectively creates ample interfaces with the polymer chains to reduce the formation of inner vacuities. Moreover, the SVs confine FSI − anions, while the electron‐rich environment induced by sulfur atoms promotes the preferential degradation of bis(trifluoromethanesulfonyl)imide anions, ensuring uniform lithium deposition. This fosters the formation of inorganic nanocrystals on the lithium anode and effectively suppresses dendrite growth, enabling an ultra‐long lifetime of over 5500 h in Li||Li symmetric cells. When paired with sulfurized polyacrylonitrile cathode, a pouch cell capacity of 0.524 Ah is achieved, demonstrating the effectiveness of a homogeneous, high‐throughput Li‐ions transport mechanism.

Lithium-ion batteries (LIBs) as an effective low carbon technology provide a solution for achieving NetZero emissions, in line with the Sustainable Development Goals set by the United Nations. Research efforts have been devoted to increasing the energy density and efficiency of LIBs. However, large-scale deployment of LIBs is challenged by thermal runaway and safety problems, particularly under abusive conditions. To tackle this challenge, we must gain insight into the safety features of batteries and design durable strategies by fundamentally analyzing battery thermal runaway processes. In this review, we systematically summarize the abusive indicators that may trigger the thermal issues at the macroscopic level from thermal, chemical, and mechanical perspectives, and point out failure mechanisms that correlate with each component, e.g., cathode, anode, separator, electrolyte and current collector. Beyond material innovations, we emphasize the importance of optimizing industrial-scale manufacturing, integrating regulatory frameworks through advanced battery management systems, and enhancing safety engineering from an battery external perspective. Moreover, we systematically evaluate the contributions of theoretical and computational approaches to battery safety, critically comparing physics-based, machine learning, and hybrid models, and proposing targeted improvements. The broader implications of these safety strategies are considered in the context of environmental sustainability and recycling. Finally, we present design principles for safer, high-performance batteries and outline emerging research and industrial directions through a critical synthesis of thermal runaway mechanisms and mitigation strategies.

Li-rich Mn-based layered oxides provide a compelling amalgamation of high theoretical capacity and cost-effectiveness, positioning them as prime contenders for next-generation lithium-ion battery cathodes. However, their vulnerability to surface instability gives rise to a host of challenges, notably severe capacity and voltage fading. Consequently, the surface modification of Li-rich Mn-based layered oxides emerges as a viable solution to tackle this issue. Nevertheless, current methods exhibit various drawbacks, encompassing time-intensive procedures, environmental unfriendliness, and challenges in scalability. Hence, we present a technique employing ultrafast high-temperature heating technology to dynamically reshape the chemistry and structure of the surface of individual single-crystal Li1.2Mn0.54Ni0.13Co0.13O2 cathode particles (LMLO) within a rapid 8-second timeframe. Structural analysis reveals the seamless integration of the spinel structure onto the surface, intricately linked to the internal layered structure, accompanied by a notable abundance of oxygen vacancies. Leveraging the distinctive features of this modified structure, the material demonstrates enhanced discharge capacity, superior rate performance, and prolonged cycling stability compared to the unmodified counterpart. Significantly, in stark contrast to alternative preparation methods, this technique accomplishes the formation of the protective layer within a mere 8 seconds, showcasing unparalleled efficiency. Furthermore, it boasts safety and environmental friendliness, necessitates basic instrumentation, boasts ease of operation, and is well-suited for large-scale adoption. Consequently, this method is positioned to drive the commercialization of Li-rich Mn-based layered oxide cathode materials.

Traditional lithium-ion battery (LIB) anodes, whether intercalation-type like graphite or alloying-type like silicon, employing a single lithium storage mechanism, are often limited by modest capacity or substantial volume changes. Here, the kesterite multi-metal dichalcogenide (CZTSSe) is introduced as an anode material that harnesses a conversion-alloying hybrid lithium storage mechanism. Results unveil that during the charge-discharge processes, the CZTSSe undergoes a comprehensive phase evolution, transitioning from kesterite structure to multiple dominant phases of sulfides, selenides, metals, and alloys. The involvement of multi-components facilitates electron transport and mitigates swelling stress; meanwhile, it results in formation of abundant defects and heterojunctions, allowing for increased lithium storage active sites and reduced lithium diffusion barrier. The CZTSSe delivers a high specific capacity of up to 2266 mA h g-1 at 0.1 A g-1; while, maintaining a stable output of 116 mA h g-1 after 10 000 cycles at 20 A g-1. It also demonstrates remarkable low-temperature performance, retaining 987 mA h g-1 even after 600 cycles at -40 °C. When employed in full cells, a high specific energy of 562 Wh kg-1 is achieved, rivalling many state-of-the-art LIBs. This research offers valuable insights into the design of LIB electrodes leveraging multiple lithium storage mechanisms.

Aqueous zinc-sulfur batteries are a high-capacity and cost-effective energy storage technology. However, the performance is plagued by the dissolution of intermediate polysulfides formed during conversion. Here, this issue is addressed by developing aqueous rechargeable Zn-sulfurized polyacrylonitrile (SPAN) batteries using tandem catalytic systems, containing water and tetraglyme (G4) with iodine (I-2) additives. Mechanistic study and experiments reveal that the fully conjugated molecular configurations circumvent the formation of soluble polysulfides and enable reversible co-storage of H+/Zn2+ with multiple redox-active centers. The reduced I-2 by G4 activates I-/I-3(-) redox couple in SPAN, reducing activation energy, and accelerating Zn-ion transfer kinetics. Additionally, it stabilizes the Zn anode by forming an organic-inorganic interphase that induces the generation of the predominant (002) plane. The as-assembled Zn-SPAN batteries exhibit excellent performances, with a high capacity of 1260.4 mAh g(-1) at 0.2 A g(-1), a high-rate performance (409.3 mAh g(-1) at 5 A g(-1)), and a long cycling stability (81.8% capacity remained over 800 cycles at 2 A g(-1)). This work takes a crucial step forward in organosulfur compounds accompanied by multi-electron transfer for the high-performance aqueous zinc-ion batteries.