High-voltage (>4.5 V) lithium-ion batteries (LIBs) with LiCoO2 cathode and graphite anode are necessary for heavy-duty smart electronics. However, their development is substantially hindered by uncontrollable interface degradation on both cathode and anode sides. Here we report a Janus electrolyte additive that can simultaneously stabilize cathode- and solid-electrolyte interphases via a bifunctional decomposition pathway. The Janus additive, 1,3-propane sultone (PS), can be oxidized to generate Li2SO4 for cathode-electrolyte interphase (CEI), while being reduced to ROSO2Li species for solid-electrolyte interphase (SEI), thereby protecting both cathode and anode. Atomic force microscopy and focused ion beam-scanning electron microscopy reveal that the CEI formed in PS-containing electrolyte is thin and uniform (similar to 23.5 nm thick), substantially thinner than that without the PS additive (similar to 43.6 nm). The robust CEI layer effectively suppresses the PF6- decomposition and HF formation, leading to a more stable cathode interface at a high voltage cutoff. Meanwhile, the ROSO2Li-rich SEI can mitigate electrolyte decomposition and cobalt-ion crossover for improved anode stability. Therefore, 4.5 V LiCoO2||graphite pouch cells exhibit stable cycling over 300 cycles at 45 degrees C. This work demonstrates a Janus electrolyte additive for simultaneous interface regulation on both cathode and anode, offering a new electrolyte design strategy for high-voltage LIBs.

Charge transfer across interfaces constitutes the rate-determining step in electrochemical systems. Sluggish kinetics triggers side reactions and hazardous surface morphologies, as represented by dendritic/dead lithium (Li0) in Li-metal batteries (LMBs), especially under ultrafast charging (UFC). Here we report an approach to accelerate interfacial charge transfer by redesigning the solvent molecular structure into a distinctive planar coordination of lone-pair electrons (LPEs) with alkaline cations (Li+ or Na+). This planar-aligned electron channel (PAEC) greatly strengthens the coupling between LPEs and Li+, promoting Li+/Li0 redox reaction kinetics and reversibility. The designed electrolyte dramatically enables stable cycling of industrial 2 Ah Li||LiNi0.8Mn0.1Co0.1O2 pouch cells at an ultrahigh rate of 4 C, achieving 100% full charge within 15 min at a charging power density of 1,747.6 W kg-1. We establish a link between the solvation electronic structure and charge-transfer dynamics, highlighting a potential strategy for electrolyte design under extreme electrochemical conditions.

3D structured lithium metal anodes (LMAs) tackle planar anode challenges in solid-state batteries. This review emphasizes failure mechanisms, material design and manufacturing for high-performance 3D LMAs in solid-state batteries.

The advancement of nonaqueous magnesium metal batteries (MMBs) is critically impeded by severe interfacial instability at the Mg anode. The primary challenge stems from the high charge density of Mg2+ ions, which promotes the formation of tenacious solvation structures and a passivating solid electrolyte interphase (SEI). These phenomena jointly lead to sluggish Mg2+ desolvation kinetics and inhomogeneous, dendritic Mg deposition. To address this, this review systematically dissects these fundamental interfacial challenges. We thoroughly evaluate in situ and operando characterization techniques that elucidate the dynamic processes at the electrode-electrolyte interface. Building on these mechanistic insights, we present a comprehensive analysis of rational optimization strategies, focusing on electrolyte solvation structure modulation, artificial interphase engineering, and 3D anode architecture design. By bridging advanced diagnostic insights with strategic material design, this review aims to deepen the fundamental understanding of Mg anode interfacial chemistry and provide a clear roadmap for developing practical, high-performance MMBs.

The safety behaviors of Lithium-Ion Batteries are critical for public safety and economic development. However, the thermal runaway behaviors of LIBs, especially under the coupled environment of complex abuse conditions, are not fully understood. Herein, we systematically trace the safety behaviors of LIBs with an energy of 20 Wh, which is assembled with Graphite/Silicon composite anode and LiCoO2 cathode, that undergo a series of coupled abuse conditions, such as overcharge extrusion, temperature circulating storage extrusion, fast charging extrusion, thermal abuse extrusion. The ultimate extrusion force, deformation amount, highest TR temperature, and evolutionary images of safety behaviors of cell are reported and their relationships are analyzed. Batteries operating under different coupling conditions undergo various changes in their internal structure and substances, exhibiting distinctly different safety performances. This study demonstrates that relying solely on fresh-cell safety standards implemented at product launch cannot accurately evaluate the full-lifecycle risk of lithium-ion batteries.

Developing advanced iridium (Ir)-based oxygen evolution reaction (OER) catalysts is critical for proton exchange membrane water electrolyzers (PEMWEs). Unfortunately, conventional adsorbate evolution mechanism (AEM) and lattice oxygen mechanism (LOM) pathways suffer from an activity-stability trade-off, posing substantial challenges for catalyst design. Here, we report a charge-redistribution-induced oxygen (O) spillover strategy by designing amorphous VOx-supported iridium-tin (IrSn) alloy OER catalysts, which can effectively transfer the poisoning oxygenated intermediates and maintain Ir valence stability (+2.5) during the dynamic OER to enhance activity and stability. In particular, the IrSn-VOx-based PEMWE anode can deliver a current density of 3.0 amperes per square centimeter @ 1.798 volts (0.4 milligrams of platinum and Ir per square centimeter), surpassing the US Department of Energy (DOE) 2026 targets. A 25-square centimeter PEMWE operates stably for 5000 hours at industrial currents (≥25 amperes) with an exceptionally low degradation rate of 5.6 microvolts per hour, representing one of the best OER catalysts reported for practical PEMWEs. Theoretical calculations predict that the charge redistribution within IrSn-VOx could reduce the kinetic energy barrier for *O spillover (from Ir to VOx) by 69% relative to O-O coupling, thus triggering the O spillover against the Ir overoxidation/dissolution. Consequently, IrSn-VOx follows a support-involved LOM pathway with a reduced rate-determining-step barrier (0.37 electron volts) relative to IrSn following AEM (0.66 electron volts). In addition, Sn doping in IrSn-VOx can further promote the regeneration of VOx lattice O and improve stability.

Single-atom catalysts (SACs) have been extensively explored for the oxygen evolution reaction (OER) owing to their maximal atom utilization and high mass activity. However, isolated single-metal centers often suffer from intrinsic linear scaling relationships among oxygenated intermediates, thereby limiting their catalytic efficiency in the complex four-electron OER process. To overcome these limitations, we construct atomically dispersed Ir-Ir duet atoms anchored on CoOOH surface (Ir2/CoOOH) to break the intrinsic scaling relationships governing the OER. Benefiting from the synergistic interaction between adjacent Ir atoms, Ir2/CoOOH exhibits an ultralow overpotential of similar to 235 mV at 10 mA cm-2 and outstanding durability over 1200 h at 500 mA cm-2 in 1 M KOH. Remarkably, Ir2/CoOOH achieves a turnover frequency approximately three times higher than that of isolated Ir single atoms on the CoOOH surface (Ir1/CoOOH), highlighting the critical role of synergistic duet cooperation in enhancing intrinsic OER activity. Operando spectroscopic measurements combined with theoretical calculations reveal that cooperative Ir-Ir interactions and strong metal-support interactions optimize the local charge density of Ir active centers, regulate the rate-determining step, and significantly lower the activation free energy of the OER. These findings demonstrate the effectiveness of atomically dispersed duet-metal sites in overcoming activity limitations in water oxidation catalysis.

Fe-based polyanionic cathodes are promising for large-scale Na-ion batteries owing to their stability, safety and elemental abundance, however their capacity remains limited by electrochemically inactive Na sites and irreversible Na loss. Here we identify that the Na+ coordination environment critically influences the Na-site accessibility and redox activity in Na4Fe3(PO4)(2)P2O7-type cathodes. Combined experimental and theoretical analyses reveal that precise V3+ substitution at the Fe2 site harmonizes Na+ coordination geometry and softens the polyanionic framework, thereby activating previously inert Na sites and stabilizing high-voltage redox reactions above 4 V. The optimized Na3.4Fe2.4V0.6(PO4)(2)P2O7 achieves full Na+ utilization (3.4 Na+, 150.7 mAh g(-1)) and a 52% increase in energy density (487 Wh kg(-1)), approaching the practical limit of Li-ion phosphate cathodes. It also demonstrates exceptional durability over 10,000 cycles in the 2.1-4.5 V range and stable pouch-cell performance. These findings provide a coordination-based strategy to overcome intrinsic capacity limitations in phosphate cathodes, enabling high-energy, durable Na-ion batteries.

Developing non-noble metal catalysts for hydrocracking polyolefins is a promising yet formidable challenge for upcycling waste plastics in practice. Herein, we report a NiW/WOx (2 < x < 3) catalyst, which accomplishes polyolefin hydrocracking at 250 degrees C, yielding a liquid product of about 73 wt % and a gaseous product of about 22 wt %. The liquid fraction primarily consists of hydrocarbons in the C-4-C-25 range, with more than 77% falling within the jet-fuel-range components (C-8-C-16). The gas product is dominated by branched C-3-C-6 hydrocarbons, characteristic of liquefied petroleum gas (LPG), with negligible carbon loss, such as methane and ethane.A sequence change from inactive to active, and back to inactive in polyolefin hydrocracking was found accompanying the reconstruction of the surface structure of the catalyst from Ni-doped WO3 to NiW alloy nanoparticles supported on WOx (NiW/WOx), and then to WO2-encapsulated NiW (NiW@WO2). The coexposure of NiW alloy nanoparticles and WOx is further demonstrated to be necessary for fulfilling the bifunctionality of the catalyst in hydrogen dissociation and C-C bond cleavage in polyolefin hydrocracking, and the absence of either will deactivate the catalyst.

ABSTRACT Temperature plays a critical role in governing the plating behavior of metallic anodes by regulating ionic conductivity of the electrolyte, desolvation energy, and charge transfer processes in the solid‐electrolyte interphase (SEI). While low temperature commonly triggers dendritic growth on metallic anodes (e.g., Li, Na, and Zn), the temperature effect on Mg plating/stripping behaviors remains unknown thus far. Herein, we report an unconventional temperature‐dependent deposition behavior of Mg anodes that tends to form dendrite‐free deposits at low temperatures. Integration of cryo‐transmission electron microscopy, atomic force microscopy, and x‐ray photoelectron spectroscopy reveals that the SEI layer formed at low temperatures has an ultrathin thickness (∼2‐3 nm) and is enriched in high‐modulus inorganic compounds, which facilitates the uniform deposition of Mg anodes. As a result, the Mg metal anode realizes an exceptional average Coulombic efficiency up to 99.92% over 2000 cycles at −20°C. This study demonstrates the unconventional deposition behavior of Mg metal anodes at low temperatures, underpinning their potential for low‐temperature applications and advancing the fundamental understanding of metal deposition.

Lithium metal batteries promise energy densities beyond 500 Wh kg-1; but their practical deployment remains limited by low Coulombic efficiency and uncontrolled electrolyte-interface reactions. Here, we show that physics-guided machine learning can identify the molecular origin of Coulombic efficiency (CE) from small experimental datasets by embedding 3D electrolyte structures into data-driven descriptors. Among the descriptors examined, the physics-derived solvent-surrounding-Li+ descriptor (LiSSL) enables accurate CE prediction, achieving a test-set R2 of 91.15%. Explainable machine learning further reveals LiSSL as the dominant factor governing model performance, indicating that high-efficiency lithium deposition requires suppression of direct Li+-solvent interactions. This insight establishes a molecular design principle for electrolytes: weakening solvent participation in the primary Li+ solvation environment promotes higher CE. Our work provides a physics-informed, data-driven framework for accelerating electrolyte discovery toward high-energy lithium metal batteries.

Upcycling waste plastics into liquid fuels presents significant potential for advancing the circular economy but is hindered by poor selectivity and low-value methane byproduct formation. In this work, we report that atomic Ru-doped ZrO 2 can selectively convert 100 grams of post-consumer polyethylene and polypropylene, yielding 85 mL of liquid in a solvent-free hydrocracking. The liquid (C 5 -C 20 ) comprises ~70% jet-fuel-ranged branched hydrocarbons (C 8 -C 16 ), while the gas product is liquefied-petroleum-gas (C 3 -C 6 ) without methane and ethane. We found that the atomic Ru dopant in the Ru-O-Zr moiety functionalizes its neighboring O atom, originally inert, to create a Brønsted acid site. This Brønsted acid site, rather than the atomic Ru dopant itself, selectively governs the internal C−C bond cleavage in polyolefins through a carbonium ion mechanism, thereby enhancing the yield of jet-fuel-ranged hydrocarbons and suppressing methane formation. This oxide modulation strategy provides a paradigm shift in catalyst design for hydrocracking waste plastics and holds potential for a broad spectrum of applications.

Solid electrolyte interphases (SEIs) play essential roles in lithium metal batteries by dictating the deposition morphology and Coulombic efficiency (CE) of lithium metal anodes. However, the understanding of the formation and evolution of SEIs remains elusive so far. Herein, we present an operando investigation of the formation and evolution dynamics of LiNO3-induced SEI under liquid electrolytes using high-resolution electrochemical atomic force microscopy (EC-AFM). For the first time, we discovered the in situ formation of an ultrathick SEI (∼648 nm) under liquid electrolytes, which far exceeded the thicknesses observed via ex situ characterization techniques. This ultrathick SEI formed through a sequential reduction process, wherein an inorganic-rich inner layer was initially formed, followed by the deposition of a soft outer layer with a modulus of approximately 24 MPa. We also observed that the outer SEI layer was metastable and susceptible to dissolution in liquid electrolytes. Our findings provide a comprehensive investigation of the formation and evolution processes of the LiNO3-induced SEI, deepening the understanding of the in situ structure of SEIs under liquid electrolytes.

An oscillating Li + -acceptor fluorine-donor electrolyte incorporating a new co-solvent with an asymmetric super-lithiophilic fluorine group resolves the dilemma between fast electrolyte Li + transport and stable interphases.

The electric double layer (EDL) plays a pivotal role in governing interfacial composition and electrode behavior in electrochemical systems. However, the intricate relationship between EDL architectures and electrochemical processes remains elusive. Here the fundamental significance of hydrogen bond polarity within the EDL in orchestrating the interfacial lithium-ions (Li+) exchange dynamics is elucidated. At charged interfaces, the electropositive aprotic hydrogen (Hδ+) and Li+ ions exhibit comparable electrostatic responses, resulting in their competitive effect for the solvent oxygen sites, which modulates the de-solvation process and ultimately impacts battery performance. Based on this, a solvent-centered de-solvation mechanism is proposed, wherein the microenvironment with enhanced hydrogen polarity in the EDL facilitates solvent displacement from Li+ coordination shells. Furthermore, the presence of polar hydrogen at charged cathode interface can effectively anchor uncoordinated solvents molecules, increasing the energy barrier for detrimental dehydrogenation reaction. As a result, electrolytes design based on this strategy enables remarkable electrochemical stability, achieving over 2000 cycles in a 5 V dual-ion battery. In addition, the Gr||NCM811 pouch cell exhibits exceptional longevity, retaining 90.2% of its initial capacity after 1000 cycles.

Low-loading iridium (Ir) catalysts hold great promise for the acidic oxygen evolution reaction (OER) due to their typically high Ir utilization and reduced cost. However, their practical application is limited by poor stability under the harsh acidic oxidative conditions of proton exchange membrane (PEM) water electrolysis. Here, a controlled structural transformation strategy is presented that converts an unstable LiCoO2-supported Ir single-atom catalyst (Ir-LiCoO2) into a corrosion-resistant Co3O4-supported IrOx nanocluster catalyst (IrOx/Co3O4), significantly enhancing catalyst durability. Strong catalyst-support interactions between IrOx and Co3O4 facilitate charge transfer, thereby stabilizing the IrOx nanoclusters against leaching and optimizing the electronic structure of the Ir active sites. As a result, IrOx/Co3O4 exhibits substantially enhanced OER performance compared to Ir-LiCoO2, achieving excellent operational stability over 1200 h and a low overpotential of approximate to 233 mV at 10 mA cm-2 in 0.5 m H2SO4. This superior performance is further validated in PEM electrolyzers, confirming its practical applicability. Furthermore, theoretical calculations reveal that Ir sites in IrOx/Co3O4 exhibit higher dissolution potentials and improve charge transfer capabilities with OER intermediates compare to those in Ir-LiCoO2 and IrO2, which effectively suppresses Ir leaching and lowers the energy barrier of the potential-determining step.

Amorphous materials are ubiquitous in nature and are widely used for many industrial applications, including catalysis, energy storage, and environmental science. However, significant challenges remain in designing and optimizing amorphous high-entropy materials because of the lack of well-defined structure-activity relationships. Here, we use synthesis systems to discover and optimize amorphous high-entropy oxyhydroxide electrocatalysts within the entire design space for the alkaline oxygen evolution reaction. Amorphous high-entropy electrocatalysts are derived from ultrathin 2D coordination polymers composed of six nonprecious metal elements that were selected from top 16 candidate metal elements involved in oxygen evolution reaction (OER)-related literature searching, which can then be transformed in situ into amorphous oxyhydroxides. Leveraging machine learning (ML) techniques, we establish a composition-activity relationship and thereby identify an optimal composition group by traversing the entire design space (over 1,900,000 compositions). Our ML-model is validated by using 100 compositions in the high-activity region and 588 compositions in the low-activity region, which results in excellent recall values of nearly 100%. The predicted optimal amorphous high-entropy electrocatalyst demonstrates an ultralow overpotential of 159 mV at a current density of 10 mA cm-2 for the alkaline OER in a 1 M KOH while exhibiting ultralong durability 10,218 h under a practical current density of 1 A cm-2 in a 6 M KOH. Our work provides a general strategy for the automatic discovery and optimization of amorphous high-entropy oxyhydroxide electrocatalysts and could significantly impact the development of other amorphous high-entropy materials.

Electrochemical water splitting has attracted tremendous interest as a promising approach for generating sustainable hydrogen for transportation and other industrial applications. However, the oxygen evolution reaction (OER) significantly limits the efficiency of electrochemical water splitting because of the sluggish reaction kinetics derived from the intrinsic four-electron-transfer process. In addition, the stability of OER electrocatalysts encounters significant challenges during long-term operation under harsh conditions. To overcome these challenges, we demonstrate that monolithic electrodes composed of medium-entropy alloys (MEAs) containing Fe, Co, Cr, and Ni can be used as efficient and stable OER catalysts in alkaline solutions. The monolithic FeCoCrNi alloy electrode exhibited a remarkably low overpotential of 237 mV at a current density of 10 mA/cm2 in a 1 mol/L KOH solution. Significantly, the monolithic alloy electrode can operate stably for more than 20 0 0 h at a practical current density of 1 A/cm2 . The enhanced activity and stability of the alloy electrode are ascribed to surface reconstruction. This work presents a novel and effective approach for fabricating high-performance electrodes with excellent stability for the oxygen evolution reaction. (c) 2025 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.