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.

Developing lithium-ion batteries (LIBs) operable across extreme temperatures (−40 to 60 °C) is imperative for electric vehicles and space technologies, yet hindered by incompatible interphasial requirements: cathode–electrolyte interphase (CEI) degradation at high temperatures and anode solid-electrolyte interphase (SEI) impedance surge under subzero conditions. Here, we report a novel dual-salt electrolyte composed of weakly dissociated LiPO2F2 (LiDFP) and commonly used LiPF6 in an ethyl acetate (EA)/ethylene carbonate (EC) co-solvent, enabling wide-temperature LIB operation with exceptional interphasial stability. LiDFP with elevated solubility renders contact ion pairs and aggregates surrounding Li+, enriching PO2F2− coordination within the Li+ solvation shell. This unique solvation structure promotes the preferential decomposition of PO2F2− anions at electrode surfaces, forming thin, dense CEI/SEI layers dominated by Li3PO4 and LiF, which simultaneously enhance interphasial robustness and Li+ transport. As a result, 5 Ah NCM613‖graphite pouch cells deliver over 80% capacity retention after 200 cycles at 60 °C and maintain 57% reversible capacity at −40 °C, while the cell using the LiPF6-EC electrolyte retains 80% capacity after only 200 cycles at 45 °C. By decoupling anion-mediated interfacial regulation from solvent-centric limitations, this work establishes a universal electrolyte paradigm to achieve intrinsically stable, wide-temperature LIBs.

Density functional theory (DFT) serves as the basis for computational discovery in materials science and chemistry, yet each calculation demands extensive human effort: adjusting algorithms when convergence stalls, revising plans when unexpected physics emerges, and inserting steps as intermediate results reshape the problem. Existing LLM-based agents automate only the initial planning stage, producing a full execution plan upfront and leaving all subsequent adaptation to hand-crafted rules. As a result, these workflows remain fragile, do not generalize well beyond pre-planned scenarios, and often require expert intervention when failures or unexpected intermediate results require changes to the calculation path. Here, we introduce AutoDFT, a closed-loop multi-agent framework that embeds LLM reasoning into every stage of the DFT lifecycle, where a strategic planner produces a skeletal plan of step objectives; a step planner generates numerical parameters just in time from preceding results; and a monitor-recover-reflect cycle diagnoses failures, repairs them, and revises the plan when the evidence justifies it. We demonstrate both breadth and depth: breadth on VASPBench, a purpose-built benchmark spanning 34 tasks and 9 DFT calculation types, where AutoDFT achieves 94.1

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.

Lithium metal batteries possess the high theoretical specific energy owing to the high theoretical specific capacity of lithium metal. However, practical implementations necessitate a reduction in both lithium mass fraction and lithium utilization within the negative electrode to enhance cycling life and suppress dendrite formation, resulting in a practical reversible capacity of only 30 - 50% of the theoretical value. Herein, we present a lithium metal-based multicomponent solid-solution alloy comprising approximately 90 wt.% lithium, with equal atomic ratios of cadmium, silver, magnesium, and aluminium constituting the remaining 10 wt.%. The increased mixing entropy enables high lithium-atom diffusivity, facilitating inward lithium transport into the metal foil rather than the surface deposition typically observed in conventional lithium metal negative electrodes, while simultaneously promoting a thermodynamically stable (110) crystal facet. These factors collectively yield a dendrite-free negative electrode with a reversible specific capacity of 3100 mAh g-1. One-ampere-hour pouch cells employing this negative electrode and a LiNi0.8Co0.1Mn0.1O2 positive electrode achieve an specific energies of 385 Wh kg-1 (based on the total mass of the pouch cell) with 82% capacity retention over 600 cycles. This achievement highlights the potential of this alloy negative electrode to enable safe and durable high-energy-density lithium metal batteries for practical applications.

Polymer-based quasi-solid-state electrolytes (QSSE) are believed to be the most feasible candidates for solid-state batteries, but they are hindered by relatively lower ionic conductivity and narrower electrochemical window. Here, we synthesize a series of ether-free acrylates containing Li+-ligands for high-voltage-stable QSSEs. Our findings demonstrate that the polymer-involved solvation structure is critical in determining the ionic conductivity, and low-temperature crystallization of the polymer can be used for non-destructive life extension of batteries. The prepared polymers do not contain ether unit and exhibit a polymerization degree of 99% in cells without residual double-bonded monomer, endowing them with high antioxidation capability and compatibility with high-voltage positive electrodes including LiNi0.85Co0.075Mn0.075O2, 4.6 V LiCoO2 and 4.8 V Li1.13Ni0.3Mn0.57O2. The confinement of liquid in QSSEs effectively suppresses the interfacial reactions, but the residual interface reactions still gradually consume liquid electrolytes and cause capacity fading, due to the limited diffusion of the confined solvent to wet the interface. Through crystallizing the polymer matrices at -50 °C, the confined liquid in QSSEs is released and re-wets the Li-metal/polymer interface, thereby recovering the capacity and extending the life of solid-state batteries in a non-destructive manner.

Lithium ion batteries have gained great success since 1st commercial application in 1991. The relations between battery design and manufacturing process, however, are still not well discussed, partially due to the gap between industry and academic. To elucidate the relations, major different types of battery structure are addressed first, which is not commonly discussed in the literature. Different battery structure will require different of electrode structures and assembly processes, which means different manufacturing processes. Some examples are further discussed to show how these relations are interactive formed. In the future, from the systematic view of battery design and manufacturing, research and application of battery manufacturing could be accelerated and impactful.

Developing a carbon anode with high performance but low cost is one most pivotal challenges for the commercialization of sodium ion batteries (SIBs). Therefore, an sulfur-mediated solid-state approach is proposed to form 3D crosslinked polymer networks in a pitch precursor and then achieve elaborate microstructures for effective sodium storage. Sulfur-linked structures interfere with the stacking regularity of carbon layers, thereby eliminating the graphitic transformation of pitch at high treatment temperatures, expanding interlayer distances, and promoting the development of closed pores. Consequently, sodium storage capacity in such carbon material is impressively augmented from 109 to 315 mA h g-1, with a plateau contribution exceeding 81.3% at low voltages, which can improve energy density of SIBs. Compared to prior Oxygen-related methodologies, this sulfur-mediated technique not only offers a more scalable strategy but also achieves superior plateau performance at lower carbonization temperatures (≈1300 °C), far below the conventional threshold of 1500 °C. Additionally, comprehensive testing demonstrates that sodium storage operates via an "adsorption-intercalation-pore filling" mechanism, with closed nanopores playing a crucial role in enabling efficient Na storage through pore filling in the low voltage region. This work also presents a scalable strategy for the development of high-performance carbon anode materials from low-cost pitch.

The structural complexity and heterogeneity of disordered carbons give rise to significant challenges in elucidating the sodiation mechanism in them. Herein, by means of a precisely controlled gaseous corrosion strategy, disordered carbon samples with tailored local structures are prepared elaborately so that we are able to unravel the sodium storage explicitly in such materials. In terms of results, a multi-stage sodium storage model comprising "physical adsorption - chemical interaction -(solid phase diffusion) - sodium cluster filling" is proposed. This work is the first to highlight the critical role of "solid phase diffusion" as an essential kinetic bridge, which is activated upon the saturation of defect sites and functional groups and governs the initial stage of sodium cluster formation within closed pores. Furthermore, our study reveals that sodium storage mechanisms are related to structures of disorder carbon materials, dictated by their defect concentrations, types and spatial distributions. It is demonstrated that a superior disordered carbon anode for a sodium ion battery necessitates an elaborate balance between abundant closed pores and moderate monovacancy-type defects so as to possess good capacity, rate performance and initial coulombic efficiency. With balanced features, the disordered carbon sample delivers a high reversible capacity of 367.1 mA h g-1, and the full cell achieves an energy density of 307.7 Wh kg-1 while maintains 95.1 % capacity retention after 160 cycles. This research advances the understanding of sodium storage and provides new insights for engineering next-generation high-performance carbon anodes for sodium ion batteries.

The discovery of advanced metallic alloys is hindered by vast composition spaces, competing property objectives, and real-world constraints on manufacturability. Here we introduce MATAI, a generalist machine learning framework for property prediction and inverse design of as-cast alloys. MATAI integrates a curated alloy database, deep neural network-based property predictors, a constraint-aware optimization engine, and an iterative AI-experiment feedback loop. The framework estimates key mechanical propertie, sincluding density, yield strength, ultimate tensile strength, and elongation, directly from composition, using multi-task learning and physics-informed inductive biases. Alloy design is framed as a constrained optimization problem and solved using a bi-level approach that combines local search with symbolic constraint programming. We demonstrate MATAI's capabilities on the Ti-based alloy system, a canonical class of lightweight structural materials, where it rapidly identifies candidates that simultaneously achieve lower density (<4.45 g/cm3), higher strength (>1000 MPa) and appreciable ductility (>5

Alloy discovery is constrained by vast compositional spaces, competing objectives, and prohibitive experimental costs. Although simulations and machine learning have each accelerated parts of this process, unifying scientific knowledge, scalable search, and experimental confirmation into a data-efficient workflow remains challenging. Here, we present AutoMAT, a hierarchical autonomous framework spanning ideation to experimental validation. Integrating large language models, automated CALPHAD simulations, residual-learning-based correction, and AI-guided optimization, AutoMAT translates design targets into candidate alloys, refines compositions through closed-loop computational search, and validates results experimentally without hand-curated datasets. Targeting lightweight, high-strength alloys, AutoMAT identifies a titanium alloy 8.1

Next‐generation lithium‐ion batteries (LIBs) require electrolytes compatible with high‐voltage (>4.3 V) and low‐temperature (<−10 °C) operation, yet commercial ethylene carbonate (EC)‐based systems remain constrained by intrinsic limitations including poor oxidation stability at cathode side and high melting points. Although propylene carbonate (PC) demonstrates superior oxidative stability and lower melting temperature than EC, its tendency to cointercalate with Li + within the graphite anode interlayers restricts its applicability in LIBs. We propose a PC‐based weakly‐solvating electrolyte engineered with difluoroethylene carbonate (DFEC) that resolves interfacial challenges at both electrodes. The PC solvent facilitates oxidative resistance through formation of an inorganic‐dominated cathode–electrolyte interphase (CEI), effectively mitigating transition metal dissolution at 4.4 V operation. Simultaneously, DFEC disrupts Li + ‐PC coordination through reduced solvent molecule numbers in the solvation shell, enabling generation of a stable solid electrolyte interphase (SEI) on graphite anodes with minimized interfacial impedance. Implemented in 5 Ah pouch cells, this electrolyte demonstrates 76.7% capacity retention after 2000 cycles (2.8–4.4 V) at room temperature (RT) and maintains 91% of its RT capacity at −20 °C, surpassing conventional EC‐based electrolytes. This work presents an electrolyte engineering approach that synergistically addresses high‐voltage durability and low‐temperature functionality, providing a scalable solution for advanced LIB technologies.

The development of high-voltage LiCoO2 (LCO) is crucial for achieving lithium-ion batteries with a high volumetric energy density. However, LCO experiences accelerated degradation at high voltages due to severe interface and structure instability. A uniform and robust cathode-electrolyte interphase (CEI) serves as a vital barrier for protecting the interface. However, the smooth surface of single-crystalline LCO, lacking grain boundaries, poses challenges in generating an effective CEI. Herein, ZrO2 nano-rivets are constructed on the surface of LCO to provide phase boundaries for preferential film-forming sites, inducing the formation of a uniform and robust CEI. The high-quality CEI derived from ZrO2 nano rivets stabilizes the fragile surface of high-voltage LCO and facilitates lithium-ion diffusion. In addition, a Zr diffusion layer is simultaneously built in the LCO bulk. Zr diffusion into the LCO lattice not only effectively suppresses unfavorable phase transitions to stabilize the bulk structure, but also mitigates oxygen charge deficiencies at the highly delithiated state, therefore stabilizing lattice oxygen. Consequently, the modified LCO exhibits excellent capacity retention of 80% after 700 cycles at 4.6 V. This work emphasizes the significance of material surface properties in CEI formation and provides new insights for the design of CEI.

The development of practical lithium metal cells is plagued by their limited lifespan, primarily due to the poor interfacial stability of the electrolytes. Here we present a compact ion-pair aggregate (CIPA) electrolyte that enables high-performance Li metal pouch cells under lean electrolyte conditions. The electrolyte features a unique nanometre-scale solvation structure in which ion pairs are densely packed to form large CIPAs, in contrast to conventional electrolytes that comprise small aggregates. Notably, the CIPAs facilitate fast interfacial reduction kinetics on the Li metal anode via a collective electron-transfer process, leading to the formation of a stable interface. A 505.9 Wh kg(-1) Li metal pouch cell with a high-nickel-content cathode (LiNi0.905Co0.06Mn0.035O2) exhibited a 91% energy retention after 130 cycles. This work demonstrates nanostructured electrolyte design for realizing high-performance Li metal batteries. It also showcases the importance of understanding interfacial reaction mechanisms in the design and development of electrolytes.

The ever-increasing energy demanding and concerns on scarcity of lithium minerals drive the development of sodium ion batteries, which are regarded as a promising option apart from lithium ion batteries for energy storage technologies. In this perspective, we first provide an overview of characteristics of sodium ion batteries compared to lithium ion batteries. Next we discuss critical metrics in the commercialization of sodium ion batteries in terms of costs including bill of materials and manufacturing cost, performances like maximizing energy density via some important design metrics and market acceptance. Furthermore, we point out the challenges from different components for achieving better electrochemical properties including the closed-loop battery recycling, and conduct a technological trend analysis based on sodium ion battery patent landscapes, with the expectation that the insights provided in this perspective may help to inspire researchers and to shorten the gap between the academia and industry for accelerating sodium ion batteries in practical applications.

For the first time, this work investigates the synergetic impact of yttrium (Y) and aluminium (Al) co-doping on the electrochemical properties of 4.6 V LiCoO2 (LCO) cathode for high energy density lithium-ion batteries. The optimized LCO demonstrates an impressive initial discharge capacity of 208.6 mAh g−1 in the voltage range of 3-4.6 V, along with superior structural stability, retaining over 86% of its initial capacity even after 125 cycles at the current of 100 mA g−1 that is far higher than the capacity retention of 40% for the pristine LCO under the same condition. Thanks to the synergistic effect, Al in Co layers enhances the bonds of Al/Co-O to stabilize oxygen in the LCO crystal structure while Y serves “pillar” in Li layers, migrated from the initial Co layers during cycling process, effectively curtail the formation and expansion of interlayer cracking, which contributes to the long-term cycle stability of LCO under high voltage. Most importantly, Al/Y co-doping is a facile process compatible with the existing industrial infrastructure for LCO mass production, and thus it can be scaled up readily for commercial applications. Al/Y co-doped LCO is assembled into commercial-level pouch cells with graphite anode, achieves an extremely high energy density of 750 Wh/L, and exhibits a superior cycling stability and obtains a capacity retention of 88.2% at 25 °C after 800 cycles with the high cutoff voltage of 4.55 V.

Batteries with increasing energy density have boosted the development of electric vehicles with longer driving ranges but are also arousing safety concerns, especially thermal runaway, which impede their large-scale application....

Carbon quantum dots (CQDs) have versatile applications in luminescence, whereas identifying optimal synthesis conditions has been challenging due to numerous synthesis parameters and multiple desired outcomes, creating an enormous search space. In this study, we present a novel multi-objective optimization strategy utilizing a machine learning (ML) algorithm to intelligently guide the hydrothermal synthesis of CQDs. Our closed-loop approach learns from limited and sparse data, greatly reducing the research cycle and surpassing traditional trial-and-error methods. Moreover, it also reveals the intricate links between synthesis parameters and target properties and unifies the objective function to optimize multiple desired properties like full-color photoluminescence (PL) wavelength and high PL quantum yields (PLQY). With only 63 experiments, we achieve the synthesis of full-color fluorescent CQDs with high PLQY exceeding 60% across all colors. Our study represents a significant advancement in ML-guided CQDs synthesis, setting the stage for developing new materials with multiple desired properties.

Electrocatalysis is generally confined to dynamic liquid-solid and gas-solid interfaces and is rarely applicable in solid-state reactions. Here, we report a paradigm shift strategy to exploit electrocatalysis to accelerate solid-state reactions in the context of lithium-ion batteries (LIBs). We employ heteroatom doping, specifically boron for silicon and sulfur for phosphorus, to catalyze electrochemical Li-alloying reactions in solid-state electrode materials. The preferential cleavage of polar dopant-host chemical bonds upon lithiation triggers chemical bond breaking of the host material. This solid-state catalysis, distinct from liquid and gas phases, requires a critical doping concentration for optimal performance. Beyond a critical concentration of similar to 1 atom %, boron and sulfur doping drastically reduces activation energies and accelerates redox kinetics during lithiation/delithiation processes, leading to markedly enhanced rate performance in boron-doped silicon and sulfur-doped black/red phosphorus anode. Notably, a sulfur-doped black phosphorus anode coupled with a lithium cobalt oxide cathode achieves an ultrafast-charging battery, recharging 80% energy of a battery in 302 Wh kg(-1) in 9 min, surpassing the thus far reported LIBs.

Constructing structured anodes with lithiophilic materials has emerged as an essential strategy to stabilize Li deposition and accomplish highly reversible Li metal batteries (LMBs). Nevertheless, a lithiophilic material, which meets the requirements of low cost, excellent electronic conductivity and especially chemical stability, is still absent. Herein, we report the discovery of a new class of lithiophilic anti-perovskite nitrides MNNi3 (M=Zn, Cu, In) that not only are cost-effective and highly conductive, but also possess excellent stability against Li metal. More specifically, electrochemical tests in combination with density functional theory (DFT) calculations reveal that the lithiophilicity of MNNi3 arises from unique chemical/physical adsorption rather than the previously proposed alloying or conversion reaction mechanisms. The MNNi3@CC enabled symmetric cells exhibit better rate capability and longer cycle life than the cells with pure carbon cloth and Ni3N@CC. More importantly, the excellent electrochemical performances of MNNi3 anodes are also verified by ZnNNi3@CC in a LiFePO4 coupled full cell with minimal capacity degradation of 28% in 1500 cycles under the charge/discharge current of 1C. Beyond offering a new type of non-reactive lithiophilic materials to outstanding achieve battery performance, this study deepens the understanding of the lithiophilic nature of different metal nitrides, which paves a way for developing highly reversible lithium metal anode.