The development of high-energy lithium metal batteries (LMBs) requires cathode areal capacities exceeding 4 mAh cm(-2), ultra-thin lithium (Li) foil (<50 mu m), and over 500 cycles with 80 % capacity retention to achieve commercially viable applications. While significant advances in electrolyte formulation, pressure control, and interfacial engineering have improved LMB performance, the interplay among cathode capacity loading, Li utilization, and cycle life remains underexplored in practical cell configurations. Here, we investigate the impact of cathode capacity loading on electrochemical reversibility, Li loss mechanisms, and cycle life using a 20 mu m Li anode. Li||Cu half-cell analysis benchmarks Coulombic efficiency (CE) behavior across varied Li cycling capacities. We find that while higher cathode loadings (4-5 mAh cm(-2)) yield higher Li cycling CE, they also result in greater cumulative Li loss and faster degradation from solid-electrolyte interphase (SEI) formation and inactive Li. These cells require >= 99.8 % CE to achieve 500 cycles with 80 % of capacity retention, compared to similar to 99.6 % for lower-capacity designs (2 mAh cm(-2)). Full cell studies with LiNi0.8Mn0.1Co0.1O2 (NMC811) reveal further deviations from Li-metal estimation, attributed to increased cathode polarization at higher loadings. A quantitative inverse linear relationship is established between cathode capacity loading and achievable cycle life. These findings highlight the importance of standardized testing conditions for evaluating improvement strategies and provide practical design guidance for integrating high-loading cathodes with ultra-thin Li anodes, advancing the realization of high-energy LMB systems.
Abstract All‐solid‐state lithium batteries (ASSLBs) are the leading next‐generation energy storage solutions due to their superior safety, high energy density, and broad temperature adaptability. Solid‐state polymer electrolytes (SPEs) are critical factors in the development of ASSLBs, requiring high ionic conductivity (IC), mechanical strength, and electrode interface stability. Polyethylene oxide (PEO) is a significant SPE material, offering lithium salt complexation and flexible processability. Its high crystallinity causes poor IC at room temperature and uncontrollable lithium dendrite growth, which are hindering ASSLB commercialization. In this review, we mainly summarize three optimization synthesis strategies for PEO‐based SPEs: (1) Optimizing PEO molecular design: Reducing the crystallinity of PEO through the molecular structure design of linear, cross‐linked, and hyperbranched copolymers elevates the room‐temperature IC of the electrolyte to 10 −5 –10 −4 S·cm −1 . (2) Doping or modification: Introducing inert, active, and functional fillers for the doping modification of PEO‐based electrolytes effectively promotes lithium salt dissociation and suppresses lithium dendrite growth. Inert fillers can enhance the room‐temperature IC of the electrolyte by 50‐fold. (3) Advanced material preparation methods: Employing advanced fabrication techniques such as solution casting, electrospinning, 3D printing, and doctor blading optimizes the microstructure of PEO‐based electrolytes to enhance overall performance. For instance, electrolytes prepared by automated doctor‐blading exhibit a conductivity of 2.19 × 10 −4 S·cm −1 at 17°C. Although these strategies improve cyclic stability and safety, their performance at room temperature remains below commercial standards. Therefore, future research should focus on multiscale characterization techniques to delve into the electrode/electrolyte interface mechanisms for fabricating high‐energy‐density, long‐life ASSLBs.
Photoreduction of CO2 and H2O to CH4 offers a sustainable pathway for solar-to-chemical energy conversion. However, premature desorption of the CO* intermediate before coupling with protons (H*) to form a CHO* intermediate remains a major bottleneck, severely suppressing CH4 selectivity. Herein, we design a novel biomimetic "nucleus-cytoplasm" configuration photocatalyst, Pd1(C)/Ns/CNNs, where atomically dispersed Pd single atoms (Pd1(C)) serve as the cytoplasm for selective CO2 activation, while the adjacent Pd nanosheets (PdNs) act as the "nucleus" to supply H* and catalyze downstream hydrogenation. This configuration induces a short-range internal electric field, analogous to intracellular signaling, which synchronizes electron-H* transfer, facilitates directional CO* migration toward the "nucleus", and restrains premature desorption, enabling CHO* formation seamlessly. Experimental results and density functional theory calculations show that Pd1(C) binds and activates CO2, while PdNs stabilize CO* and promote H2O dissociation to generate H*. Ab initio molecular dynamics simulations capture the CO*-H* coupling into CHO*, directly visualizing this key transformation step. As a result, the Pd1(C)/Ns/CNNs achieves an outstanding CH4 evolution rate of 876.8 µmol g-1 h-1 with nearly 100% selectivity. This work introduces a biologically inspired spatial design that regulates intermediate evolution via local electronic synergy, providing a new idea for highly efficient and selective CO2 photomethanation.
More recently, aqueous fluoride-ion batteries (FIBs) have attracted significant attention due to their high theoretical energy density, enhanced safety, low cost, and rapid charge/discharge capabilities. However, a large number of active water molecules in the aqueous electrolyte leads to instability of the electrolyte and the dissolution of the active materials. Herein, a novel strategy is proposed to disrupt the hydrogen bond network of water molecules by designing a KF-H2O-sulfolane hybrid electrolyte, which enables reversible fluorination/ defluorination reactions at both the positive electrode and negative electrode. The results confirm that sulfolane can effectively break the hydrogen bond network, optimize the solvation shell structure, and suppress H2O activity, thereby minimizing HF generation. It has been found that the optimized electrolyte provides over 500 h of long-term cycling stability and an expanded electrochemical stability window (-2.0 to 1.53 V vs. Ag/AgCl). When the optimized electrolyte is applied in a Pb//BiF3 cell, the cell delivers a high initial discharge capacity (301 mAh g- 1). Therefore, this work provides fundamental insights into electrolyte design principles for aqueous FIBs, demonstrating a viable pathway to achieve both high energy density and long-term stability in FIB systems.
ABSTRACT Aqueous zinc‑iodine (Zn‐I 2 ) batteries demonstrate significant potential for large‑scale energy storage, yet their practical application remains hindered by polyiodide shuttling at the cathode and uncontrolled Zn dendrite growth at the anode. In this work, an asymmetric twist molecule (ATM) was designed, which disrupts the equilibrium of molecular charge distribution and spatial steric effects. The rigid twist backbone locks the amino and carboxyl groups in a fixed orientation, generating a permanent molecular dipole that creates a stable local electrostatic field. This field adsorbs iodide ions, suppressing iodine hydrolysis and preventing polyiodide migration. Meanwhile, the oriented local electric field homogenizes the Zn 2+ flux and mitigates dendrite formation at the Zn anode, enabling uniform Zn deposition. Consequently, experimental results demonstrate that the Zn‐I 2 battery delivers a reversible capacity of 235 mAh g −1 under a high loading of 7.3 mg cm −2 . Furthermore, the ATM containing Zn//Zn symmetric cell exhibits an ultralong cycling lifespan exceeding 6100 h at 1 mA cm −2 . This study proposes a feasible technical pathway for constructing highly stable aqueous Zn‐I 2 batteries through the concept of asymmetric twist molecular design.
Metal-organic frameworks (MOFs)-based composite polymer electrolytes (CPEs) face critical challenges in solidstate battery applications, including the interfacial incompatibility between the rigid MOF lattice and flexible polymer segments, as well as nanoparticle agglomeration. This study innovatively proposes a synergistic strategy combining topological network construction and Lewis acid site enhancement. By the combined effect of the Lewis acid site (-Al-OH) of MOF-808 (Al) and the polar environment of beta-phase Polyvinylidene difluoride (PVDF) effectively, the Na+ transference number is significantly enhanced to 0.62. Constructing an efficient ion transport channel dominated by Solvent-Separated Ion Pairs (SSIP), achieving a high ionic conductivity of 1.07 x 10-3 S cm- 1. Moreover, the unique topological network structure effectively suppresses MOF particle agglomeration while synergizing with the MOF-808 (Al) component to promote the rapid formation of a stable solid electrolyte interphase layer, effectively suppressing sodium dendrite growth. The resulting electrolyte achieves a critical current density to 0.8 mA cm-2 and demonstrates ultralong cycling stability (800 h at 0.1 mA cm-2). The assembled Na|6 % MOF@PPN|Na3V2(PO4)3 battery retains a high capacity retention rate of 88 % after 500 cycles at 0.5C, demonstrating its tremendous potential for the development of high-performance solid-state batteries.
Abstract Electrocatalytic nitrate reduction (eNO3−RR) is widely recognized as sustainable green ammonia production strategy. However, the complex adsorption–activation–hydrogenation behavior of multiple nitrogen-oxygen intermediates and the intrinsic mismatch in proton-coupled electron transfer kinetics severely hinder the NH3 yield. Herein, a structurally engineered FeCo-MOF electrocatalyst featuring an asymmetric Co−O−Fe center was constructed via competitive coordination. The unique electronic orbital distribution in the Co−O−Fe bimetallic center promotes O-mediated charge transfer from Co to Fe. This charge redistribution induces enhanced electronic localization and asymmetry within the Co−O−Fe unit, thereby facilitating the activation and reduction of nitrogen-oxygen intermediates. Notably, in this asymmetric electronic configuration, the Co site enables efficient electron provisioning and promotes water dissociation to generate active hydrogen (Hads) species, ensuring well-matched proton-coupled electron transfer kinetics and accelerating the rapid conversion of the key *NO intermediate on electron-enriched Fe sites. Theoretical calculations further demonstrate that the asymmetric Co−O−Fe motif significantly lowers the thermodynamic barrier of *NO → *NOH step. The catalyst delivers a NH3 production rate of 0.653 mmol cm−2 h−1 (1306 mmol gcat−1 h−1) with a near-unity Faradaic efficiency of 99.8%. This study provides comprehensive insights into optimizing proton-coupled electron transfer dynamics and elucidating structure-performance relationships for advanced green-ammonia electrocatalysis.
The concentration of dissolved oxygen is pivotal to the corrosion resistance of structural materials in lead-cooled fast reactor (LFR), which in turn has a substantial influence on operational safety. This study focuses on achieving precise prediction of oxygen variation trends in the liquid lead-bismuth eutectic (LBE) represented by electromotive force, with temperature serving as an assisting parameter. A novel forecasting approach, named Feature-Enhanced Variant Attention Network (FEVA-Net), is proposed. This approach is based on a hybrid neural network of CNN-BiLSTM incorporated with a variant attention mechanism. In this paper, experimental data were acquired from the LBE loop facility, KYLIN-II-M. A comprehensive verification process, involving multi-dimensional comparative experiments, was carried out to demonstrate the validity of the proposed method. The results reveal the superior performance of FEVA-Net over the EMD-CNNBiLSTM model across several key metrics. Specifically, improvements in RMSE, MAE, MAPE, and R2 are observed, with average enhancements of 31.40 %, 43.58 %, 2.05 %, and 4.17 %, respectively. This study illustrates the promising accuracy of the proposed model, especially for dissolved oxygen process in practice.
Gel polymer electrolytes combine the advantages of solid and liquid electrolytes, making them promising electrolyte candidates for lithium-metal batteries. However, low-temperature performance is hindered by sluggish ion transport and unstable electrolyte–electrode interfaces. Herein, a topology-driven solvation-decoupling strategy is proposed by designing a topological ester-based polymer electrolyte with dynamically polar side chains, enabling high-voltage lithium-metal batteries to operate reliably at low temperatures. This strategy dynamically reconstructs the local solvation environment within ester electrolytes, which simultaneously enhances lithium salt dissociation and lowers the desolvation energy barrier. The electrolyte exhibits ionic conductivities of 2.39 × 10−3 and 2.1 × 10−4 S cm−1 at 25 ℃ and −30 ℃, respectively, with a Li+ transference number of 0.76. Moreover, the tailored electrolyte composition stabilizes both lithium metal anodes and high-voltage cathodes (LiNi0.6Co0.2Mn0.2O2 and LiCoO2), enabling polymer-based cells to operate below −30 ℃. At −20 ℃ and 0.1 C, Li||LiNi0.6Co0.2Mn0.2O2 cells deliver a high discharge capacity of 151.3 mA h g−1 (>85% of that at 25 ℃). Notably, a Li||LiNi0.6Co0.2Mn0.2O2 pouch cell with a mass loading of 11.7 mg cm−2 can be stably cycled at −30 ℃. The Li||LiNi0.6Co0.2Mn0.2O2 cells demonstrate outstanding stability over a broad temperature range. This study provides a feasible strategy for designing high-performance gel polymer electrolytes for high-voltage lithium-metal batteries at extreme temperatures.
ABSTRACT The development of ultrathin, high ionic conductivity sulfide solid‐state electrolytes (SSEs) film is essential for achieving high‐energy‐density all‐solid‐state batteries (ASSBs). However, conventional chemically inert binders inevitably impede Li‐ion transport kinetics within SSE films, and the underlying Li‐ion transport mechanisms remain elusive. In this work, we report an Li‐ion‐conductive polymer binder (LiTFSI‐PMEMA) and integrate it with SSEs via dry processing to fabricate an ultrathin SSE film (USF). The resulting USF is only 18 µm thick and exhibits a high ionic conductivity of 1.56 mS cm ‒1 . By combining cryogenic transmission electron microscopy (cryo‐TEM), solid‐state nuclear magnetic resonance (ssNMR), and theoretical simulations, we propose an Li + transport model in which the SSE phase provides the dominant conduction pathway, while the polymer binder and SSEs/polymer contact regions can assist local Li + transport continuity between neighboring SSE particles. When implemented in ASSBs, the USF exhibits exceptional interfacial compatibility and kinetic stability, enabling a long‐term cycling life with 70.3% capacity retention over 1500 cycles. Furthermore, a LiNi 0.7 Co 0.2 Mn 0.1 O 2 ||USF||nSi pouch cell delivers a high stack‐level energy density of 322.7 Wh kg ‒1 . This work provides crucial insights into the multiphase Li‐ion transport kinetics and demonstrates a scalable manufacturing strategy for sulfide‐based ASSBs.
Li-rich Mn-based oxide (LRMO) cathodes represent promising candidates for high-energy-density all-solid-state lithium batteries (ASSLBs). Nonetheless, irreversible oxygen release and sluggish transport kinetics result in faded voltage and degraded cycling stability, severely impeding their practical applications in ASSLBs. Herein, a high-quality artificial interface layer was constructed on the LRMO surface via a facile sol–gel method followed by thermal treatment, yielding a Li3ScF6 protective layer comprising a Li3ScF6 surface coating region and a subsurface Sc doping region. Specifically, Li3ScF6 surface coating effectively suppresses continuous interfacial side reactions between the cathode and solid electrolyte, thereby improving interfacial transport kinetics; the strong Sc–O bond stabilizes the lattice oxygen framework and inhibits oxygen release, thereby enhancing the reversibility of the oxygen redox reaction. Consequently, the ASSLBs with the modified LRMO cathode exhibit remarkable fast-charging capability (136.8 mAh g−1 at 1.0 C) and excellent capacity retention (83.9
The development of ultrathin, high ionic conductivity sulfide solid-state electrolytes (SSEs) film is essential for achieving high-energy-density all-solid-state batteries (ASSBs). However, conventional chemically inert binders inevitably impede Li-ion transport kinetics within SSE films, and the underlying Li-ion transport mechanisms remain elusive. In this work, we report an Li-ion-conductive polymer binder (LiTFSI-PMEMA) and integrate it with SSEs via dry processing to fabricate an ultrathin SSE film (USF). The resulting USF is only 18 µm thick and exhibits a high ionic conductivity of 1.56 mS cm‒1. By combining cryogenic transmission electron microscopy (cryo-TEM), solid-state nuclear magnetic resonance (ssNMR), and theoretical simulations, we propose an Li+ transport model in which the SSE phase provides the dominant conduction pathway, while the polymer binder and SSEs/polymer contact regions can assist local Li+ transport continuity between neighboring SSE particles. When implemented in ASSBs, the USF exhibits exceptional interfacial compatibility and kinetic stability, enabling a long-term cycling life with 70.3% capacity retention over 1500 cycles. Furthermore, a LiNi0.7Co0.2Mn0.1O2||USF||nSi pouch cell delivers a high stack-level energy density of 322.7 Wh kg‒1. This work provides crucial insights into the multiphase Li-ion transport kinetics and demonstrates a scalable manufacturing strategy for sulfide-based ASSBs.
Integrating ultrathin inorganic electrolyte films with high-voltage oxide cathodes and low-potential Li anodes in all-solid-state Li-metal batteries (ASSLMBs) emerges as a compelling strategy to overcome the 400 Wh kg(-1) threshold. However, plagued by narrow electrochemical windows, standalone halide or sulfide films struggle to sustain compatibility with high-capacity electrodes, triggering irreversible interfacial degradation. Herein, leveraging halide-sulfide bilayer film architecture, the wet-coated 40-mu m Li2.6In0.8Ta0.2Cl6-Li5.3PS4.3ClBr0.7 (LITC-LPSCB) film achieves high ionic conductivity (1.76 mS cm(-1)), expanded electrochemical window, and decent mechanical durability. Multiscale simulations and experimental characterizations validate superior interfacial compatibility across cathode-electrolyte-anode interfaces. Furthermore, to streamline fabrication protocols and enhance mechanical durability, a facile cathode-electrolyte integrated film design is adopted. When paired with LiNi(0.85)Co(0.1)Mn(0.0)5O(2) cathodes and Li anodes, film-type cells exhibit superior cycling stability (82.9% after 800 cycles at 0.5 C) and rate capability (133.6 mAh g(-1) at 1.0 C), outperforming pellet-type counterparts. Remarkably, when extended to high-voltage (4.7 V) Li-rich Mn-based oxide cathodes, film-type cells attain a promising 433.5 Wh kg(-1) at 5.21 mAh cm(-2) areal capacity and maintain stability over 200 cycles. This work provides a scalable bilayer film coupled with an integrated film architecture design, accelerating the practical deployment of high-energy ASSLMBs.
Sulfide solid electrolytes (SEs) are considered a top contender for next-generation energy storage systems due to their high ionic conductivity and relatively “soft” mechanical properties. Nevertheless, interface hydrolysis in air and reduction at the Li/SE interface hinder their practical application in all-solid-state batteries. In this work, a novel chemically stabilized argyrodite-based SE Li5.58P0.96Ga0.04S4.5Cl1.38F0.12 was developed by co-doping Ga, F in Li5.5PS4.5Cl1.5 (LPSC), which has an excellent ionic conductivity of 4.5 mS/cm at 25 °C. Notably, the co-doping strategy promotes the formation of lithium-friendly Li–Ga alloys and electron-insulating LiF at the Li/SE interface, which plays an essential role in regulating the uniform plating/stripping of Li+ and suppressing the interfacial side reactions. The Li symmetric cells exhibit a high critical current density of 1.8 mA/cm2 and stable cycling for 2,000 h at 0.2 mA/cm2. Furthermore, the Ga, F co-doped electrolyte exhibits substantial structural stability at 30% relative humidity, further demonstrated by the density functional theory calculations. When paired with LiNi0.8Co0.1Mn0.1O2 or LiCoO2 cathodes, the all-solid-state lithium metal cells demonstrate outstanding cycle stability and rate performance. Owing to their superior air stability and compatibility with Li metal, Ga/F co-doped LPSCs are poised to become the next generation of all-solid-state lithium batteries.
Anode-free lithium metal batteries offer high energy density and low cost, but their practical deployment is limited by unstable lithium-electrolyte interfaces and safety risks from dendrite growth and flammable electrolytes. Here, we report a dual-functional fluorinated additive that enables in situ gelation, forming a thin, inorganic-rich solid electrolyte interphase while simultaneously enhancing flame retardancy through radical capture. At 0.5 C discharge, the additive-enabled anode-free pouch cell delivers high specific capacities of 202.1 mAh/g (3.0-4.5 V) and 192.0 mAh/g (3.4-4.3 V), while retaining 80.3% and 80.1% of their initial values after 85 and 100 cycles, respectively. Moreover, Cu/NCA pouch cells with capacities of 1.4 Ah (3.0-4.5 V) and 200 mAh (3.6-4.3 V), incorporating the additive, retain 80.2% of initial capacity after 85 cycles and 92.9% after 100 cycles, respectively. Such performance is on par with or better than the best results in the literature. Impressively, such a 1.4 Ah cell shows no thermal runaway in a harsh drilling test at the fully charged state, even after 100 cycles. These results demonstrate that the dual-functional fluorine additive leads to both excellent electrochemical performance and enhanced safety, paving the way for the safe and practical application of anode-free lithium metal cells.
Garnet-type Li7La3Zr2O12 (LLZO) solid electrolytes exhibit high bulk ionic conductivity but suffer from poor interfacial compatibility with polymer matrices and lithium metal, due to surface Li2CO3 formation and high interfacial resistance. Here, we construct a dual-functional interfacial structure via sequential in situ phosphating and silane grafting. The phosphating forms a Li3PO4 layer, which chemically bonded to LLZO with P & horbar;O & horbar;La covalent bonds, serving as an ionic bridge to lower Li+ transport barriers. Silane grafting creates a flexible, cross-linked network, transforming the filler surface from rigid to viscoelastic. The dual-coated LLZO enables uniform dispersion in PEO/PAN blends, establishing continuous ionconducting pathways with a stress-dissipative framework. This enables the composite electrolyte to achieve a high ionic conductivity of 2.82 x 10 -4 S cm -1 while exhibiting exceptional mechanical integrity. Li symmetric cells cycle stably for over 2000 h at 0.4 mA cm-2, and cells coupled with LiFePO4 or LiNi0.8Co0.1Mn0.1O2 cathode deliver high-capacity retention over extended cycling. This work elucidates a synergistic interface-engineering mechanism where the inner Li3PO4 layer optimizes ion transfer kinetics and the outer silane network ensures lithium dendrite suppression, collectively overcoming the long-standing trade-off between ionic conductivity and interfacial stability in garnet-based composite solid-state electrolytes.
Formaldehyde (HCHO), a toxic volatile organic compound. Herein, we report generating Pt, Ag and Mn metal and metal oxide nanoparticles via thermal treatment of coordinated complexes of metal ions with polyacrylic acid anchored on graphene oxide (GO) for efficient electrochemical catalytic removal of HCHO. Reversible addition-fragmentation chain transfer (RAFT) polymerization is first utilized to synthesize pyrene-terminated polyacrylic acid (PyPAA) with controlled number of acid functionalities for complexing metal ions, followed by self-assembly on GO to form polymer/graphene oxide composite (PyPAA/GO). The PyPAA/GO composite is then complexed with metal ions through its acrylic acid groups to afford metal ions tethered polymer/graphene oxide composites (MI-PyPAA/GO), followed by thermal treatment to afford metal nanoparticle-loaded reduced graphene oxide (MP/rGO) composites. Notably, the catalytic efficiency of the MP/rGO composites for HCHO decomposition demonstrates a positive correlation with the anchored metal content in the composite material, which can be attributed to the increased density of catalytical active sites associated with higher metal loading. Among the three MP/rGO composites, Mn3O4/rGO exhibits the highest HCHO decomposition efficiency of 50.70%, surpassing those of Pt/rGO (42.78%) and Ag/rGO (40.90%). The current method provides an effective means to prepare metal or metal oxide manocatalysts with improved catalytical efficiency of HCHO decomposition.
For developing high-energy-density all-solid-state sulfide batteries (ASSBs), large-area sulfide electrolyte films produced via wet processes hold great potential. However, it is still a major obstacle in the wet process of sulfide membranes to find suitable polymer binders with excellent (electro)chemical compatibility and bonding properties. Here, we not only employ a terpolymer adhesive (Poly(ethylene-co-methyl acrylate-co-glycidyl methacrylate)) with polar-nonpolar synergistic effects to facilitate the wet-process manufacture of sulfide-based films, but also adopt a sulfide electrolyte prepared without expensive Li2S to reduce raw material costs. The sulfide-based electrolyte film (terP-SF) features an ultra-thin thickness (32 mu m), favorable mechanical properties, and high ionic conductivity (1.32 mS/cm). For electrochemical performance, the terP-SF has fast ion transport kinetics and electrical insulation, which enables the NCM83//terP-SF//In-Li battery to deliver high-rate performance and long-term cycling stability (with a capacity retention rate of approximately 76.6% after 600 cycles). Furthermore, given the cost-effectiveness of scaled-up production of ASSB, a pouch cell configured as NCM83//terP-SF//Si with an energy density of 320.4 Wh/kg and volumetric energy of 710.7 Wh/L is successfully assembled. This work inspires the selection of binders in wet-process film formation and further guides the resolution of engineering and scientific challenges in the commercialization of high-energy-density and low-cost ASSBs.
Li-rich Mn-based layered oxides (LLOs) are promising cathode materials for next-generation lithium-ion batteries due to their ultra-high capacity exceeding 250 mAh g-1. However, their practical application is severely hindered by oxygen release, phase transitions, and undesirable voltage decay. Herein, we propose a synergistic W/B co-doping strategy to stabilize lattice oxygen and enhance structural robustness. The synergistic effect of co-doping regulates the electronic density of states of lattice oxygen by modulating the It-type hybridization between O 2p and TM t2g orbitals and forming robust BO4 units with lower Bader charge. It results in the O 2p band center away from the Fermi level, which effectively suppresses undesirable oxygen release during high-voltage operation. In addition, B3+ ions in tetrahedral sites truncate TM migration pathways, thus mitigating phase transitions. As a result, the modified LLOs (WB-LLO) exhibit significantly improved capacity retention (88.0%, 300 cycles) and voltage stability (0.45 mV/cycle, 100th-300th cycle) at 0.5 C. Furthermore, the universality of this strategy was validated in Ti/B, Zr/B, and Nb/B co-doped systems, all showing enhanced cycling stability. This work provides new insights to regulate oxygen chemistry of LLOs by shifting O 2p band center.
Efficient bubble management is critical for sustaining high-current-density hydrogen evolution (HER) in anion exchange membrane water electrolysis (AEMWE). Herein, we construct a micro/nanostructured interface on nickel felt (FLN) via femtosecond laser processing to accelerate hydrogen bubble release. The optimized FLN-2 electrode achieves low overpotentials of 195 mV at 500 mA cm-2 and 219 mV at 1000 mA cm-2, respectively, for the alkaline HER. In situ bubble visualization and adhesion-force measurements reveal that FLN-2 promotes bubble detachment by reducing bubble adhesion from 0.091 to 0.035 mN. A hydrophobic control electrode further supports the important role of wettability-regulated bubble transport in high-current-density operation. A 100 cm2 AEMWE device employing the micro/nanostructured electrode configuration maintains stable operation at 1000 mA cm-2 with a cell voltage of approximately 1.997 V over 100 h. This work highlights femtosecond laser structuring as a scalable interfacial engineering route for practical gas-evolving electrodes.