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Hybrid halide perovskites are good candidates for a range of functional materials such as optical electronic and photovoltaic devices due to their tunable band gaps, long carrier diffusion lengths, and solution processability. However, the instability in moisture/air, the toxicity of lead, and rigorous reaction setup or complex postprocessing have long been the bottlenecks for practical application. Herein, we present a simultaneous configurational entropy design at A-sites, B-sites, and X-sites in the typical (CHA)2PbBr4two-dimensional (2D) hybrid perovskite. Our results demonstrate that the high-entropy effect favors the stabilization of the hybrid perovskite phase and facilitates a simple crystallization process without precise control of the cooling rate to prepare regular crystals. Moreover, high-entropy 2D perovskite crystals exhibit tunable energy band gaps, broadband emission, and a long carrier lifetime. Meanwhile, the high-entropy composition almost maintains the initial crystal structure in deionized water for 18 h while the original (CHA)2PbBr4crystal mostly decomposes, suggesting obviously improved humidity stability. This work offers a facile approach to synthesize humidity-stable hybrid perovskites under mild conditions, accelerating relevant preparation of optoelectronics and light-emitting devices and facilitating the ultimate commercialization of halide perovskite.

Polar metals have recently garnered increasing interest because of their promising functionalities. Here we report the experimental realization of an intrinsic coexisting ferromagnetism, polar distortion and metallicity in quasi-two-dimensional Ca3Co3O8. This material crystallizes with alternating stacking of oxygen tetrahedral CoO4monolayers and octahedral CoO6bilayers. The ferromagnetic metallic state is confined within the quasi-two-dimensional CoO6layers, and the broken inversion symmetry arises simultaneously from the Co displacements. The breaking of both spatial-inversion and time-reversal symmetries, along with their strong coupling, gives rise to an intrinsic magnetochiral anisotropy with exotic magnetic field-free non-reciprocal electrical resistivity. An extraordinarily robust topological Hall effect persists over a broad temperature–magnetic field phase space, arising from dipole-induced Rashba spin–orbit coupling. Our work not only provides a rich platform to explore the coupling between polarity and magnetism in a metallic system, with extensive potential applications, but also defines a novel design strategy to access exotic correlated electronic states.

MXene inks offer a promising avenue for the scalable production and customization of printing electronics. However, simultaneously achieving a low solid content and printability of MXene inks, as well as mechanical flexibility and environmental stability of printed objects, remains a challenge. In this study, we overcame these challenges by employing high-viscosity aramid nanofibers (ANFs) to optimize the rheology of low-concentration MXene inks. The abundant entangled networks and hydrogen bonds formed between MXene and ANF significantly increase the viscosity and yield stress up to 103Pa·s and 200 Pa, respectively. This optimization allows the use of MXene/ANF (MA) inks at low concentrations in direct ink writing and other high-viscosity processing techniques. The printable MXene/ANF inks with a high conductivity of 883.5 S/cm were used to print shields with customized structures, achieving a tunable electromagnetic interference shielding effectiveness (EMI SE) in the 0.2–48.2 dB range. Furthermore, the MA inks exhibited adjustable infrared (IR) emissivity by changing the ANF ratio combined with printing design, demonstrating the application for infrared anticounterfeiting. Notably, the printed MXene/ANF objects possess outstanding mechanical flexibility and environmental stability, which are attributed to the reinforcement and protection of ANF. Therefore, these findings have significant practical implications as versatile MXene/ANF inks can be used for customizable, scalable, and cost-effective production of flexible printed electronics.

Ferroelectricity, especially the Si-compatible type recently observed in hafnia-based materials, is technologically useful for modern memory and logic applications, but it is challenging to differentiate intrinsic ferroelectric polarization from the polar phase and oxygen vacancy. Here, we report electrically controllable ferroelectricity in a Hf0.5Zr0.5O2-based heterostructure with Sr-doped LaMnO3, a mixed ionic–electronic conductor, as an electrode. Electrically reversible extraction and insertion of an oxygen vacancy into Hf0.5Zr0.5O2are macroscopically characterized and atomically imaged in situ. Utilizing this reversible process, we achieved multilevel polarization states modulated by the electric field. Our study demonstrates the usefulness of the mixed conductor to repair, create, manipulate, and utilize advanced ferroelectric functionality. Furthermore, the programmed ferroelectric heterostructures with Si-compatible doped hafnia are desirable for the development of future ferroelectric electronics.

Electrical control of magnetism is highly desirable for energy-efficient spintronic applications. Realizing electric-field-driven perpendicular magnetization switching has been a long-standing goal, which, however, remains a major challenge. Here, electric-field control of perpendicularly magnetized ferrimagnetic order via strain-mediated magnetoelectric coupling is reported. We show that the gate voltages isothermally toggle the dominant magnetic sublattice of the compensated ferrimagnet FeTb at room temperature, showing high reversibility and good endurance under ambient conditions. By implementing this strategy in FeTb/Pt/Co spin valves with giant magnetoresistance (GMR), we demonstrate that the distinct high and low resistance states can be selectively controlled by the gate voltages with assisting magnetic fields. Our results provide a promising route to use ferrimagnets for developing electric-field-controlled, low-power memory and logic devices.

Owing to their excellent discharged energy density over a broad temperature range, polymer nanocomposites offer immense potential as dielectric materials in advanced electrical and electronic systems, such as intelligent electric vehicles, smart grids and renewable energy generation. In recent years, various nanoscale approaches have been developed to induce appreciable enhancement in discharged energy density. In this Review, we discuss the state-of-the-art polymer nanocomposites with improved energy density from three key aspects: dipole activity, breakdown resistance and heat tolerance. We also describe the physical properties of polymer nanocomposite interfaces, showing how the electrical, mechanical and thermal characteristics impact energy storage performances and how they are interrelated. Further, we discuss multi-level nanotechnologies including monomer design, crosslinking, polymer blending, nanofiller incorporation and multilayer fabrication. We conclude by presenting the current challenges and future opportunities in this field.

Abstract

In a recent study published in Angewandte Chemie, Li and colleagues report that introducing disorder into Li5.5PS4.5ClxBr1.5−xsolid electrolytes via Cl−/Br−/S2−mixing affects charge transport, leading to a room temperature ionic conductivity beyond 20 mS/cm. This entails the possibility of improving ion mobility by tailoring the occupational disorder in lithium argyrodites.

Flexible polymer nanocomposites reinforced by high-dielectric-constant ceramic nanofillers have shown great potential for dielectric energy storage applications in advanced electronic and electrical systems. However, it remains a challenge to improve their energy density and energy efficiency at high temperatures above 150°C. Here, we report a nanofiber-reinforced polyetherimide nanocomposite employing BN-BaTiO3heterogeneous nanofibers as fillers, where the BN nanoparticles were embedded inside BaTiO3nanofibers to create BN/BaTiO3/PEI hierarchical interfaces. The high dielectric constant and the geometric large aspect ratio of the BN-BaTiO3heterogeneous nanofibers lead to simultaneously increased dielectric constant and breakdown strength of the nanocomposite over a broad temperature range. In particular, the emerging hierarchical BN/BaTiO3/PEI interfaces enable promoted density and energy level of traps for the mobile charges, which further suppresses the conduction loss and improves the breakdown strength under high temperatures, as confirmed by a combination of thermally stimulated depolarization current measurement and phase-field simulation. Finally, the nanocomposite with hierarchical interfaces boosts an ultrahigh energy density of 5.23 J cm−3with an energy efficiency of > 90% at 150°C, which is the highest energy density reported so far in nanofiber-reinforced polymer nanocomposites and also outperforms most nanocomposites counterparts dispersed with nanoparticles and nanosheets. Our work demonstrates hierarchical interface engineering as an effective strategy to promote the high-temperature energy storage performance of fiber-reinforced polymer nanocomposites, which is of significance for their applications in high-temperature harsh conditions.

The Jahn–Teller effect (JTE) arising from lattice–electron coupling is a fascinating phenomenon that profoundly affects important physical properties in a number of transition-metal compounds. Controlling JT distortions and their corresponding electronic structures is highly desirable to tailor the functionalities of materials. Here, we propose a local coordinate strategy to regulate the JTE through quantifying occupancy in the ${{d}_{{{z}^2}}}$and ${{d}_{{{x}^2} - {{y}^2}}}$orbitals of Mn and scrutinizing the symmetries of the ligand oxygen atoms in MnO6octahedra in LiMn2O4and Li0.5Mn2O4. The effectiveness of such a strategy has been demonstrated by constructing P2-type NaLixMn1–xO2oxides with different Li/Mn ordering schemes. In addition, this strategy is also tenable for most 3dtransition-metal compounds in spinel and perovskite frameworks, indicating the universality of local coordinate strategy and the tunability of the lattice–orbital coupling in transition-metal oxides. This work demonstrates a useful strategy to regulate JT distortion and provides useful guidelines for future design of functional materials with specific physical properties.This work provides a general orbital engineering strategy to regulate the Jahn-Teller distortion and will inspire continued efforts to design structures with different physical properties for functional materials.

Emergent topological textures coupled with ferroic orders have become the promising basis for exotic phenomena and application advances. While the number of materials observed with polar topological textures is growing, manipulation of these emergent polar topologies with the aid of external stimuli (e.g. electric field, strain, thermal perturbation) remains rare. Here, we report a pyrotoroidic transition accompanying the Curie transition in face-on lamellae of poly(vinylidene fluoride-ran-trifluoroethylene) (P(VDF-TrFE)), with a chirality reversal revealed in the polar topology. The existence of toroidal order in paraelectric polymers has been validated by further confirming the toroidal order in face-on lamellae of relaxor ferroelectric polymer induced by physical defects. This work demonstrates the manipulation of polar topological texture with the controls of the thermal condition. It should also expand the reach of toroidal polar topologies to a range of flexible materials and offer an insight into their formation.

Polymer-based electrolytes have attracted ever-increasing attention for solid-state batteries due to their excellent flexibility and processability. Among them, poly(vinylidene difluoride) (PVDF)-based electrolytes with high ionic conductivity, wide electrochemical stability window, and good mechanical properties show great potential and have been widely investigated by using different Li salts, solvents, and inorganic fillers. Here, we report the influence of the molecular weight of PVDF itself on the electrochemical properties of the electrolytes by using two kinds of common PVDF polymers, i.e., PVDF 761 and 5130. Our results demonstrate that the electrolyte with a larger molecular weight (PVDF 5130) has a denser structure and lower crystallinity, and thus much better electrochemical performance, than one with a smaller molecular weight (PVDF 761). With PVDF 5130, the LiFePO4-based solid-state cells present a steady cycling performance with a capacity retention of 85% after 1000 cycles at 1 C and 30 °C. The cycle life of the LiCoO2-based solid-state cells is also extended by using PVDF 5130.

Lead-free relaxor ferroelectric ceramics are potential for energy storage applications due to their comprehensive energy storage properties. However, the energy efficiency of many relaxor ceramics is not high enough, leading to high Joule heat during the charge–discharge cycles, thus lowering their energy storage performance. In this work, tantalum (Ta) dopants were introduced into sodium niobate-based relaxor ceramics to improve the resistivity and energy efficiency. The leakage current was reduced by Ta doping, especially at the high electric field. The enhanced resistivity is attributed to the increased bandgap induced by Ta doping. The impedance spectroscopy shows that both the grain and grain boundary resistivities are improved in the high temperature region. As a result, the optimal recoverable energy density and energy efficiency are 6.5 J/cm3and 94% at 450 kV/cm, respectively. In addition, the energy storage properties exhibit satisfactory temperature stability and cycling reliability. All these merits demonstrate that the Ta modified sodium niobate-based relaxor ceramic a potential candidate for high-power energy storage applications.

All-solid-state batteries (ASSBs) by utilizing sulfide electrolytes (SEs) have recently attracted much attention because of their advantages such as high ionic conductivity and low processing temperature of SEs. To enhance the electrochemical properties of ASSBs such as areal capacity and cycle performance, it is highly desired to obtain an intimate contact between active materials and SEs in the cathode and decrease the content of non-active materials including electronically conductive carbon and SEs. In this work, a carbon-free composite cathode with CuS as the active material and lithium argyrodite Li5.5PS4.5Cl1.5(LPSCl) as the SE was prepared by ball milling. Due to the tight contact between LPSCl and CuS caused by ball milling, high theoretical specific capacity, and relatively large electronic conductivity of CuS, the ASSB with a composite cathode containing a CuS loading of 10.2 mg cm−2delivered a large initial discharge capacity of 434.3 mAh g–1electrodebased on the cathode mass and a high areal capacity of 5.5 mAh cm−2at room temperature. At a higher CuS loading of 20.4 mg cm−2, an ultrahigh areal capacity of 12.7 mAh cm−2and a calculated specific energy of 955 Wh kg–1electrodebased on the cathode were obtained at 60 °C. Our work demonstrates that the carbon-free, CuS-based composite cathode is a highly promising cathode for high-energy-density ASSBs.

Ferroelectric tunneling junctions have attracted intensive research interest due to their potential applications in high-density data storage and neural network computing. However, the prerequisite of an ultrathin ferroelectric tunneling barrier makes it a great challenge to simultaneously implement the robust polarization and negligible leakage current in a ferroelectric thin film, both of which are significant for ferroelectric tunneling junctions with reliable operating performance. Here, we observe a large tunneling electroresistance effect of ∼1.0 × 104% across the BiFeO3nanoisland edge, where the intrinsic ferroelectric polarization of the nanoisland makes a major contribution to tuning the barrier height. This phenomenon is beneficial from the artificially designed tunneling barrier between the nanoscale top electrode and the inclined conducting phase boundary, which is located between the rhombohedral-island and tetragonal-film matrix and arranged with the dislocation array. More significantly, the tunneling electroresistance effect is further improved to ∼1.6 × 104% by the introduction of photoinduced carriers, which are separated by the flexoelectric field arising from the dislocations.

In this paper, we review in view of their potential but also from the aspect of being potentially the most interesting examples of the non-intuitive composite effects, which provides an impression of the dynamic evolution and the future opportunities of non-intuitive composite effects, with many promising applications.

Manipulating the insulator–metal transition in strongly correlated materials has attracted a broad range of research activity due to its promising applications in, for example, memories, electrochromic windows and optical modulators1,2. Electric-field-controlled hydrogenation using ionic liquids3–6and solid electrolytes7–9is a useful strategy to obtain the insulator–metal transition with corresponding electron filling, but faces technical challenges for miniaturization due to the complicated device architecture. Here we demonstrate reversible electric-field control of nanoscale hydrogenation into VO2with a tunable insulator–metal transition using a scanning probe. The Pt-coated probe serves as an efficient catalyst to split hydrogen molecules, while the positive-biased voltage accelerates hydrogen ions between the tip and sample surface to facilitate their incorporation, leading to non-volatile transformation from insulating VO2into conducting HxVO2. Remarkably, a negative-biased voltage triggers dehydrogenation to restore the insulating VO2. This work demonstrates a local and reversible electric-field-controlled insulator–metal transition through hydrogen evolution and presents a versatile pathway to exploit multiple functional devices at the nanoscale.

Electrostatic dielectric capacitors are essential components in advanced electronic and electrical power systems due to their ultrafast charging/discharging speed and high power density. A major challenge, however, is how to improve their energy densities to effectuate the next-generation applications that demand miniaturization and integration. Here, we report a high-entropy stabilized Bi2Ti2O7-based dielectric film that exhibits an energy density as high as 182 J cm−3with an efficiency of 78% at an electric field of 6.35 MV cm−1. Our results reveal that regulating the atomic configurational entropy introduces favourable and stable microstructural features, including lattice distorted nano-crystalline grains and a disordered amorphous-like phase, which enhances the breakdown strength and reduces the polarization switching hysteresis, thus synergistically contributing to the energy storage performance. This high-entropy approach is expected to be widely applicable for the development of high-performance dielectrics.

Oxide-based ceramics could be promising thermoelectric materials because of their thermal and chemical stability at high temperature. However, their mediocre electrical conductivity or high thermal conductivity is still a challenge for the use in commercial devices. Here, we report significantly suppressed thermal conductivity in SrTiO3-based thermoelectric ceramics via high-entropy strategy for the first time, and optimized electrical conductivity by defect engineering. In high-entropy (Ca0.2Sr0.2Ba0.2Pb0.2La0.2)TiO3bulks, the minimum thermal conductivity can be 1.17 W/(m·K) at 923 K, which should be ascribed to the large lattice distortion and the huge mass fluctuation effect. The power factor can reach about 295 μW/(m·K2) by inducing oxygen vacancies. Finally, the ZTvalue of 0.2 can be realized at 873 K in this bulk sample. This approach proposed a new concept of high entropy into thermoelectric oxides, which could be generalized for designing high-performance thermoelectric oxides with low thermal conductivity.

Sulfide solid electrolytes (e.g., lithium thiophosphates) have the highest room-temperature ionic conductivity (∼10−2 S cm−1) among solid Li-ion conductors so far, and thus have attracted ever-increasing attention for high energy-density and safety all-solid-state batteries (ASSBs). However, interfacial issues between sulfide electrolytes and electrodes have been the main challenges for their applications in ASSBs. The interfacial instabilities would occur due to side reactions of sulfides with electrodes, poor solid-solid contact, and lithium dendrites during charge/discharge cycling. In this review, we analyze the interfacial issues in ASSBs based on sulfide electrolytes, and in particular, discuss strategies for solving these interfacial issues and stabilize the electrode-electrolyte interfaces. Moreover, a perspective of the interfacial engineering for sulfide-based ASSBs is provided.

AgSbSe2is a typical member of cubic I–V–VI2semiconductors, which are known for their extremely low lattice thermal conductivity (κl). However, the low electrical conductivity of AgSbSe2, below ∼10 S cm–1at room temperature, has hindered its thermoelectric performance. In this work, single-phase AgSbSe2bulk samples with much higher electrical conductivity were synthesized via self-propagating high-temperature synthesis (SHS) combined with spark plasma sintering (SPS) for the first time. Pb doping through the nonequilibrium process further increases the electrical conductivity to >100 S cm–1. Furthermore, continuously increased effective mass md*can be achieved upon Pb doping because of the multiple degenerate valence bands of AgSbSe2and the energy-filtering effect induced by in situ-formed nanodots. The simultaneous enhancement of both the electrical conductivity and Seebeck coefficient contributes to an unprecedentedly high average power factor of 6.75 μW cm–1K–2. Meanwhile, the introduced dense grain boundaries and point defects enhance the phonon scattering and consequently suppress κl, yielding a high ZTvalue of 1.2 at 723 K in AgSb0.94Pb0.06Se2. This study opens a new avenue for rapid, low-cost, large-scale production of AgSbSe2-based materials and demonstrates that Pb-doped AgSbSe2prepared via the SHS–SPS method is a promising candidate for thermoelectric applications.

Understanding the interface effect in dielectric nanocomposites is crucial to the enhancement of their performance. In this work, a data-driven interface design strategy based on high-throughput phase-field simulations is developed to study the interface effect and then optimize the permittivity and breakdown strength of nanocomposites. Here, we use two microscopic features that are closely related to the macroscopic dielectric properties, the thickness and permittivity of the interface phases, to evaluate the role of interfaces in experimental configuration, and thus provide quantitative design schemes for the interfacial phases. Taking the polyvinyl difluoride (PVDF)BaTiO3nanocomposite as an example, the calculation results demonstrate that the interfacial polarization could account for up to 83.6% of the increase in the experimentally measured effective permittivity of the nanocomposite. Based on the interface optimized strategy, a maximum enhancement of ∼156% in the energy density could be achieved by introducing an interface phase with d/r = 0.55 and εinterface/εfiller=0.036, compared to the pristine nanocomposite. Overall, the present work not only provides fundamental understanding of the interface effect in dielectric nanocomposites, but also establishes a powerful data-driven interface design framework for such materials that could also be easily generalized and applied to study interface issues in other functional nanocomposites, such as solid electrolytes and thermoelectrics.

Ionic conducting polymer electrolytes for solid-state lithium-ion batteries have attracted ever-increasing attention because of their decent ionic conductivity, flexibility, no liquid leakage, and good processability. Poly(vinylidene fluoride) (PVDF)-based polymer electrolytes have recently stood out among the polymer electrolytes due to their high room temperature ionic conductivity. However, the interface between PVDF-based polymer electrolytes and lithium metal decays over time until the batteries break down. Here, we introduce a small amount of poly(acrylic acid) (PAA) into a PVDF-based polymer electrolyte and synthesize an organic–organic composite electrolyte that alleviates the interfacial reaction with lithium metal, which shows great superiority over other modification methods such as coating. The cycle life of lithium symmetric cells is prolonged from 130 to 850 h at 0.44 mA cm–2due to the effective suppression of interfacial reaction. The much more stable interface also enables excellent cycle performance in a solid-state LiCoO2||Li cell at 30 °C with a capacity decay of 0.03% per cycle for 1000 cycles, which is much lower than that of a cell without blending PAA (0.13% per cycle for only 450 cycles). The results would shed light on the applications of PVDF-based polymer electrolytes in solid-state lithium metal batteries.

Bulk-type all-solid-state batteries (ASSBs) using sulfide solid electrolyte are considered as a promising alternative to commercial lithium-ion batteries owing to their high energy density and safety. However, cell energy density is often comparatively low due to use of a thick solid electrolyte separator and a lithium alloy as anode. For achieving high-performance ASSBs, creating a thin free-standing electrolyte with high-conductivity and good cycling stability against lithium anode is essential. In this work, we present Li6PS5Cl/poly(vinylidene difluoride) (LPSCl/PVDF) composite electrolytes prepared by a slurry method. The influence of the PVDF content on the microstructure, morphology, ionic conductivity and activation energy of the LPSCl/PVDF electrolytes is systematically investigated. Free-standing LPSCl/PVDF membranes with a thickness of 100–120 μm and a high ionic conductivity of about 1·10−3 S cm−1 at 25 °C are obtained. After adding PVDF to the LPSCl electrolyte, the cycling stability of the LPSCl electrolyte against lithium metal improves significantly. Therefore, LPSCl/PVDF composite electrolytes are promising candidates to be used in ASSBs.

A series of 20Li2O-30V2O5-(50-x)SiO2-xB2O3(mol.%) (x = 10, 20, 30, 40) glasses were prepared by the traditional melt-quenching synthesis. The amorphous nature of the glasses was determined by XRD, DSC and TEM investigations. FTIR measurement revealed the functional group of obtained glasses. And EDS results confirmed the presence and uniform distribution of elements in the glasses. 20Li2O-30V2O5-40SiO2-10B2O3(LVSB10) sample with the highest V4+ratio exhibited the best cycling capacity. In order to further improve cycling stability of LVSB10 sample, ball milling was employed to reduce the particle size. The ball milled LVSB10 sample (LVSB10-b) showed an improved first discharge capacity, cycling stability and rate capacity. EIS measurements showed that ball milling can effectively decrease charge transfer impedance and facilitate Li+ion diffusion. This work provides a new way to explore a new type of cathode materials for lithium ion batteries.

Two-dimensional (2D) materials have recently drawn tremendous attention because of their novel properties and potential applications in high-speed transistors, solar cells, and catalysts. Few-layer SnSe is a new member of the 2D family with excellent performance in optoelectronic and thermoelectric devices. It is necessary to synthesize few-layer SnSe nanosheets in large scale for various applications. In this work, we develop a scalable liquid-phase exfoliation method to synthesize high-quality crystalline SnSe nanosheets. The morphology and microstructure of SnSe nanosheets are systematically investigated with high-resolution transmission electron microscopy, atomic force microscopy, and Raman spectroscopy. The thinnest nanosheets are bilayered. The optical absorption properties of SnSe nanosheets from near-infrared to ultraviolet light are studied. It is worth noting that the band gap of the nanosheets monotonically increases with the reduction of the nanosheet thickness. The electronic structure of SnSe nanosheets with various thicknesses is calculated by first-principles calculations, the evolution of the band gap as a function of the nanosheet thickness is confirmed, and the mechanism of the band gap evolution is discussed. Our work paves the way for the scalable synthesis of 2D SnSe with tunable optical absorption and band gap, which has potential for use in photoelectronic and photocatalytic applications.

A most recent exciting research result in the area of solid-state batteries that has been accepted for publication by the journal Nature Energyis highlighted. The research designed a new type of inorganic solid electrolyte named “viscoelastic inorganic glass (VIGLAS)” electrolyte with the compositions of LiAlCl2.5O0.75and NaAlCl2.5O0.75. The newly developed solid electrolyte material showcases an exceptional degree of deformability at room temperature, high ionic conductivity (>1 mS/cm at room temperature) and high oxidation stability (up to 4.3 V vs.Li+/Li or Na+/Na). Using it as a catholyte enables a facile fabrication and a stable operation under practical stack pressure (＜0.1 MPa) of all-solid-state batteries. VIGLAS represents a new path in the design of promising solid electrolytes for realizing high performance all-solid-state batteries.

Lithium–oxygen (Li–O2) batteries with ultra-high theoretical specific energy (3500Whkg−1) have attracted significant attention, but the sluggish electrochemical processes of discharge product Li2O2lead to poor cycling stability. Redox mediators (RMs) as soluble catalysts are widely used to assist with the electrochemical formation/decomposition of Li2O2. However, the shuttle effect of RMs causes severe deterioration of both RMs and Li metal anodes. Herein, for the first time we synthesize a lithiated zeolite-based protective layer on Li anodes to mitigate the shuttle effect of 2,2,6,6-tetramethylpiperidinyloxy (TEMPO) in Li–O2batteries. The protective layer successfully blocks the migration of TEMPO toward the Li anode owing to the angstrom-level aperture size of lithiated zeolite. Due to the excellent redox-mediator-sieving capability of the protective layer, the cycle life of the Li−O2batteries is significantly prolonged more than ten times at a current density of 250mAg−1and a limited capacity of 500mAh g−1. This work demonstrates that the lithiated zeolite-based protective layer capable of molecular sieving is a facile and scalable way to mitigate the shuttle effect of RMs in Li–O2batteries.

Engineering ferromagnetism, by modulating its magnitude or anisotropy, is an important topic in the field of magnetism and spintronics. Among different types of magnetic materials, ferromagnetic insulators, in which magnetic moment unusually coexists with localized electrons, are of particular interest. Here, we report a remarkable interfacial enhancement of the ferromagnetism by adding one unit-cell LaAlO3adjacent to an insulating LaMnO3ultrathin film. The enhancement of ferromagnetism is explained in terms of charge transfer at the interface, as evidenced by X-ray absorption spectroscopy and ab initio calculations. This study demonstrates an effective and dramatic approach to modulate the functionality of ferromagnetic insulators, contributing to the arsenal of engineering techniques for future spintronics.