E‐field Control of the RKKY Interaction in FeCoB/Ru/FeCoB/PMN‐PT (011) Multiferroic Heterostructures

E‐field control of antiferromagnetic (AFM) orders is promising for the realization of fast, compact, and energy‐efficient AFM applications. However, as the AFM spins are strongly pinned, the E‐field control process is mainly based on the exchange bias regulation that usually confines at a low temperature. Here, a new magnetoelectric (ME) coupling mechanism for the modulation of AFM orders at room temperature is explored. Based on the FeCoB/Ru/FeCoB/(011) Pb(Mg_1/3Nb_2/3)O₃‐PbTiO₃ (PMN‐PT) synthetic antiferromagnetic (SAF) heterostructures, the external E‐field generates relative magnetization switching in the two ferromagnetic (FM) layers, leading the Ruderman–Kittel–Kasuya–Yosida (RKKY) interaction tuning. This voltage‐induced switching behavior can be repeated in a stable and reversible manner for various SAFs, which is a key challenge in the E‐field control of AFM coupling and is not resolved yet. The voltage‐induced RKKY interaction changes by analyzing the dynamic optical and acoustic modes is quantified, and with first‐principles calculations, it is found that the distortion of the Fermi surface by the lattice reconstruction is the key of the relative magnetization switching and RKKY interaction modulation. This voltage control of the RKKY interaction in ME heterostructures provides an easy way to achieve the next generation of AFM/FM spintronic applications.     

High‐Performance Integrated Self‐Package Flexible Li–O2 Battery Based on Stable Composite Anode and Flexible Gas Diffusion Layer

With the rising development of flexible and wearable electronics, corresponding flexible energy storage devices with high energy density are required to provide a sustainable energy supply. Theoretically, rechargeable flexible Li–O₂ batteries can provide high specific energy density; however, there are only a few reports on the construction of flexible Li–O₂ batteries. Conventional flexible Li–O₂ batteries possess a loose battery structure, which prevents flexibility and stability. The low mechanical strength of the gas diffusion layer and anode also lead to a flexible Li–O₂ battery with poor mechanical properties. All these attributes limit their practical applications. Herein, the authors develop an integrated flexible Li–O₂ battery based on a high‐fatigue‐resistance anode and a novel flexible stretchable gas diffusion layer. Owing to the synergistic effect of the stable electrocatalytic activity and hierarchical 3D interconnected network structure of the free‐standing cathode, the obtained flexible Li–O₂ batteries exhibit superior electrochemical performance, including a high specific capacity, an excellent rate capability, and exceptional cycle stability. Furthermore, benefitting from the above advantages, the as‐fabricated flexible batteries can realize excellent mechanical and electrochemical stability. Even after a thousand cycles of the bending process, the flexible Li–O₂ battery can still possess a stable open‐circuit voltage, a high specific capacity, and a durable cycle performance.     

Probing Energy Migration through Precise Control of Interfacial Energy Transfer in Nanostructure

A novel mechanistic strategy for probing the energy migration through constructing the interfacial energy transfer (IET) in a core–shell–shell nanostructure is reported. In this design, the trilayer nanostructure is composed of a sensitizing core, a migratory interlayer, and a detective shell layer that interact with each other only by IET and the latter two shell layers are nonresponsive to the incident irradiation. This model is well applied in investigating the energy migration over the Tb, Gd, and Yb sublattices, and the results show that the Gd sublattice holds the best energy migratory performance. Moreover, the finding of energy migration over the Yb sublattice enables the 808 nm excited long‐lived upconversion of Tb³⁺ and Eu³⁺, which exhibits unique time‐gating performance for information security. The results provide a facile and powerful nanosized model for an in‐depth understanding of the fundamentals involving lanthanide interactions, which will further help excite new chances for the frontier applications of lanthanide‐based luminescent materials.     

Recent Advances on Self‐Supported Arrayed Bifunctional Oxygen Electrocatalysts for Flexible Solid‐State Zn–Air Batteries

Flexible solid‐state Zn–air batteries have been rapidly developed benefiting from the uprising demand for wearable electronic devices, wherein the air electrode integrated with efficient bifunctional oxygen electrocatalysts plays an important role to achieve high performance. Binder‐free self‐supported bifunctional catalysts can provide large active surface area, fast electron transport path, easy ion diffusion, and excellent structural stability and flexibility, thus acting as promising flexible air cathodes. In this review, recent advances on the application of nanoarrayed electrocatalysts as air cathodes in flexible Zn–air batteries are reviewed. Especially, various types of bifunctional oxygen electrocatalysts, including carbonaceous material arrays, transition metal compound arrays, transition metal/carbon arrays, transition metal compound/carbon arrays, and other hybrid arrays, are discussed. The applications of flexible Zn–air batteries with two configurations (i.e., planar stacks and cable fibers) are also introduced. Finally, perspectives on the optimization of arrayed air cathodes for future development to achieve high‐performance flexible Zn–air batteries are shared.     

2D Metal–Organic Frameworks (MOFs) for High‐Performance BatCap Hybrid Devices

Two identical layered metal–organic frameworks (MOFs) (CoFRS and NiFRS) are constructed by using flexible 1,10‐bis(1,2,4‐triazol‐1‐yl)decane as pillars and 1,4‐benzenedicarboxylic acid as rigid linkers. The single‐crystal structure analysis indicates that the as‐synthesized MOFs possess fluctuant 2D networks with large interlayer lattices. Serving as active electrode elements in supercapacitors, both MOFs deliver excellent rate capabilities, high capacities, and longstanding endurances. Moreover, the new intermediates in two electrodes before and after long‐lifespan cycling are also examined, which cannot be identified as metal hydroxides in the peer reports. After assembled into battery‐supercapacitor (BatCap) hybrid devices, the NiFRS//activated carbon (AC) device displays better electrochemical results in terms of gravimetric capacitance and cycling performance than CoFRS//AC devices, and a higher energy‐density value of 28.7 Wh kg^?1 compared to other peer references with MOFs‐based electrodes. Furthermore, the possible factors to support the distinct performances are discussed and analyzed.     

Multilayer Polypyrrole Nanosheets with Self‐Organized Surface Structures for Flexible and Efficient Solar–Thermal Energy Conversion

Converting solar energy into concentrated heat is very appealing for various applications. Polypyrrole (PPy) is known to possess excellent photothermal property with low thermal conductivity, and thus is an ideal candidate for solar–thermal energy conversion. However, solar–thermal materials based on PPy or other conducting polymers still exhibit limited energy conversion efficiency due to the lack of effective light‐trapping schemes. Here, it is demonstrated that multilayer PPy nanosheets with spontaneously formed surface structures such as wrinkles and ridges via sequential polymerization on paper substrates can dramatically enhance broadband and wide‐angle light absorption across the full solar spectrum, leading to an impressive solar–thermal conversion efficiency of 95.33%. The intriguing solar–thermal properties and structural features of multilayer PPy nanosheets can be used for solar heating and photoactuators. Meanwhile, when used for solar steam generation, the measured efficiency could achieve ≈92% under one sun irradiation. The hierarchically multilayer structure is mechanically flexible and robust, holding great potential for practical solar energy utilization. This study provides a simple and straightforward approach toward engineering light‐weight and thermally insulating polymers into efficient solar–thermal materials for emerging solar energy‐related applications.     

Component‐Interaction Reinforced Quasi‐Solid Electrolyte with Multifunctionality for Flexible Li–O2 Battery with Superior Safety under Extreme Conditions

High‐performance flexible lithium–oxygen (Li–O₂) batteries with excellent safety and stability are urgently required due to the rapid development of flexible and wearable devices. Herein, based on an integrated solid‐state design by taking advantage of component‐interaction between poly(vinylidene fluoride‐co‐hexafluoropropylene) and nanofumed silica in polymer matrix, a stable quasi‐solid‐state electrolyte (PS‐QSE) for the Li–O₂ battery is proposed. The as‐assembled Li–O₂ battery containing the PS‐QSE exhibits effectively improved anodic reversibility (over 200 cycles, 850 h) and cycling stability of the battery (89 cycles, nearly 900 h). The improvement is attributed to the stability of the PS‐QSE (including electrochemical, chemical, and mechanical stability), as well as the effective protection of lithium anode from aggressive soluble intermediates generated in cathode. Furthermore, it is demonstrated that the interaction among the components plays a pivotal role in modulating the Li‐ion conducting mechanism in the as‐prepared PS‐QSE. Moreover, the pouch‐type PS‐QSE based Li–O₂ battery also shows wonderful flexibility, tolerating various deformations thanks to its integrated solid‐state design. Furthermore, holes can be punched through the Li–O₂ battery, and it can even be cut into any desired shape, demonstrating exceptional safety. Thus, this type of battery has the potential to meet the demands of tailorability and comformability in flexible and wearable electronics.     

Ionic Liquid Gating Control of Spin Reorientation Transition and Switching of Perpendicular Magnetic Anisotropy

Electric field (E‐field) modulation of perpendicular magnetic anisotropy (PMA) switching, in an energy‐efficient manner, is of great potential to realize magnetoelectric (ME) memories and other ME devices. Voltage control of the spin‐reorientation transition (SRT) that allows the magnetic moment rotating between the out‐of‐plane and the in‐plane direction is thereby crucial. In this work, a remarkable magnetic anisotropy field change up to 1572 Oe is achieved under a small operation voltage of 4 V through ionic liquid (IL) gating control of SRT in Au/[DEME]⁺[TFSI]^?/Pt/(Co/Pt)₂/Ta capacitor heterostructures at room temperature, corresponding to a large ME coefficient of 378 Oe V^?1. As revealed by both ferromagnetic resonance measurements and magnetic domain evolution observation, the magnetization can be switched stably and reversibly between the out‐of‐plane and in‐plane directions via IL gating. The key mechanism, revealed by the first‐principles calculation, is that the IL gating process influences the interfacial spin–orbital coupling as well as net Rashba magnetic field between the Co and Pt layers, resulting in the modulation of the SRT and in‐plane/out‐of‐plane magnetization switching. This work demonstrates a unique IL‐gated PMA with large ME tunability and paves a way toward IL gating spintronic/electronic devices such as voltage tunable PMA memories.     

Co Nanoislands Rooted on Co–N–C Nanosheets as Efficient Oxygen Electrocatalyst for Zn–Air Batteries

Developing non‐precious‐metal bifunctional oxygen reduction and evolution reaction (ORR/OER) catalysts is a major task for promoting the reaction efficiency of Zn–air batteries. Co‐based catalysts have been regarded as promising ORR and OER catalysts owing to the multivalence characteristic of cobalt element. Herein, the synthesis of Co nanoislands rooted on Co–N–C nanosheets supported by carbon felts (Co/Co–N–C) is reported. Co nanosheets rooted on the carbon felt derived from electrodeposition are applied as the self‐template and cobalt source. The synergistic effect of metal Co islands with OER activity and Co–N–C nanosheets with superior ORR performance leads to good bifuctional catalytic performances. Wavelet transform extended X‐ray absorption fine spectroscopy and X‐ray photoelectron spectroscopy certify the formation of Co (mainly Co⁰) and the Co–N–C (mainly Co²⁺ and Co³⁺) structure. As the air‐cathode, the assembled aqueous Zn–air battery exhibits a small charge–discharge voltage gap (0.82 V@10 mA cm^?2) and high power density of 132 mW cm^?2, outperforming the commercial Pt/C catalyst. Additionally, the cable flexible rechargeable Zn–air battery exhibits excellent bendable and durability. Density functional theory calculation is combined with operando X‐ray absorption spectroscopy to further elucidate the active sites of oxygen reactions at the Co/Co–N–C cathode in Zn–air battery.     

An Ultrastable and High‐Performance Flexible Fiber‐Shaped Ni–Zn Battery based on a Ni–NiO Heterostructured Nanosheet Cathode

Currently, the main bottleneck for the widespread application of Ni–Zn batteries is their poor cycling stability as a result of the irreversibility of the Ni‐based cathode and dendrite formation of the Zn anode during the charging–discharging processes. Herein, a highly rechargeable, flexible, fiber‐shaped Ni–Zn battery with impressive electrochemical performance is rationally demonstrated by employing Ni–NiO heterostructured nanosheets as the cathode. Benefiting from the improved conductivity and enhanced electroactivity of the Ni–NiO heterojunction nanosheet cathode, the as‐fabricated fiber‐shaped Ni–NiO//Zn battery displays high capacity and admirable rate capability. More importantly, this Ni–NiO//Zn battery shows unprecedented cyclic durability both in aqueous (96.6% capacity retention after 10 000 cycles) and polymer (almost no capacity attenuation after 10 000 cycles at 22.2 A g^?1) electrolytes. Moreover, a peak energy density of 6.6 µWh cm^?2, together with a remarkable power density of 20.2 mW cm^?2, is achieved by the flexible quasi‐solid‐state fiber‐shaped Ni–NiO//Zn battery, outperforming most reported fiber‐shaped energy‐storage devices. Such a novel concept of a fiber‐shaped Ni–Zn battery with impressive stability will greatly enrich the flexible energy‐storage technologies for future portable/wearable electronic applications.     

CdS@SiO2 Core–Shell Electroluminescent Nanorod Arrays Based on a Metal–Insulator–Semiconductor Structure

Enormous advancement has been achieved in the field of one‐dimensional (1D) semiconductor light‐emitting devices (LEDs), however, LEDs based on 1D CdS nanostructures have been rarely reported. The fabrication of CdS@SiO₂ core–shell nanorod array LEDs based on a Au–SiO₂–CdS metal–insulator–semiconductor (MIS) structure is presented. The MIS LEDs exhibit strong yellow emission with a low threshold voltage of 2.7 V. Electroluminescence with a broad emission ranging from 450 nm to 800 nm and a shoulder peak at 700 nm is observed, which is related to the defects and surface states of the CdS nanorods. The influence of the SiO₂ shell thickness on the electroluminescence intensity is systematically investigated. The devices have a high light‐emitting spatial resolution of 1.5 μm and maintain an excellent emission property even after shelving at room temperature for at least three months. Moreover, the fabrication process is simple and cost effective and the MIS device could be fabricated on a flexible substrate, which holds great potential for application as a flexible light source. This prototype is expected to open up a new route towards the development of large‐scale light‐emitting devices with excellent attributes, such as high resolution, low cost, and good stability.     

Dendrite‐Free Sodium‐Metal Anodes for High‐Energy Sodium‐Metal Batteries

Sodium (Na) metal is one of the most promising electrode materials for next‐generation low‐cost rechargeable batteries. However, the challenges caused by dendrite growth on Na metal anodes restrict practical applications of rechargeable Na metal batteries. Herein, a nitrogen and sulfur co‐doped carbon nanotube (NSCNT) paper is used as the interlayer to control Na nucleation behavior and suppress the Na dendrite growth. The N‐ and S‐containing functional groups on the carbon nanotubes induce the NSCNTs to be highly “sodiophilic,” which can guide the initial Na nucleation and direct Na to distribute uniformly on the NSCNT paper. As a result, the Na‐metal‐based anode (Na/NSCNT anode) exhibits a dendrite‐free morphology during repeated Na plating and striping and excellent cycling stability. As a proof of concept, it is also demonstrated that the electrochemical performance of sodium–oxygen (Na–O₂) batteries using the Na/NSCNT anodes show significantly improved cycling performances compared with Na–O₂ batteries with bare Na metal anodes. This work opens a new avenue for the development of next‐generation high‐energy‐density sodium‐metal batteries.     

Capillarity Composited Recycled Paper/Graphene Scaffold for Lithium–Sulfur Batteries with Enhanced Capacity and Extended Lifespan

An effective strategy to tackle the twin crises of global deforestation and fossil fuel depletion is to recycle biomass materials for energy storage devices. This study reports a unique and innovative solution to capitalize on a currently overlooked resource to produce high‐performance lithium–sulfur (Li–S) batteries from recycled paper. The recycled paper fibers are creatively composited with graphene oxide sheets via a capillary adsorption method. The recycled paper/graphene oxide hybrid is then converted to activated paper carbon/reduced graphene oxide (APC/graphene) scaffold for sulfur infiltration. The assembled Li–APC/graphene/S battery exhibits a superior lifespan of 620 cycles with an excellent capacity retention rate of 60.5%. An APC interlayer is sandwiched between the Li anode and the separator to suppress the degradation of Li anode by preventing the nonhomogeneous growth of mossy Li whiskers, stretching the battery lifespan up to 1000 cycles with a capacitance retention rate of 52.3%. The capillary adsorption method coupled with the porous carbonaceous anode interlayer configuration creates a new opportunity for the development of batteries derived from porous biomass materials.     

Highly Efficient and Bright Inverted Top‐Emitting InP Quantum Dot Light‐Emitting Diodes Introducing a Hole‐Suppressing Interlayer

InP quantum dots (QDs) based light‐emitting diodes (QLEDs) are considered as one of the most promising candidates as a substitute for the environmentally toxic Cd‐based QLEDs for future displays. However, the device architecture of InP QLEDs is almost the same as the Cd‐based QLEDs even though the properties of Cd‐based and InP‐based QDs are quite different in their energy levels and shapes. Thus, it is highly required to develop a proper device structure for InP‐based QLEDs to improve the efficiency and stability. In this work, efficient, bright, and stable InP/ZnSeS QLEDs based on an inverted top emission QLED (ITQLED) structure by newly introducing a “hole‐suppressing interlayer” are demonstrated. The green‐emitting ITQLEDs with the hole‐suppressing interlayer exhibit a maximum current efficiency of 15.1–21.6 cd A^?1 and the maximum luminance of 17 400–38 800 cd m^?2, which outperform the recently reported InP‐based QLEDs. The operational lifetime is also increased when the hole‐suppressing interlayer is adopted. These superb QLED performances originate not only from the enhanced light‐outcoupling by the top emission structure but also from the improved electron–hole balance by introducing a hole‐suppressing interlayer which can control the hole injection into QDs.     

A Water‐/Fireproof Flexible Lithium–Oxygen Battery Achieved by Synergy of Novel Architecture and Multifunctional Separator

To meet the increasing demands for portable and flexible devices in a rapidly developing society, it is urgently required to develop highly safe and flexible electrochemical energy‐storage systems. Flexible lithium–oxygen batteries with high theoretical specific energy density are promising candidates; however, the conventional half‐open structure design prevents it from working properly under water or fire conditions. Herein, as a proof‐of‐concept experiment, a highly safe flexible lithium–oxygen battery achieved by the synergy of a vital multifunctional structure design and a unique composite separator is proposed and fabricated. The structure can effectively prevent the invasion of water from the environment and combustion, which is further significantly consolidated with the help of a polyimide and poly(vinylidene fluoride‐co‐hexafluoropropylene) composite separator, which holds good water resistance, thermal stability, and ionic conductivity. Unexpectedly, the obtained lithium–oxygen battery exhibits superior flexibility, water resistance, thermal resistance, and cycling stability (up to 218 cycles; at a high current of 1 mA and capacity of 4 mA h). This novel water/fireproof, flexible lithium–oxygen battery is a promising candidate to power underwater flexible electronics.     

Multifunctional Interlayer Based on Molybdenum Diphosphide Catalyst and Carbon Nanotube Film for Lithium–Sulfur Batteries

A multifunctional interlayer, composed of molybdenum diphosphide (MoP₂) nanoparticles and a carbon nanotube (CNT) film, is introduced into a lithium–sulfur (Li–S) battery system to suppress polysulfide migration. Molybdenum diphosphide acts as the catalyst and can capture polysulfides and improve the polysulfide conversion activity during the discharge/charge processes. The CNT film acts as a conductive skeleton to support the MoP₂ nanoparticles and to ensure their uniform distribution. The CNT film physically hinders polysulfide migration, acts as a current collector, and provides abundant electron pathways. The Li–S battery containing the multifunctional MoP₂/CNT interlayer exhibits excellent electrochemical performance. It delivers a reversible specific capacity of 905 mA h g^?1 over 100 cycles at 0.2 C, with a capacity decay of 0.152% per cycle. These results suggest the introduction of the multifunctional CNT/MoP₂ interlayer as an effective and practical method for producing high‐performance Li–S batteries.     

Design Multifunctional Catalytic Interface: Toward Regulation of Polysulfide and Li2S Redox Conversion in Li–S Batteries

The polysulfide shuttle effect and sluggish reaction kinetics hamper the practical applications of lithium–sulfur (Li–S) batteries. Incorporating a functional interlayer to trapping and binding polysulfides has been found effective to block polysulfide migration. Furthermore, surface chemistry at soluble polysulfides/electrolyte interface is a crucial step for Li–S battery in which stable cycling depends on adsorption and reutilization of blocked polysulfides in the electrolyte. A multifunctional catalytic interface composed of niobium nitride/N‐doped graphene (NbN/NG) along the soluble polysulfides/electrolyte is designed and constructed to regulate corresponding interface chemical reaction, which can afford long‐range electron transfer surfaces, numerous strong chemisorption, and catalytic sites in a working lithium–sulfur battery. Both experimental and theoretical calculation results suggest that a new catalytic interface enabled by metal‐like NbN with superb electrocatalysis anchored on NG is highly effective in regulating the blocked polysulfide redox reaction and tailoring the Li₂S nucleation–growth–decomposition process. Therefore, the Li–S batteries with multifunctional NbN/NG barrier exhibit excellent rate performance (621.2 mAh g^?1 at 3 C) and high stable cycling life (81.5% capacity retention after 400 cycles). This work provides new insights to promote Li–S batteries via multifunctional catalytic interface engineering.     

Interfacial Synthesis of Conjugated Crystalline 2D Fluorescent Polymer Film Containing Aggregation‐Induced Emission Unit

A fully conjugated 2D fluorescent film containing a tetraphenylethene (TPE) unit is constructed by Glaser–Hay coupling reaction on the surface of copper foil. A large‐area, freestanding fluorescent films with an average thickness 4.5 nm can be obtained through the strategy of solid–liquid interfacial synthesis. The film and the pore structure are characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), atomic force microscopy (AFM), X‐ray photoelectron spectroscopy (XPS). High‐resulution TEM and selected area electron diffraction (SAED) further confirm the dual pores structure with triangular‐ and hexagonal‐shaped pores. The as‐prepared 2D films exhibit excellent solid‐state fluorescence emission arising from the confinement of TPE units.     

Exploration of Advanced Electrode Materials for Approaching High‐Performance Nickel‐Based Superbatteries

The surging interest in high performance, low‐cost, and safe energy storage devices has spurred tremendous research efforts in the development of advanced electrode active materials. Herein, the in situ growth of zinc–iron layered double hydroxide (Zn–Fe LDH) on graphene aerogel (GA) substrates through a facile, one‐pot hydrothermal method is reported. The strong interaction and efficient electronic coupling between LDH and graphene substantially improve interfacial charge transport properties of the resulting nanocomposite and provide more available redox active sites for faradaic reactions. An LDH–GA||Ni(OH)₂ device is also fabricated that results in greatly enhanced specific capacity (187 mAh g^?1 at 0.1 A g^?1), outstanding specific energy (147 Wh kg^?1), excellent specific power (16.7 kW kg^?1), along with 88% capacity retention after >10 000 cycles. This approach is further extended to Ni–MH and Ni–Cd batteries to demonstrate the feasibility of compositing with graphene for boosting the energy storage performance of other well‐known Ni‐based batteries. In contrast to conventional Ni‐based batteries, the nearly flat voltage plateau followed by a sloping potential profile of the integrated supercapacitor–battery enables it to be discharged down to 0 V without being damaged. These findings provide new prospects for the design of high‐performance and affordable superbatteries based on earth‐abundant elements.     

Hollow Co3O4 Nanosphere Embedded in Carbon Arrays for Stable and Flexible Solid‐State Zinc–Air Batteries

Highly active and durable air cathodes to catalyze both the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are urgently required for rechargeable metal–air batteries. In this work, an efficient bifunctional oxygen catalyst comprising hollow Co₃O₄ nanospheres embedded in nitrogen‐doped carbon nanowall arrays on flexible carbon cloth (NC‐Co₃O₄/CC) is reported. The hierarchical structure is facilely derived from a metal–organic framework precursor. A carbon onion coating constrains the Kirkendall effect to promote the conversion of the Co nanoparticles into irregular hollow oxide nanospheres with a fine scale nanograin structure, which enables promising catalytic properties toward both OER and ORR. The integrated NC‐Co₃O₄/CC can be used as an additive‐free air cathode for flexible all‐solid‐state zinc–air batteries, which present high open circuit potential (1.44 V), high capacity (387.2 mAh g^?1, based on the total mass of Zn and catalysts), excellent cycling stability and mechanical flexibility, significantly outperforming Pt‐ and Ir‐based zinc–air batteries.