High‑Entropy Electrode Materials:Synthesis,Properties and Outlook

High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has continuously evolved.In the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode materials.Recently,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches.However,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy materials.It should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy materials.In this review,the definition and development of high-entropy materials are briefly reviewed.Subsequently,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods.Finally,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.

Advances in Graphene‑Based Electrode for Triboelectric Nanogenerator

With the continuous development of wearable electronics,wireless sensor networks and other micro-electronic devices,there is an increasingly urgent need for miniature,flexible and efficient nanopower generation technology.Triboelectric nanogenerator(TENG)technology can convert small mechanical energy into electricity,which is expected to address this problem.As the core component of TENG,the choice of electrode materials significantly affects its performance.Traditional metal electrode materials often suffer from problems such as durability,which limits the further application of TENG.Graphene,as a novel electrode material,shows excellent prospects for application in TENG owing to its unique structure and excellent electrical properties.This review systematically summarizes the recent research progress and application prospects of TENGs based on graphene electrodes.Various precision processing methods of graphene electrodes are introduced,and the applications of graphene electrode-based TENGs in various scenarios as well as the enhancement of graphene electrodes for TENG performance are discussed.In addition,the future development of graphene electrode-based TENGs is also prospectively discussed,aiming to promote the continuous advancement of graphene electrode-based TENGs.

Electrode/Electrolyte Optimization‑Induced Double‑Layered Architecture for High‑Performance Aqueous Zinc‑(Dual)Halogen Batteries

Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources,intrinsic safety,and high theoretical capacity.Nevertheless,the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical implementation.Herein,a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid(ZEA)artificial film and ZnF2-rich solid electrolyte interphase(SEI)layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.The ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer,therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal anode.Such double-layered architecture not only modulates Zn2+flux and suppresses the zinc dendrite growth,but also blocks the direct contact between the metal anode and electrolyte,thus mitigating the corrosion from the active species.When employing optimized metal anodes and electrolytes,the as-developed zinc-(dual)halogen batteries present high areal capacity and satisfactory cycling stability.This work provides a new avenue for developing aqueous zinc-(dual)halogen batteries.

Well-aligned Ni Pt alloy counter electrodes for high-efficiency dye-sensitized solar cell applications

Development of cost-effective and robust counter electrodes(CEs) is a persistent objective for highefficiency dye-sensitized solar cells(DSSCs). To achieve this goal, we present here the hydrothermal synthesis of well-aligned Ni Pt alloy CEs, which is templated by ZnO nanowires and nanosheets. The preliminary results demonstrate that Ni Pt alloy electrodes are featured by increased charge-transfer processes and electrocatalytic activity in comparison with expensive Pt CE, yielding power conversion efficiencies of 8.29% and 7.41% in corresponding DSSCs with Ni Pt nanowire and nanosheet alloy CEs, respectively. Additionally, the Ni Pt alloy CEs also display extraordinary dissolution-resistant ability when suffering longterm utilization in liquid-junction DSSCs.

Cerium and ruthenium co-doped La_(0.7)Sr_(0.3)FeO_(3-δ) as a high-efficiency electrode for symmetrical solid oxide fuel cell

Symmetrical solid oxide fuel cells(SSOFCs)could be alternative energy conversion devices due to their simple fabrication process and low cost.Herein,perovskite La_(0.6)Ce_(0.1)Sr_(0.3)Fe_(0.95)Ru_(0.05O3-δ)(LCSFR)was synthesized and evaluated as a high-performance electrode for SSOFCs based on the electrolyte of La_(0.9)Sr_(0.1)Ga_(0.8)Mg_(0.2)O_(3-δ)(LSGM).LCSFR retains their stable perovskite crystal structure in both reducing and oxidizing atmospheres,though a minor amount of LaSrFeO4 phase is present under reducing conditions.Morphology investigation shows that homogeneously dispersed Ru metallic nanoparticles are exsolved on the surface of LCSFR after being reduced.The polarization resistance(Rp)of LCSFR-CGO(Ce_(0.9)Gd_(0.1O2-δ))is about 0.11Ω·cm^(2)at 800℃in air,while the value of Rp for LCSFR-CGO in wet H_(2)(3%H_(2)O)increases up to 0.32Ω·cm^(2).The symmetrical LCSFR-CGOILSGMILCSFR-CGO cell demonstrates a performance with an open circuit potential(OCV)of 1.07 V and a maximum peak power density of 904 mW/cm^(2)at 800℃using wet H2 as the fuel.This high performance indicates that LCSFR is a candidate electrode for SSOFCs.

High-efficiency extraction synthesis for high-purity copper nanowires and their applications in flexible transparent electrodes

Copper nanowires(Cu NWs)are considered an excellent alternative to indium tin oxide(ITO)in flexible transparency electrodes(FTEs).However,the mixed particles and surface oxidation of Cu NWs degrade the transmittance and conductivity of the electrodes.Therefore,highly purified Cu NWs without oxidation are vital for high-performance FTEs.Herein,a facile and effective purification process is introduced to purify Cu NWs in a water and n-hexane system,which takes advantage of the differences in hydrophilicity between Cu NWs and Cu NPs caused by their different adsorption affinities to octadecylamine(ODA).At the same sheet resistance,the transmittance of the purified Cu NW-based FTEs improved approximately 2%compared to that of non-purified Cu NW-based FTEs.Immersion of the electrode in glacial acetic acid removed the surface organics and oxides.After only 40 s of treatment,the sheet resistance dramatically decreased from 10^5 Ohm/sq to 31 Ohm/sq with a transmittance of 85%.In addition,the Cu NW-based FTE conductors showed excellent flexibility(remaining stable after 1000 bending cycles).The Cu NW-based FTEs were further applied to fabricate a flexible transparent heater.At a voltage of 10 V,the temperature of the heater reached 73℃,demonstrating the potential applications of this material in various fields.

High-Efficiency Bottom-Emitting Organic Light-Emitting Diodes with Double Aluminum as Electrodes

Bottom-emitting organic light-emitting diodes （BOLEDs）, using AI/MoO3 as the semitransparent anode and LiF/Al as the reflective cathode and Alqa as the emitter, are fabricated. At the same time, the performance improvement of the BOLEDs having a capping layer inserted between the semitransparent anode and the glass substrate is studied. The optimized microcavity BOLED shows a current efficiency （5.49cd/A） enhancement of 10% compared with a conventional BOLED based on ITO （5.0cd/A）. Slight color variation is observed in 120° forward viewing angle with 5Onto BCP as the capping layer. Strong dependence of efficiency on A1 anode thickness and the thickness and refractor index of the capping layer is explained. The results indicate that the BOLEDs with the double-aluminum electrode have potential practical applications.

High-Efficiency(Over 10%) Parallel Tandem Dye-Sensitized Solar Cells Based on Tri-Carbon Electrodes

Ensuring high power conversion efficiency,partially or completely replacing Pt electrodes with inexpensive materials is one of the important development directions of dye-sensitized solar cells(DSSCs).In this work,we have developed a threecomponent(MWCNTs,carbon black and graphite) carbon(tri-carbon) electrode material for DSSC devices combined with the advantages of high electron transfer kinetics of MWCNTs,plentiful catalytic sites in crystal edges of carbon black and superior electrical conductivity and catalytic activity of graphite.Using a tri-carbon electrode,a Pt electrode,and two N719-sensitized photoanodes,a parallel tandem dye-sensitized solar cells are assembled obtaining a high PCE of 10.26%(V_(OC)=0.70 V,J_(SC)=19.99 mA/cm~2,FF=73.33%).It opens up a new avenue for the development of low-cost and highperformance DSSCs.

Broadband high-efficiency dielectric metalenses based on quasi-continuous nanostrips

Benefiting from the abrupt phase changes within subwavelength thicknesses,metasurfaces have been widely applied for lightweight and compact optical systems.Simultaneous broadband and high-efficiency characteristics are highly attractive for the practical implementation of metasurfaces.However,current metasurface devices mostly adopt discrete micro/nano structures,which rarely realize both merits simultaneously.In this paper,dielectric metasurfaces composed of quasi-continuous nanostrips are proposed to overcome this limitation.Via quasi-continuous nanostrips metasurface,a normal focusing metalens and a superoscillatory lens overcoming the diffraction limit are designed and experimentally demonstrated.The quasi-continuous metadevices can operate in a broadband wavelength ranging from 450 nm to 1000nm and keep a high power efficiency.The average efficiency of the fabricated metalens reaches 54.24%,showing a significant improvement compared to the previously reported metalenses with the same thickness.The proposed methodology can be easily extended to design other metadevices with the advantages of broadband and high-efficiency in practical optical systems.

Implantable probe with integrated reference electrode for in situ neural signal and calcium ion monitoring

Monitoring the electrophysiology activity of neurons and blood calcium signals can enable a better understanding of disease-related neural system circuits.However,currently,in situ calcium ion monitoring tools are scarce and exhibit low integration and limited sensitivity.In this letter,we propose an implantable probe with an integrated in situ Ag/AgCl reference electrode(ISA/ARE)that can monitor action potential(AP)and Ca^(2+) concentrations.

A drug-loaded flexible substrate improves the performance of conformal cortical electrodes

Cortical electrodes are a powerful tool for the stimulation and/or recording of electrical activity in the nervous system.However,the inevitable wound caused by surgical implantation of electrodes presents bacterial infection and inflammatory reaction risks associated with foreign body exposure.Moreover,inflammation of the wound area can dramatically worsen in response to bacterial infection.These consequences can not only lead to the failure of cortical electrode implantation but also threaten the lives of patients.Herein,we prepared a hydrogel made of bacterial cellulose(BC),a flexible substrate for cortical electrodes,and further loaded antibiotic tetracycline(TC)and the anti-inflammatory drug dexamethasone(DEX)onto it.The encapsulated drugs can be released from the BC hydrogel and effectively inhibit the growth of Gram-negative and Gram-positive bacteria.Next,therapeutic cortical electrodes were developed by integrating the drug-loaded BC hydrogel and nine-channel serpentine arrays;these were used to record electrocorticography(ECoG)signals in a rat model.Due to the controlled release of TC and DEX from the BC hydrogel substrate,therapeutic cortical electrodes can alleviate or prevent symptoms associated with the bacterial infection and inflammation of brain tissue.This approach facilitates the development of drug delivery electrodes for resolving complications caused by implantable electrodes.

Ionic Liquid-Enhanced Assembly of Nanomaterials for Highly Stable Flexible Transparent Electrodes

The controlled assembly of nanomaterials has demon-strated significant potential in advancing technological devices.However,achieving highly efficient and low-loss assembly technique for nanomate-rials,enabling the creation of hierarchical structures with distinctive func-tionalities,remains a formidable challenge.Here,we present a method for nanomaterial assembly enhanced by ionic liquids,which enables the fabrication of highly stable,flexible,and transparent electrodes featuring an organized layered structure.The utilization of hydrophobic and non-volatile ionic liquids facilitates the production of stable interfaces with water,effectively preventing the sedimentation of 1D/2D nanomaterials assembled at the interface.Furthermore,the interfacially assembled nanomaterial monolayer exhibits an alternate self-climbing behavior,enabling layer-by-layer transfer and the formation of a well-ordered MXene-wrapped silver nanowire network film.The resulting composite film not only demonstrates exceptional photoelectric performance with a sheet resistance of 9.4Ωsq^(-1) and 93%transmittance,but also showcases remarkable environmental stability and mechanical flexibility.Particularly noteworthy is its application in transparent electromagnetic interference shielding materials and triboelectric nanogenerator devices.This research introduces an innovative approach to manufacture and tailor functional devices based on ordered nanomaterials.

Flexible,high-density,laminated ECoG electrode array for high spatiotemporal resolution foci diagnostic localization of refractory epilepsy

High spatiotemporal resolution brain electrical signals are critical for basic neuroscience research and high-precision focus diagnostic localization,as the spatial scale of some pathologic signals is at the submillimeter or micrometer level.This entails connecting hundreds or thousands of electrode wires on a limited surface.This study reported a class of flexible,ultrathin,highdensity electrocorticogram(ECoG)electrode arrays.The challenge of a large number of wiring arrangements was overcome by a laminated structure design and processing technology improvement.The flexible,ultrathin,high-density ECoG electrode array was conformably attached to the cortex for reliable,high spatial resolution electrophysiologic recordings.The minimum spacing between electrodes was 15μm,comparable to the diameter of a single neuron.Eight hundred electrodes were prepared with an electrode density of 4444 mm^(-2).In focal epilepsy surgery,the flexible,high-density,laminated ECoG electrode array with 36 electrodes was applied to collect epileptic spike waves inrabbits,improving the positioning accuracy of epilepsy lesions from the centimeter to the submillimeter level.The flexible,high-density,laminated ECoG electrode array has potential clinical applications in intractable epilepsy and other neurologic diseases requiring high-precision electroencephalogram acquisition.

Rational Design of Ruddlesden-Popper Perovskite Ferrites as Air Electrode for Highly Active and Durable Reversible Protonic Ceramic Cells

Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7−δ)(SF)exhibits superior proton uptake and rapid ionic conduction,boosting activity.However,excessive proton uptake during RePCC operation degrades SF’s crystal structure,impacting durability.This study introduces a novel A/B-sites co-substitution strategy for modifying air electrodes,incorporating Sr-deficiency and Nb-substitution to create Sr_(2.8)Fe_(1.8)Nb_(0.2)O_(7−δ)(D-SFN).Nb stabilizes SF’s crystal,curbing excessive phase formation,and Sr-deficiency boosts oxygen vacancy concentration,optimizing oxygen transport.The D-SFN electrode demonstrates outstanding activity and durability,achieving a peak power density of 596 mW cm^(−2)in fuel cell mode and a current density of−1.19 A cm^(−2)in electrolysis mode at 1.3 V,650℃,with excellent cycling durability.This approach holds the potential for advancing robust and efficient air electrodes in RePCCs for renewable energy storage.

Unveiling Organic Electrode Materials in Aqueous Zinc-Ion Batteries:From Structural Design to Electrochemical Performance

Aqueous zinc-ion batteries(AZIBs)are one of the most compelling alternatives of lithium-ion batteries due to their inherent safety and economics viability.In response to the growing demand for green and sustainable energy storage solutions,organic electrodes with the scalability from inexpensive starting materials and potential for biodegradation after use have become a prominent choice for AZIBs.Despite gratifying progresses of organic molecules with electrochemical performance in AZIBs,the research is still in infancy and hampered by certain issues due to the underlying complex electrochemistry.Strategies for designing organic electrode materials for AZIBs with high specific capacity and long cycling life are discussed in detail in this review.Specifically,we put emphasis on the unique electrochemistry of different redox-active structures to provide in-depth understanding of their working mechanisms.In addition,we highlight the importance of molecular size/dimension regarding their profound impact on electrochemical performances.Finally,challenges and perspectives are discussed from the developing point of view for future AZIBs.We hope to provide a valuable evaluation on organic electrode materials for AZIBs in our context and give inspiration for the rational design of high-performance AZIBs.

Recent progress of self-supported air electrodes for flexible Zn-air batteries

Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.

A high Li-ion diffusion kinetics in multidimensional and compact-structured electrodes via vacuum filtration casting

Manufacturing process,diffusion co-efficient and areal capacity are the three main criteria for regulating thick electrodes for lithium-ion batteries(LIBs).However,simultaneously regulating these criteria for LIBs is desirable but remains a significant challenge.In this work,niobium pentoxide(Nb_(2)O_(5))anode and lithium iron phosphate(LiFePO_(4))cathode materials were chosen as the model materials and demonstrate that these three parameters can be simultaneously modulated by incorporation of micro-carbon fibers(MCF)and carbon nanotubes(CNT)with both Nb_(2)O_(5) and LFP via vacuum filtration approach.Both as-prepared MNC-20 anode and MLC-20 cathode achieves high reversible areal capacity of≈5.4 m A h cm^(-2)@0.1 C and outstanding Li-ion diffusion coefficients of≈10~(-8)cm~2 s~(-1)in the half-cell configuration.The assembled MNC-20‖MLC-20 full cell LIB delivers maximum energy and power densities of244.04 W h kg^(-1)and 108.86 W kg^(-1),respectively.The excellent electrochemical properties of the asprepared thick electrodes can be attributed to the highly conductive,mechanical compactness and multidimensional mutual effects of the MCF,CNT and active materials that facilitates rapid Li-ion diffusion kinetics.Furthermore,electrochemical impedance spectroscopy(EIS),symmetric cells analysis,and insitu Raman techniques clearly validates the enhanced Li-ion diffusion kinetics in the present architecture.

Perovskite solar cells with high-efficiency exceeding 25%:A review

Metal halide perovskite solar cells(PSCs)are one of the most promising photovoltaic devices.Over time,many strategies have been adopted to improve PSC efficiency,and the certified efficiency has reached 26.1%.However,only a few research groups have fabricated PSCs with an efficiency of>25%,indicating that achieving this efficiency remains uncommon.To develop the PSC industry,outstanding talent must be reserved with the latest technologies.Herein,we summarize the recent developments in high-efficiency PSCs(>25%)and highlight their effective strategies in crystal regulation,interface passivation,and component layer structural design.Finally,we propose perspectives based on current research to further enhance the efficiency and promote the commercialization process of PSCs.

The use of carbon-based particle electrodes in three-dimensional electrode reactors for wastewater treatment

The use of three-dimensional(3D)electrodes in water treatment is competitive because of their high catalytic efficiency,low energy consumption and promising development.The use of particle electrodes is a key research focus in this technology.They are usually in the form of particles that fill the space between the cathode and anode,and the selection of materials used is important.Carbon-based materials are widely used because of their large specific surface area,good adsorption performance,high chemical stability and low cost.The principles of 3D electrode technology are introduced and recent research on its use for degrading organic pollutants using carbon-based particle electrodes is summarized.The classification of particle electrodes is introduced and the challenges for the future development of carbon-based particle electrodes in wastewater treatment are discussed.

Correction: Surface Patterning of Metal ZincElectrode with an In-Region Zincophilic Interfacefor High-Rate and Long-Cycle-Life Zinc MetalAnode

Correction to:Nano-Micro Letters(2024)16:112 https://doi.org/10.1007/s40820-024-01327-2 In the supplementary information the following corrections have been carried out:1.Institute of Energy and Climate Research,Materials Synthesis and Processing,Forschungszentrum Jülich GmbH,52425 Jülich,Germany.Corrected:Institute of Energy and Climate Research:Materials Synthesis and Processing(IEK-1),Forschungszentrum Jülich GmbH,52425 Jülich,Germany.