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.

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.

Recent advances in nanofiber-based flexible transparent electrodes

Flexible and stretchable transparent electrodes are widely used in smart display,energy,wearable devices and other fields.Due to the limitations of flexibility and stretchability of indium tin oxide electrodes,alternative electrodes have appeared,such as metal films,metal nanowires,and conductive meshes.However,few of the above electrodes can simultaneously have excellent flexibility,stretchability,and optoelectronic properties.Nanofiber(NF),a continuous ultra-long one-dimensional conductive material,is considered to be one of the ideal materials for high-performance transparent electrodes with excellent properties due to its unique structure.This paper summarizes the important research progress of NF flexible transparent electrodes(FTEs)in recent years from the aspects of NF electrode materials,preparation technology and application.First,the unique advantages and limitations of various NF materials are systematically discussed.Then,we summarize the preparation technology of various advanced NF FTEs,and point out the future development trend.We also discuss the application of NFs in solar cells,supercapacitors,electric heating equipments,sensors,etc,and analyze its development potential in flexible electronic equipment,as well as problems that need to be solved.Finally,the challenges and future development trends are proposed in the wide application of NF FTEs in the field of flexible optoelectronics.

Self-supported metal(Fe, Co, Ni)-embedded nitrogen-doping carbon nanorod framework as trifunctional electrode for flexible Zn-air batteries and switchable water electrolysis

To meet the practical demand of wearable/portable electronics, developing high-efficiency and durable multifunctional catalyst and in-situ assembling catalysts into electrodes with flexible features are urgently needed but challenging. Herein, we report a simple route to fabricate bendable multifunctional electrodes by in-situ carbonization of metal ion absorbed polyaniline precursor. Alloy nanoparticles encapsulated in graphite layer are uniformly distributed in the N-doping carbon nanorod skeleton. Profiting from the favorable free-standing structure and the cooperative effect of metallic nanoparticles, graphitic layer and N doped-carbon architecture, the trifunctional electrodes exhibit prominent activities and stability toward HER, OER and ORR. Notably, due to the protection of carbon layer, the electrocatalysts show the reversible catalytic HER/OER properties. The overall water splitting device can continuously work for 12 h under frequent exchanges of cathode and anode. Importantly, the bendable metal air batteries fabricated by self-supported electrode not only displays the outstanding battery performance,achieving a decent peak power density(125 mW cm^(-2)) and exhibiting favorable charge-discharge durability of 22 h, but also holds superb flexible stability. Specially, a lightweight self-driven water splitting unit is demonstrated with stable hydrogen production.

Bifunctional flexible electrochromic energy storage devices based on silver nanowire flexible transparent electrodes

Flexible electrochromic energy storage devices(FECESDs)for powering flexible electronics have attracted considerable attention.Silver nanowires(AgNWs)are one kind of the most promising flexible transparent electrodes(FTEs)materials for the emerging flexible devices.Currently,fabricating FECESD based on AgNWs FTEs is still hindered by their intrinsic poor electrochemical stability.To address this issue,a hybrid AgNWs/Co(OH)_(2)/PEDOT:PSS electrode is proposed.The PEDOT:PSS could not only improve the resistance against electrochemical corrosion of AgNWs,but also work as functional layer to realize the color-changing and energy storage properties.Moreover,the Co(OH)_(2)interlayer further improved the color-changing and energy storage performance.Based on the improvement,we assembled the symmetrical FECESDs.Under the same condition,the areal capacitance(0.8 mF cm^(−2))and coloration efficiency(269.80 cm^(2)C−1)of AgNWs/Co(OH)_(2)/PEDOT:PSS FECESDs were obviously higher than AgNWs/PEDOT:PSS FECESDs.Furthermore,the obtained FECESDs exhibited excellent stability against the mechanical deformation.The areal capacitance remained stable during 1000 times cyclic bending with a 25 mm curvature radius.These results demonstrated the broad application potential of the AgNWs/Co(OH)_(2)/PEDOT:PSS FECESD for the emerging portable and multifunctional electronics.

Engineering Geometric Electrodes for Electric Field-Enhanced High-Performance Flexible In-Plane Micro-Supercapacitors

In plane micro-supercapacitors that are miniaturized energy storage components have attracted significant attention due to their high power densities for various ubiquitous and sustainable device systems as well as their facile integration on various flexible/wearable platform.To implement the micro-supercapacitors in various practical applications that can accompany solid state or gel electrolyte and flexible substrates,ions must be readily transported to electrodes for achieving high power densities.Herein,we show large enhancement in electrochemical properties of flexible,inplane micro-supercapacitor using sharp-edged interdigitated electrode design,which was simply fabricated through direct laser scribing method.The sharp-edged electrodes allowed strong electric field to be induced at the corners of the electrode fingers which led to the greater accumulation of ions near the surface of electrode,significantly enhancing the energy storage performance of micro-supercapacitors.The electric field-enhanced in-plane micro-supercapacitor showed the volumetric energy density of 1.52 Wh L^(−1)and the excellent cyclability with capacitive retention of 95.4%after 20000 cycles.We further showed various practicability of our sharp-edged design in micro-supercapacitors by showing circuit applicability,mechanical stability,and air stability.These results present an important pathway for designing electrodes in various energy storage devices.

Emerging CoMn-LDH@MnO2 electrode materials assembled using nanosheets for flexible and foldable energy storage devices

CoMn layered double hydroxides(CoMn-LDH)are promising electrode materials for supercapacitors because of their excellent cyclic stability.However,they possess relatively low capacitances.In this work,hybrid CoMn-LDH@MnO2 products grown on Ni foams were obtained through a facile hydrothermal method.The as-synthesized samples employed as electrodes deliver a specific capacitance of 2325.01 F g^-1 at 1 A g^-1.An assembled asymmetric supercapacitor using these products as positive electrodes shows a maximum energy density of 59.73 W h kg^-1 at 1000.09 W kg^-1.The prominent electrochemical performance of the as-prepared electrodes could be attributes to hierarchical structures.These findings suggest that hybrid structures might be potential alternatives for future flexible energy storage devices.

Recent Progress of Electrode Materials for Flexible Perovskite Solar Cells

Flexible perovskite solar cells(FPSCs) have attracted enormous interest in wearable and portable electronics due to their high power-per-weight and low cost. Flexible and efficient perovskite solar cells require the development of flexible electrodes compatible with the optoelectronic properties of perovskite. In this review, the recent progress of flexible electrodes used in FPSCs is comprehensively reviewed. The major features of flexible transparent electrodes, including transparent conductive oxides, conductive polymer, carbon nanomaterials and nanostructured metallic materials are systematically compared. And the corresponding modification strategies and device performance are summarized. Moreover, flexible opaque electrodes including metal films, opaque carbon materials and metal foils are critically assessed. Finally, the development directions and difficulties of flexible electrodes are given.

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.

Deciphering the lithium storage chemistry in flexible carbon fiber-based self-supportive electrodes

Flexible carbon fiber cloth(CFC)is an important scaffold and/or current collector for active materials in the development of flexible self-supportive electrode materials(SSEMs),especially in lithium-ion batteries.However,during the intercalation of Li ions into the matrix of CFC(below 0.5 V vs.Li/Li+),the incompatibility in the capacity of the CFC,when used directly as an anode material or as a current collector for active materials,leads to difficulty in the estimation of its actual contribution.To address this issue,we prepared Ni_(5)P_(4)nanosheets on CFC(denoted CFC@Ni_(5)P_(4))and investigated the contribution of CFC in the CFC@Ni_(5)P_(4)by comparing to the powder Ni_(5)P_(4)nanosheets traditionally coated on a copper foil(CuF)(denoted P-Ni_(5)P_(4)).At a current density of 0.4 mA cm^(−2),the as-prepared CFC@Ni_(5)P_(4)showed an areal capacity of 7.38 mAh cm^(−2),which is significantly higher than that of the PNi_(5)P_(4)electrode.More importantly,theoretical studies revealed that the CFC has a high Li adsorption energy that contributes to the low Li-ion diffusion energy barrier of the Ni_(5)P_(4)due to the strong interaction between the CFC and Ni_(5)P_(4),leading to the superior Li-ion storage performance of the CFC@Ni_(5)P_(4)over the pristine Ni_(5)P_(4)sample.This present work unveils the underlying mechanism leading to the achievement of high performance in SSEMs.

High‑Performance Flexible Microneedle Array as a Low‑Impedance Surface Biopotential Dry Electrode for Wearable Electrophysiological Recording and Polysomnography

Microneedle array(MNA)electrodes are an effective solution to achieve high-quality surface biopotential recording without the coordination of conductive gel and are thus very suitable for long-term wearable applications.Existing schemes are limited by flexibility,biosafety,and manufacturing costs,which create large barriers for wider applications.Here,we present a novel flexible MNA electrode that can simultaneously achieve flexibility of the substrate to fit a curved body surface,robustness of microneedles to penetrate the skin without fracture,and a simplified process to allow mass production.The compatibility with wearable wireless systems and the short preparation time of the electrodes significantly improves the comfort and convenience of electrophysiological recording.The normalized electrode–skin contact impedance reaches 0.98 kΩcm^(2)at 1 kHz and 1.50 kΩcm^(2)at 10 Hz,a record low value compared to previous reports and approximately 1/250 of the standard electrodes.The morphology,biosafety,and electrical/mechanical properties are fully characterized,and wearable recordings with a high signal-to-noise ratio and low motion artifacts are realized.The first reported clinical study of microneedle electrodes for surface electrophysiological monitoring was conducted in tens of healthy and sleep-disordered subjects with 44 nights of recording(over 8 h per night),providing substantial evidence that the electrodes can be leveraged to substitute for clinical standard electrodes.

Low temperature fabrication of flexible carbon counter electrode on ITO-PEN for dye-sensitized solar cells

A novel low temperature method was used to prepare the mesoporous carbon（MC） counter electrode（CE） on indium-doped tin oxide coated polyethylene naphthalate（ITO-PEN） for flexible dye-sensitized solar cells（DSSCs）.The obtained flexible MC CEs with carbon loading of 280μg cm^（-2） were characterized by SEM,XRD and electrochemical impedance.The light-to-electricity conversion efficiency of the DSSC fabricated with the prepared flexible MC CE was 86%of that of DSSC based on the decomposited Pt CE.

Advanced flexible electrode materials and structural designs for sodium ion batteries

With the spectacular rise of wearable and portable electronics,flexible power supplying systems with robust mechanical flexibility and high energy storage performance under various mechanical deformation conditions are imperative to be needed.Sodium ion batteries(SIBs)with sustainable natural abundance,low cost and superb properties similar to equivalent lithium ion batteries(LIBs),which have shown significant potentials as energy source for flexible electronic devices.In this review,the recent advances in flexible electrode materials based on different types of conductive substrates are addressed and the strategies underlying rational design for flexible structures are highlighted,as well as their applications in flexible SIBs.The remaining key challenges in rational electrodes design are discussed,and perspectives for practical applications of flexible SIBs are proposed as general guidance for future research of high-performance flexible SIBs.

Solution‑Processed Transparent Conducting Electrodes for Flexible Organic Solar Cells with 16.61% Efficiency

Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.

High loading carbon nanotubes deposited onto porous nickel yarns by solution imbibition as flexible wire-shaped supercapacitor electrodes

The deposition of active materials directly onto metal wires is a general strategy to prepare wire-shaped electrodes for flexible and wearable energy storage devices. However, it is still a critical challenge to coat active materials onto the aimed metal wires because of their smooth surface and small specific surface area. In this work, high porous nickel yarns（PNYs） was fabricated using commercial nylon yarns as templates through step-wise electroless plating, electroplating and calcination processes. The PNYs are composed of multiplied fibers with hollow tubular structure of 5–10 μm in diameter, allowing the imbibition of carbon nanotubes（CNTs） solution by a facile capillary action process. The prepared CNTs/PNY electrodes showed a typical electrochemical double layer capacitive performance and the constructed allsolid flexible wire-shaped symmetric supercapacitors provided a specific capacitance of 4.67 F/cm3 with good cycling stability at a current density of 0.6 A/cm3.

Electrothermal analysis of radiofrequency tissue ablation with injectable flexible electrodes considering bio-heat transfer

Flexible electrodes have been widely focused on in recent years due to their special mechanical properties,which can be directly integrated onto human soft tissues to actively take effects on human body or passively monitor human vital signs.These flexible electrodes provide a new routine to realize clinical treatment of accurate thermal ablation in the biological tissues via radiofrequency ablation(RFA).Meanwhile,accurately controlling of thermal field is very significant for the thermal ablation in the clinical therapeutics to prevent the healthy tissue from excessive burning.In this paper,both one-dimensional and two-dimensional axisymmetric analytical models for the electrothermal analysis of radiofrequency ablation considering bio-heat transfer are established,which are verified by finite element analysis(FEA)and in vitro experiments on pig skins.In the model,the electrical field and thermal field are both derived analytically to accurately predict the temperature rise in the biological tissues.Furthermore,parameters,such as the blood flow convection in living tissues and thickness of tissue,have obvious effects on the thermal field in the tissues.They may pave the theoretical foundation and provide guidance of RFA with flexible electrodes in the future.

Recent progress in flexible Zn-ion hybrid supercapacitors: Fundamentals, fabrication designs, and applications

One of the most exciting new developments in energy storage technology is flexible Zn-ion hybrid supercapacitors(f-ZIHSCs),which combine the high energy of Zn-ion batteries with high-power supercapacitors to satisfy the needs of portable flexible electronics.However,the development of f-ZHSCs is still in its infancy,and there are numerous barriers to overcome before they can be widely implemented for practical applications.This review gives an up-to-date description of recent achievements and underlying concepts in energy storage mechanisms of f-ZIHSCs and emphasizes the critical role of cathode,anode,and electrolyte materials systems in speeding the prosperity of f-ZIHSCs.The innovative nanostructured-based cathode materials for f-ZIHSCs include carbon(e.g.,porous carbon,heteroatom-doped carbon,biomass-derived porous carbon,graphene,etc.),metal-oxides,MXenes,and metal/covalentorganic frameworks,and other materials(e.g.,activated carbon,phosphorene,etc.)are mainly focused.Afterward,the latest developments in flexible anode and electrolyte frameworks and impacts of electrolyte compositions on the electrochemical properties of f-ZIHSC are elaborated.Subsequently,the advancements based on fabrication designs,including quasi-solid-state,micro,fiber-shaped,and all climate-changed f-ZIHSCs,are discussed in detail.Lastly,a summary of current challenges and recommendations for the future progress of advanced f-ZIHSC are addressed.This review article is anticipated to further understand the viable strategies and achievable approaches for assembling high-performance f-ZIHSCs and boost the technical revolutions on cathode,anode,and electrolytes for f-ZIHSC devices.

A review on system and materials for aqueous flexible metal-air batteries

The exploration of aqueous flexible metal-air batteries with high energy density and durability has attracted many research efforts with the demand for portable and wearable electronic devices.Aqueous flexible metal-air batteries feature Earth-abundant materials,environmental friendliness,and operational safety.Each part of one metal-air battery can significantly affect the overall performance.This review starts with the fundamental working principles and the basic battery configurations and then highlights on the common issues and the recent advances in designing high-performance metal electrodes,solid-state electrolytes,and air electrodes.Bifunctional oxygen electrocatalysts with high activity and long-term stability for constructing efficient air electrodes in flexible metal-air batteries are summarized including metal-free carbon-based materials and nonprecious Co/Fe-based materials(alloys,metal oxides,metal sulfites,metal phosphates,metal nitrates,single-site metal-nitrogen-carbon materials,and composites).Finally,a perspective is provided on the existing challenges and possible future research directions in optimizing the performance and lifetime of the flexible aqueous solid-state metal-air batteries.

Large-Area Gravure-Printed AgNWs Electrode on Water/Oxygen Barrier Substrate for Long-Term Stable Large-Area Flexible Organic Solar Cells

Large-area AgNWs electrodes(25 cm×10 cm)were fabricated through roll-to-roll printing on the polyvinyl alcohol(PVA)modified water and oxygen barrier substrate.The modification of the barrier film with PVA improved the wettability of silver nanowires on the barrier films and led to the formation of homogenous large-area AgNWs networks.The mechanical flexibility,especially the adhesion force between the silver electrode and the barrier film substrate was dramatically improved through PVA modification.The efficiency of 13.51%for the flexible OSCs with an area of 0.64 cm2 was achieved based on the PET/barrier film/PVA/AgNWs electrode.The long-term stability showed the flexible OSCs based on the PET/barrier film/PVA/AgNWs electrode have a significantly improved stability relative to the device on PET/AgNWs electrode,and comparable air stability as the rigid device with glass/ITO device.The unencapsulated devices maintained nearly 50%of the original efficiency after storage for 600 h in air.After a simple top encapsulation,the flexible devices remained at 60%of the initial efficiency after 2000 h in the air.Therefore,the flexible AgNWs electrode based on the barrier film would have the potential to improve the air storage stability of organic flexible solar cells.

Synthesis of nanostructured zinc oxide and its composite with carbon dots for DSSCs applications using flexible electrode

ZnO nanowires(ZnO NWs),ZnO nanoparticles(ZnO NPs)and carbon dots(C-dots)were synthesized by hydrothermal,sol-gel and hydrothermal methods respectively.They were also characterized and applied for dye sensitized solar cells(DSSCs).The effects of C-dots on ZnO NWs and ZnO NPs have been evaluated.The C-dots were used at a mole ratio of citric acid(CA)to ethylene diamine(EDA)of 1:1.5.These C-dots were found to enhance the performance of the flexible electrode DSSCs.After the addition of C-dots,the power conversion efficiency(PCE)of ZnO NPs was boosted to be two times higher than that of ZnO NPs DSSCs without C-dots.Similarly,the ultraviolet(UV)-band revealed a blue shift,resulting in a lower band gap and a reduced charge transfer resistance,which can enhance the PCE of DSSCs.The loaded quantity on the flexible electrode substrate made of polyethylene terephthalate(PET)was optimized(50 mg).For DSSCs,the PET flexible electrode conductive polymer has produced positive outcomes.For ZnO NWs and ZnO NWs@C-dots,the PCE values were 1.45%and 4.25%;while for ZnO NPs and ZnO NPs@C-dots,they were 2.34%and 5.81%,respectively.This work achieved remarkable and competitive performance when compared to solid(indium tin oxides/glass)-based substrate.