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 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.

Langmuir-Blodgett assembly of ultra-large graphene oxide films for transparent electrodes

Monolayer ultra-large graphene oxide （UL-GO） sheets with diameter up to about 100 μm were synthesized based on a chemical method. Transparent conductive films were produced using the UL-GO sheets that were deposited layer-by-layer on a substrate by the Langmuir-Blodgett （L-B） assembly technique. The films produced from UL-GO sheets with a close-packed flat structure exhibit exceptionally high electrical conductivity and transparency after thermal reduction. A remarkable sheet resistance of 605 -/sq at 86% transparency is obtained, which outperforms the graphene films grown on a Ni substrate by chemical vapor deposition. The technique used to produce transparent conductive films is facile, inexpensive and tunable for mass production.

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.

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.

Synthesis and purification of long copper nanowires. Application to high performance flexible transparent electrodes with and without PEDOT：PSS

We demonstrate the hydrothermal synthesis of long copper nanowires based on a simple protocol. We show that the purification of the nanowires is very important and can be achieved easily by wet treatment with glacial acetic acid. Fabrication of random networks of purified copper nanowires leads to flexible transparent electrodes with excellent optoelectronic performances （e.g., 55 Ω/sq. at 94% transparency）. The process is carried out at room temperature and no post-treatment is necessary. Hybrid materials with the conductive polymer PEDOT：PSS show similar properties （e.g., 46 Ω/sq, at 93% transparency）, with improved mechanical properties. Both electrodes were integrated in capacitive touch sensors.

Low haze transparent electrodes and highly conducting air dried films with ultra-long silver nanowires synthesized by one-step polyol method

Transparent electrodes made of silver nanowires （AgNWs） exhibit higher flexibility when compared to those made of tin doped indium oxide （ITO） and are expected to be applied in plastic electronics. However, these transparent electrodes composed of AgNWs show high haze because the wires cause strong light scattering in the visible range. Reduction of the wire diameter has been proposed as a way to weaken light scattering, although there have seldom been any studies focusing on the haze because of the difficulty involved in controlling the wire diameter. In this report, we show that the haze can be easily reduced by increasing the length of AgNWs with a large diameter. Ultra-long （u-long） AgNWs with lengths in the range of 20-100 μm and a maximum length of 230 μm have been successfully synthesized by adjusting the reaction temperature and the stirring speed of a one-step polyol process. Compared to typical AgNWs （with diameter and length of 70 nm and 10 μm, respectively） and ITO, a transparent electrode consisting of u-long AgNWs 91 nm in diameter demonstrated a low haze of 3.4%-1.6% and a low sheet resistance of 24-109 Ω/sq. at a transmittance of 94%-97%. Even when fabricated at room temperature without any post-treatment, the electrodes composed of u-long AgNWs achieved a sheet resistance of 19 Ω/sq, at a transmittance of 80%, which is six orders of magnitude lower than that of typical AgNWs.

A Rapid Synthesis of High Aspect Ratio Silver Nanowires for High-Performance Transparent Electrodes

A rapid,simple and cost-effective polyol method has been developed for the synthesis of silver nanowires with high aspect ratio and high purity.The aspect ratios of the silver nanowires as high as ca.1000(average length 40μm and some even as long as 80μm,diameter 50-100 nm)were obtained via optimizing the reaction conditions.Transparent electrodes with excellent optoelectronic performances(optical transmittance of 90%,sheet resistance of 23.2Ω/□and optical transmittance of 87%,sheet resistance of 19.7Ω/□)comparable to commercial ITO were fab-ricated via simple spin coating the resulting silver nanowires onto the glass substrates.The high optoelectronic per-formances and the facile all-solution process of the as-prepared transparent electrodes render them rather promising candidates for use in cost-effective large-area optoelectronic devices.

Fabrication of Silver Nanowire Transparent Electrodes at Room Temperature

Silver nanowires （AgNWs） surrounded by insulating poly（vinylpyrrolidone） have been synthesized by a polyol process and employed as transparent electrodes. The AgNW transparent electrodes can be fabricated by heattreatment at about 200 ℃ which forms connecting junctions between AgNWs. Such a heating process is, however, one of the drawbacks of the fabrication of AgNW electrodes on heat-sensitive substrates. Here it has been demonstrated that the electrical conductivity of AgNW electrodes can be improved by mechanical pressing at 25 MPa for 5 s at room temperature. This simple process results in a low sheet resistance of 8.6 Ω/square and a transparency of 80.0%, equivalent to the properties of the AgNW electrodes heated at 200 ℃. This technique makes it possible to fabricate AgNW transparent electrodes on heat-sensitive substrates. The AgNW electrodes on poly（ethylene terephthalate） films exhibited high stability of their electrical conductivities against the repeated bending test. In addition, the surface roughness of the pressed AgNW electrodes is one-third of that of the heat-treated electrode because the AgNW junctions are mechanically compressed. As a result, an organic solar cell fabricated on the pressed AgNW electrodes exhibited a power conversion as much as those fabricated on indium tin oxide electrodes. These findings enable continuous roll-to-roll processing at room temperature, resulting in relatively simple, inexpensive, and scalable processing that is suitable for forthcoming technologies such as organic solar cells, flexible displays, and touch screens.

Plasma-induced nanowelding of a copper nanowire network and its application in transparent electrodes and stretchable conductors

Copper nanowires （Cu NWs） have attracted increasing attention as building blocks for electronics due to their outstanding electrical properties and low cost. However, organic residues and oxide layers ubiquitously existing on the surface of Cu NWs impede good inter-wire contact. Commonly used methods such as thermal annealing and acid treatment often lead to nanowire damage. Herein, hydrogen plasma treatment at room temperature has been demonstrated to be effective for simultaneous surface cleaning and selective welding of Cu NWs at junctions. Transparent electrodes with excellent optical-electrical performance （19 ff）-sq-1 @ 90% T） and enhanced stability have been fabricated and integrated into organic solar cells. Besides, Cu NW conductors with superior stretchability and cycling stability under stretching speeds of up to 400 mm-min-＇ can also be produced by the nanowelding process, and the feasibility of their application in stretchable LED circuits has been demonstrated.

Fabrication of sintering-free flexible copper nanowire/ polymer composite transparent electrodes with enhanced chemical and mechanical stability

The thermal decomposition synthesis of long copper nanowires （CuNWs） was achieved by controlling the synthesis parameters. A detailed study was performed to determine the effect of the molar ratio of copper chloride to nickel acetylacetonate, temperature, and stirring rate on the final shape of the products. Transparent electrodes （TEs） were fabricated by wet treatment with acetic acid （AA）, without using a sintering process. The low oxidation stability and high surface roughness are the main disadvantages of the CuNW TEs, which limit their applications. In order to overcome these issues, we prepared CuNW/polymer composite TEs by partial embedding of the CuNWs into poly（methyl methacrylate） （PMMA） on poly（ethylene terephthalate） （PET） substrates. The CuNW/PMMA composite TEs exhibit excellent optoelectronic performance （91.3% at 100.7 ff2/sq）, low surface roughness （4.6 nm in height）, and good mechanical and chemical stability as compared with CuNW TEs. On the basis of these properties, we believe that CuNW-based composite TEs could serve as low-cost materials for a wide range of new optoelectronic devices.

Solution-processable graphene mesh transparent electrodes for organic solar cells

Graphene mesh electrodes （GMEs） with good conductivity and transparency have been fabricated by the standard industrial photolithography and 02 plasma etching process using graphene solutions. Organic photovoltaic （OPV） cells using GMEs as the transparent electrodes with a blend of poly-（3-hexylthiophene） phenyl-C61-butyric acid methyl ester （P3HT/PC61BM） as the active layer have been fabricated and exhibit a power conversion efficiency （PCE） of 2.04%, the highest PCE for solution-processed graphene transparent electrode-based solar cells reported to date.

UV-assisted flash light welding process to fabricate silver nanowire/graphene on a PET substrate for transparent electrodes

Graphene oxide and silver nanowires were bar coated onto polyethylene terephthalate （PET） substrates and then welded using an ultraviolet （UV）-assisted flash light irradiation process to achieve both high electrical conductivity and low haze. The irradiation process connected adjacent silver nanowires by welding, while simultaneously reducing the graphene oxide to graphene. This process was performed using a custom W-assisted flash light welding system at room temperature under ambient conditions and was extremely rapid, with processing time of several milliseconds. The effects of varying the weight fractions of the silver nanowires and graphene oxide and of varying the W-assisted flash light welding conditions （light energy and pulse duration） were investigated. The surface morphologies of the welded silver nanowire/graphene films were analyzed using scanning electron microscopy. Optical characterizations, including transmittance and haze measurements, were also conducted using a spectrophotometer. To test their resistance to oxidation, the welded silver nanowire/graphene films were subjected to high temperature in a furnace （100 ℃）, and their sheet resistances were measured every hour. The flash light welding process was found to yield silver nanowire/graphene films with high oxidation resistance, high conductivity （14.35 Ω·sq-1）, high transmittance （93.46%）, and low haze （0.9%）. This material showed uniform temperature distribution when applied as a resistive heating film.

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.

Structural, Optical and Electrical Properties of Ga Doped ZnO/Cu grid/Ga Doped ZnO Transparent Electrodes

Ga doped ZnO （OZO）/Cu grid/GZO transparent conductive electrode （TCE） structures were fabricated at room temperature （RT） by using electron beam evaporation （EBE） for the Cu grids and RF magnetron sputtering for the GZO layers. In this work, we investigated the electrical and optical characteristics of GZO/Cu grid/GZO multilayer electrode for thin film solar cells by using evaporated Cu grid and sputtered GZO thin films to enhance the optical transparency without significantly affecting their conductivity. The optical transmittance and sheet resistance of GZO/Cu grid/GZO multilayer are higher than those of GZO/Cu film/GZO multilayer independent of Cu grid separation distance and increase with increasing Cu grid separation distances. The calculation of both transmittance and sheet resistance of GZO/Cu grid] GZO multilayer was based on Cu filling factor correlated with the geometry of Cu grid. The calculated values for the transmittance and sheet resistance of the GZO/Cu grid/GZO multilayer were similar to the experimentally observed ones. The highest figure of merit ФTc is 5.18× 10^-3Ω^-1 for the GZO/Cu grid] GZO multilayer with Cu grid separation distance of 1 mm was obtained, in this case, the transmittance and resistivity were 82.72% and 2.17 × 10 ^-4Ωcm, respectively. The transmittance and resistivity are accentahle for nractical thin film snlar cell annlicatinn~

Highly stable,stretchable,and transparent electrodes based on dualheaded Ag@Au core-sheath nanomatchsticks for non-enzymatic glucose biosensor

Stretchable and transparent electrodes(STEs)based on silver nanowires(AgNWs)have garnered considerable attention due to their unique optoelectronic features.However,the low oxidation resistance of AgNWs severely limits the reliability and durability of devices based on such STEs.The present work reports a type of core-sheath silver@gold nanowires(Ag@Au NWs)with a morphology resembling dual-headed matchsticks and an average Au sheath thickness of 2.5 nm.By starting with such Ag@Au NWs,STEs with an optical transmittance of 78.7%,a haze of 13.0%,a sheet resistance of 13.5Ω·sq.−1,and a maximum tensile strain of 240%can be formed with the aid of capillary-force-induced welding.The resultant STEs exhibit exceptional oxidation resistance,high-temperature resistance,and chemical/electrochemical stability owing to the conformal and dense Au sheath.Furthermore,non-enzymatic glucose biosensors are fabricated employing the Ag@Au NW STEs.The electrocatalytic oxidation currents are proportional to glucose concentrations with a high sensitivity of 967μA·mM−1·cm−2 and a detection limit of 125μM over a detection range of 0.6 to 16 mM.Additionally,the biosensors demonstrate an appealing robustness and antiinterference characteristics,high repeatability,and great stability that make them adequate for practical use.

Ultra-Highly Cross-Aligned AgNWs Network by a Facile Liquid-Bridge Assisted Couette-Flow Solution Process:Toward Mass-Producing High-Performance Flexible Transparent Electrodes

Cross-aligned silver nanowires(CA-AgNWs),a unique networkwidely used in flexible transparent electrodes(FTEs),have been well developed using various solution processes.However,these approaches suffer from limitations of both the large alignment deviation and solution waste,especially in large-area fabrication,which deteriorates the performance of FTEs.Herein,we developed a facile liquid-bridge assisted Couette-flow solution shearing approach,which enables aligning AgNWs into a highly ordered horizontal array over a large area(120 cm^(2)).Particularly,the alignment deviation,evaluated by the statistic,full width at half-maximum,is rather small with a value of ca.12.6,several times lower than those made by other solution processes.The fibrous liquid-bridge is responsible for transferring liquid steadily onto the substrate,during which process AgNWs are aligned roughly by the solution shearing.It is worth noting that the enhanced shearing force(SF)by Couetteflow allows for further alignment.Consequently,the ultra-highly CA-AgNWs network was prepared,leading to a high-performance FTE with high conductivity(7Ωsq^(-1)),high transparency(93%),long lifetime(over 180 days),good adhesion-stability(200 times tape test),and good flexibility.Moreover,the strategy is applicable for mass-production,benefiting the practical applications of high-performance optoelectronic devices.

Biomimic Vein-Like Transparent Conducting Electrodes with Low Sheet Resistance and Metal Consumption

In this contribution,inspired by the excellent resource management and material transport function of leaf veins,the electrical transport function of metallized leaf veins is mimicked from the material transport function of the vein networks.By electroless copper plating on real leaf vein networks with copper thickness of only several hundred nanometre up to several micrometre,certain leaf veins can be converted to transparent conductive electrodes with an ultralow sheet resistance 100 times lower than that of state-of-the-art indium tin oxide thin films,combined with a broadband optical transmission of above 80%in the UV–VIS–IR range.Additionally,the resource efficiency of the vein-like electrode is characterized by the small amount of material needed to build up the networks and the low copper consumption during metallization.In particular,the high current density transport capability of the electrode of>6000 A cm^−2 was demonstrated.These superior properties of the vein-like structures inspire the design of high-performance transparent conductive electrodes without using critical materials and may significantly reduce the Ag consumption down to<10%of the current level for mass production of solar cells and will contribute greatly to the electrode for high power density concentrator solar cells,high power density Li-ion batteries,and supercapacitors.

Highly conductive and transparent carbon nanotube-based electrodes for ultrathin and stretchable organic solar cells

In this work, we have presented a freestanding and flexible CNT-based film with sheet resistance of 60 ？/ and transmittance of 82% treated by nitric acid and chloroauric acid in sequence. Based on modified CNT film as a transparent electrode, we have demonstrated an ultrathin, flexible organic solar cell（OSC） fabricated on 2.5-μm PET substrate. The efficiency of OSC, combined with a composite film of poly（3-hexylthiophene）（P3HT） and phenyl-C61 butyric acid methyl ester（PCBM） as an active layer and with a thin layer of methanol soluble biuret inserted between the photoactive layer and the cathode, can be up to 2.74% which is approximate to that of the reference solar cell fabricated with ITO-coated glass（2.93%）. Incorporating the as-fabricated ITO-free OSC with pre-stretched elastomer, 50% compressive deformation can apply to the solar cells. The results show that the as-prepared CNT-based hybrid film with outstanding electrical and optical properties could serve as a promising transparent electrode for low cost, flexible and stretchable OSCs, which will broaden the applications of OSC and generate more solar power than it now does.

Understanding of the Relationship between the Properties of Cu(In,Ga)Se_(2) Solar Cells and the Structure of Ag Network Electrodes

The relation between the structure of the silver network electrodes and the properties of Cu(In,Ga)Se_(2)(CIGS)solar cells is systemically investigated.The Ag network electrode is deposited onto an Al:ZnO(AZO)thin film,employing a self-forming cracked template.Precise control over the cracked template's structure is achieved through careful adjustment of temperature and humidity.The Ag network electrodes with different coverage areas and network densities are systemically applied to the CIGS solar cells.It is revealed that predominant fill factor(FF)is influenced by the figure of merit of transparent conducting electrodes,rather than sheet resistance,particularly when the coverage area falls within the range of 1.3–5%.Furthermore,a higher network density corresponds to an enhanced FF when the coverage areas of the Ag networks are similar.When utilizing a thinner AZO film,CIGS solar cells with a surface area of 1.0609 cm^(2)exhibit a notable performance improvement,with efficiency increasing from 10.48%to 11.63%.This enhancement is primarily attributed to the increase in FF from 45%to 65%.These findings underscore the considerable potential for reducing the thickness of the transparent conductive oxide(TCO)in CIGS modules with implications for practical applications in photovoltaic technology.