Well‐Ordered and High Density Coordination‐Type Bonding to Strengthen Contact of Silver Nanowires on Highly Stretchable Polydimethylsiloxane

Recently, Ag nanowires (AgNWs) has had a great interest as a conducting material for flexible and transparent devices, but it still shows several problems such as the ultimate detachment of AgNWs from substrate and a high contact resistance on AgNW junctions. Therefore, the novel concept to enhance permanent and closed attachment of AgNWs by silane modification to polydimethylsilaoxane (PDMS) substrate well known as high stretchable film with extremly low adhesive is suggested. According to this experiment, higher sigma (σ)‐donating ability and hydrophilicity indicate better electrical and mechanical properties in real device. Especially, densely amine self‐assembled PDMS surface exhibits the strongest contact force to the AgNWs, especially for junction side, and the longest maintenance of hydrophilicity by coordination‐type bonding. In addition, AgNWs adhere permanently to stretchable substrates while simultaneously maintaining high transparency (87%) and high conductivity (27 Ω sq^–1). Consequently, the resulting AgNW film shows excellent mechanical durability which includes enhanced performance of both flexibility and stretchability.     

Ultrastretchable Fibers with Metallic Conductivity Using a Liquid Metal Alloy Core

The fabrication and characterization of fibers that are ultrastretchable and have metallic electrical conductivity are described. The fibers consist of a liquid metal alloy, eutectic gallium indium (EGaIn), injected into the core of stretchable hollow fibers composed of a triblock copolymer, poly[styrene‐b‐(ethylene‐co‐butylene)‐b‐styrene] (SEBS) resin. The hollow fibers are easy to mass‐produce with controlled size using commercially available melt processing methods. The fibers are similar to conventional metallic wires, but can be stretched orders of magnitude further while retaining electrical conductivity. Mechanical measurements with and without the liquid metal inside the fibers show the liquid core has a negligible impact on the mechanical properties of the fibers, which is in contrast to most conductive composite fibers. The fibers also maintain the same tactile properties with and without the metal. Electrical measurements show that the fibers increase resistance as the fiber elongates and the cross sectional area narrows. Fibers with larger diameters change from a triangular to a more circular cross‐section during stretching, which has the appeal of lowering the resistance below that predicted by theory. To demonstrate their utility, the ultrastretchable fibers are used as stretchable wires for earphones and for a battery charger and perform as well as their conventional parts.     

All-solution-processed foldable transparent electrodes of Ag nanowire mesh and metal matrix films for flexible electronics

In this study, we developed foldable transparent electrodes composed of Ag nanowire (AgNW) networks welded by Ag nanoparticles (AgNPs) reduced from commercial Ag ink. All the processes used were solution-based. Using the Meyer rod method, uniform AgNW networks were roll-to-roll coated on large-area polymer substrates, and the spin-coated AgNPs firmly welded the AgNWs together at junctions and to substrates. The hybrid films consisting of AgNWs and the Ag film matrix exhibited higher electrical conductivity (5.0–7.3 × 10⁵ S/m) than and equivalent transparency (90–95%) to the AgNW networks. Furthermore, the hybrid films showed significantly better bending stability than AgNW networks. During cyclic bending tests to 10,000 cycles at 5 mm bending radius and even when almost folded with r_b of 1 mm, the resistivity changes were negligible because AgNWs were tightly held and adhered to the substrate by Ag films covering wires, thereby hindering fracturing of AgNWs under tension. Because the films were fabricated at a low temperature, there was no oxidation on the surfaces of the films. Hence, flexible organic light-emitting diodes (f-OLEDs) were successfully fabricated on polyethylene terephthalates (PET) coated with the hybrid films. The f-OLED in the bent state was comparable to that in the flat state, validating the potential applications of these transparent hybrid films as electrodes in various flexible electronics.     

Aligned Silver Nanowires Enabled Highly Stretchable and Transparent Electrodes with Unusual Conductive Property

Transparent conductors for the next generation of soft electronic devices need to be highly stretchable, conductive, and transparent, while an inevitable challenge lies in enhancing them simultaneously. Cost‐effective silver nanowires (AgNWs) are widely used but the conventional random network yields a high junction resistance as well as degraded conductivity in the stretched state. Here, a novel, facile, and versatile agitation‐assisted assembly approach is reported to control the orientation direction and density of AgNWs and to layer‐by‐layer deposit the AgNWs monolayer or multilayers onto the prestrained soft substrate. This electrode demonstrates an unprecedented low sheet resistance of 2.8 Ω sq^?1 as well as high transparency of 85% and high stretchability of 40%. It is interesting to note that contrary to most other reports, such a device shows higher conductivity in the stretched state compared to the released state.     

All‐Solution‐Processed Indium‐Free Transparent Composite Electrodes based on Ag Nanowire and Metal Oxide for Thin‐Film Solar Cells

Fully solution‐processed Al‐doped ZnO/silver nanowire (AgNW)/Al‐doped ZnO/ZnO multi‐stacked composite electrodes are introduced as a transparent, conductive window layer for thin‐film solar cells. Unlike conventional sol–gel synthetic pathways, a newly developed combustion reaction‐based sol–gel chemical approach allows dense and uniform composite electrodes at temperatures as low as 200 °C. The resulting composite layer exhibits high transmittance (93.4% at 550 nm) and low sheet resistance (11.3 Ω sq^‐1), which are far superior to those of other solution‐processed transparent electrodes and are comparable to their sputtered counterparts. Conductive atomic force microscopy reveals that the multi‐stacked metal‐oxide layers embedded with the AgNWs enhance the photocarrier collection efficiency by broadening the lateral conduction range. This as‐developed composite electrode is successfully applied in Cu(In_1‐x,Ga_x)S₂ (CIGS) thin‐film solar cells and exhibits a power conversion efficiency of 11.03%. The fully solution‐processed indium‐free composite films demonstrate not only good performance as transparent electrodes but also the potential for applications in various optoelectronic and photovoltaic devices as a cost‐effective and sustainable alternative electrode.     

Inverted Layer‐By‐Layer Fabrication of an Ultraflexible and Transparent Ag Nanowire/Conductive Polymer Composite Electrode for Use in High‐Performance Organic Solar Cells

A highly flexible and transparent conductive electrode based on consecutively stacked layers of conductive polymer (CP) and silver nanowires (AgNWs) fully embedded in a colorless polyimide (cPI) is achieved by utilizing an inverted layer‐by‐layer processing method. This CP‐AgNW composite electrode exhibits a high transparency of >92% at wavelengths of 450–700 nm and a low resistivity of 7.7 Ω ?^?1, while its ultrasmooth surface provides a large contact area for conductive pathways. Furthermore, it demonstrates an unprecedentedly high flexibility and good mechanical durability during both outward and inward bending to a radius of 40 μm. Subsequent application of this composite electrode in organic solar cells achieves power conversion efficiencies as high as 7.42%, which represents a significant improvement over simply embedding AgNWs in cPI. This is attributed to a reduction in bimolecular recombination and an increased charge collection efficiency, resulting in performance comparable to that of indium tin oxide‐based devices. More importantly, the high mechanical stability means that only a very slight reduction in efficiency is observed with bending (<5%) to a radius of 40 μm. This newly developed composite electrode is therefore expected to be directly applicable to a wide range of high‐performance, low‐cost flexible electronic devices.     

Mechanically Robust Silver Nanowires Network for Triboelectric Nanogenerators

The authors develop a mechanically robust silver nanowires (AgNWs) electrode platform for use in flexible and stretchable triboelectric nanogenerators (TENGs). The embedding of an AgNWs network into a photocurable or thermocurable polymeric matrix dramatically enhances the mechanical robustness of the flexible and stretchable TENG electrodes while maintaining a highly efficient triboelectric performance. The AgNWs/polymeric matrix electrode is fabricated in four steps: (i) the AgNWs networks are formed on a hydrophobic glass substrate; (ii) a laminating photocurable or thermocurable prepolymer film is applied to the developed AgNWs network; (iii) the polymeric matrix is crosslinked by UV exposure or thermal treatment; and (iv) the AgNWs‐embedded polymeric matrix is delaminated from the glass substrate. The AgNWs‐embedded polymeric matrix electrodes with four different sheet resistances, controlled by varying the AgNWs network deposition density, are deployed in TENG devices. The authors find that the potential difference between the two contact surfaces of the AgNWs network‐embedded polymer matrix electrodes and the nylon (or perfluoroalkoxy alkane) governs the output triboelectric performances of the devices, rather than the sheet resistance. Both Kelvin probe force microscopy and numerical simulations strongly support these observations.     

Ice-Templated,Large-Area Silver Nanowire Pattern for Flexible Transparent Electrode

Flexible transparent electrodes are critically important for the emerging flexible and stretchable electronic and optoelectronic devices. To this end, transparent polymer films coated with silver nanowires (AgNWs) have been intensively studied in the past decade. However, it remains a grand challenge to achieve both high conductivity and transmittance in large-area films, mainly due to the poor alignment of AgNWs and their high junction resistance. Here, the successful attempt to realize large-area AgNW patterns on various substrates by a 2D ice-templating approach is reported. With a relatively low dosage of AgNWs (4 µg·cm⁻²), the resulted flexible electrode simultaneously achieves high optical transmittance (≈91%) and low sheet resistance (20 Ω·sq⁻¹). In addition, the electrode exhibits excellent durability during cyclic bending (≈10 000 times) and stretching (50% strain). The potential applications of the flexible transparent electrode in both touch screen and electronic skin sensor, which can monitor the sliding pressure and direction in real-time, are demonstrated. More importantly, it is believed that the study represents a facile and low-cost approach to assemble various nanomaterials into large-area functional patterns for advanced flexible devices.     

Breathable and Flexible Polymer Membranes with Mechanoresponsive Electric Resistance

Flexible low‐resistance membranes play an important role in soft electronics as sensors for robotics, body movement monitoring, nanogenerators to collect kinetic energy from body movements, and flexible batteries. Despite great efforts, low‐resistance, mechanically stable large‐dimensional membranes that tolerate very high deformability without sacrificing resistance produce low joule heating and allow passage of gases for human comfort are still being sought. Here, one of the solutions is provided by sandwiching a network of silver nanowires (AgNWs) between two highly porous electrospun thermoplastic polyurethane (TPU) membranes. The membranes are mechanically robust (both for bending and stretching) with a strong interface and large strain before breakage (more than 700%). The sheet resistance is as low as <0.1 (±0.01) Ω sq^?1, and changed to only 1.6 (±0.43) Ω sq^?1 upon stretching to 100% strain. The combination of polymer elasticity and the AgNW network structure provides a reversible change in resistance beyond 100% strain. A detailed thermographic analysis is employed to in situ image and characterize the AgNW network morphology during various stretched conditions. It is believed that this flexible, sandwich‐like, electrically conductive membrane is a good candidate for smart wearable devices and soft robots.     

A highly conductive and smooth AgNW/PEDOT:PSS film treated by hot-pressing as electrode for organic light emitting diode

A highly conductive, smooth and transparent electrode is developed by coating poly (3,4-ethylenedioxythiophene):poly (styrenesulfonate) (PEDOT:PSS) over silver nanowires (AgNWs) followed by a hot-pressing method. The hot-pressed AgNW/PEDOT:PSS film shows a low sheet resistance of 12 Ω/square, a transmittance of 83% at 550 nm and a smooth surface. The improvement of the conductivity and smoothness are ascribed to the fusion of nanowires resulted from the mechanical hot-pressing. The AgNW/PEDOT:PSS film on polyethylene naphthalate (PEN) substrate exhibits higher conductive stability against the bending test than commonly used indium tin oxide (ITO). Using the hot-pressed AgNW/PEDOT:PSS film as the anode, we have fabricated ITO-free organic light emitting diode with a maximum current efficiency of 58.2 cd/A, which is higher than the device with ITO anode. This proves that such AgNW/PEDOT:PSS film treated by hot-pressing is a promising candidate for flexible optoelectronic devices.     

A Sensing and Stretchable Polymer-Dispersed Liquid Crystal Device Based on Spiderweb-Inspired Silver Nanowires-Micromesh Transparent Electrode

Polymer-dispersed liquid crystal (PDLC) devices are truly promising optical modulators for information display, smart window as well as intelligent photoelectronic applications due to their fast switching, large optical modulation as well as cost-effectiveness. However, realizing highly soft PDLC devices with sensing function remains a grand challenge because of the intrinsic brittleness of traditional transparent conductive electrodes. Here, inspired by spiderweb configuration, a novel type of silver nanowires (AgNWs) micromesh-based stretchable transparent conductive electrodes (STCEs) is developed to support the realization of soft PDLC device. Benefiting from the embedding design of AgNWs micromesh in polydimethylsiloxane (PDMS), the STCEs can maintain excellent electrical conductivity and transparency even in various extreme conditions such as bending, folding, twisting, stretching as well as multiple chemical corrosion. Further, STCEs with the embedded AgNWs micromesh endow the assembled PDLC device with excellent photoelectrical properties including rapid switching speed (<1 s), large optical modulation (69% at 600 nm), as well as robust mechanical stability (bending over 1000 cycles and stretching to 40%). Moreover, the device displays the pressure sensing function with high sensitivity in response to pressure stimulus. It is conceivable that AgNWs micromesh transparent electrodes will shape the next generation of related soft smart electronics.     

MXene Composite and Coaxial Fibers with High Stretchability and Conductivity for Wearable Strain Sensing Textiles

The integration of nanomaterials with high conductivity into stretchable polymer fibers can achieve novel functionalities such as sensing physical deformations. With a metallic conductivity that exceeds other solution‐processed nanomaterials, 2D titanium carbide MXene is an attractive material to produce conducting and stretchable fibers. Here, a scalable wet‐spinning technique is used to produce Ti₃C₂T_x MXene/polyurethane (PU) composite fibers that show both conductivity and high stretchability. The conductivity at a very low percolation threshold of ≈1 wt% is demonstrated, which is lower than the previously reported values for MXene‐based polymer composites. When used as a strain sensor, the MXene/PU composite fibers show a high gauge factor of ≈12900 (≈238 at 50% strain) and a large sensing strain of ≈152%. The cyclic strain sensing performance is further improved by producing fibers with MXene/PU sheath and pure PU core using a coaxial wet‐spinning process. Using a commercial‐scale knitting machine, MXene/PU fibers are knitted into a one‐piece elbow sleeve, which can track various movements of the wearer's elbow. This study establishes fundamental insights into the behavior of MXene in elastomeric composites and presents strategies to achieve MXene‐based fibers and textiles with strain sensing properties suitable for applications in health, sports, and entertainment.     

Ultrastretchable Helical Conductive Fibers Using Percolated Ag Nanoparticle Networks Encapsulated by Elastic Polymers with High Durability in Omnidirectional Deformations for Wearable Electronics

Stretchable interconnects with invariable conductivity and complete elasticity, which return to their original shape without morphological hysteresis, are attractive for the development of stretchable electronics. In this study, a polydimethylsiloxane‐coated multifilament polyurethane‐based helical conductive fiber is developed. The stretchable helical fibers exhibit remarkable electrical performance under stretching, negligible electrical and mechanical hysteresis, and high electrical reliability under repetitive deformation (10 000 cycles of stretching with 100% strain). The resistance of the helical fibers barely increases until the applied strain reaches the critical strain, which is based on the helical diameter of each fiber. According to finite element analysis, uniform stress distribution is maintained in the helical fibers even under full stretching, owing to the fibers' true helix structure. In addition, the stretchable helical fibers have the ability to completely return to their original shapes even after being fully compressed in the vertical direction. Cylinder‐shaped connecting pieces made using 3D printing are designed for stable connection between the helical fibers and commercial components. A deformable light‐emitting diode (LED) array and biaxially stretchable LED display are fabricated using helical fibers. A skin‐mountable band‐type oximeter with helical fiber‐based electrodes is also fabricated and used to demonstrate real‐time detection of cardiac activities and analysis of brain activities.     

Highly Conductive and Transparent PEDOT:PSS Films with a Fluorosurfactant for Stretchable and Flexible Transparent Electrodes

Highly conductive and transparent poly‐(3,4‐ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) films, incorporating a fluorosurfactant as an additive, have been prepared for stretchable and transparent electrodes. The fluorosurfactant‐treated PEDOT:PSS films show a 35% improvement in sheet resistance (R_s) compared to untreated films. In addition, the fluorosurfactant renders PEDOT:PSS solutions amenable for deposition on hydrophobic surfaces, including pre‐deposited, annealed films of PEDOT:PSS (enabling the deposition of thick, highly conductive, multilayer films) and stretchable poly(dimethylsiloxane) (PDMS) substrates (enabling stretchable electronics). Four‐layer PEDOT:PSS films have an R_s of 46 Ω per square with 82% transmittance (at 550 nm). These films, deposited on a pre‐strained PDMS substrate and buckled, are shown to be reversibly stretchable, with no change to R_s, during the course of over 5000 cycles of 0 to 10% strain. Using the multilayer PEDOT:PSS films as anodes, indium tin oxide (ITO)‐free organic photovoltaics are prepared and shown to have power conversion efficiencies comparable to that of devices with ITO as the anode. These results show that these highly conductive PEDOT:PSS films can not only be used as transparent electrodes in novel devices (where ITO cannot be used), such as stretchable OPVs, but also have the potential to replace ITO in conventional devices.     

Percolating Network of Ultrathin Gold Nanowires and Silver Nanowires toward “Invisible” Wearable Sensors for Detecting Emotional Expression and Apexcardiogram

2 nm thin gold nanowires (AuNWs) have extremely high aspect ratio (≈10 000) and are nanoscale soft building blocks; this is different from conventional silver nanowires (AgNWs), which are more rigid. Here, highly sensitive, stretchable, patchable, and transparent strain sensors are fabricated based on the hybrid films of soft/hard networks. They are mechanically stretchable, optically transparent, and electrically conductive and are fabricated using a simple and cost‐effective solution process. The combination of soft and more rigid nanowires enables their use as high‐performance strain sensors with the maximum gauge factor (GF) of ≈236 at low strain (<5%), the highest stretchability of up to 70% strain, and the optical transparency is from 58.7% to 66.7% depending on the amount of the AuNW component. The sensors can detect strain as low as 0.05% and are energy efficient to operate at a voltage as low as 0.1 V. These attributes are difficult to achieve with a single component of either AuNWs or AgNWs. The outstanding sensing performance indicates their potential applications as “invisible” wearable sensors for biometric information collection, as demonstrated in applications for detecting facial expressions, respiration, and apexcardiogram.     

Buckled Conductive Polymer Ribbons in Elastomer Channels as Stretchable Fiber Conductor

Conductors that can sustain large strains without change in resistance are highly needed for wearable electronic systems. Here, the fabrication of highly stretchable coaxial fiber conductors through self‐buckling of conductive polymer ribbons inside thermoplastic elastomer channels, using a “solution stretching–drying–buckling” process, is reported. The unique hierarchically buckled and conductive core in the axial direction makes the resistance of the fiber very stable, with less than 4% change when applying as much as 680% strain. These fibers can then be directly used as stretchable electrical interconnects or wearable heaters.     

Stretchable Conductive Fibers Based on a Cracking Control Strategy for Wearable Electronics

Stretchability plays an important role in wearable devices. Repeated stretching often causes the conductivity dramatically decreasing due to the damage of the inner conductive layer, which is a fatal and undesirable issue in this field. Herein, a convenient rolling strategy to prepare conductive fibers with high stretchability based on a spiral structure is proposed. With the simple rolling design, low resistance change can be obtained due to confined elongation nof the gold thin‐film cracks, which is caused by the encapsulated effect in such a structure. When the fiber is under 50% strain, the resistance change (R/R₀) is about 1.5, which is much lower than a thin film at the same strain (R/R₀ ≈ 10). The fiber can even afford a high load strain (up to 100%), but still retain good conductivity. Such a design further demonstrates its capability when it is used as a conductor to confirm signal transfer with low attenuation, which can also be woven into textile to fabricate wearable electronics.     

Neutral-pH PEDOT:PSS as over-coating layer for stable silver nanowire flexible transparent conductive films

The silver nanowire (AgNW) mesh film with poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) as the over-coating layer is a promising flexible transparent conductive film technology. In this work, experimental studies show that the hygroscopic and acid properties of the common PEDOT:PSS lead to poor stabilities of the composite films, due to the conductivity degradation of PEDOT:PSS by the water absorption and the acid corrosion of AgNWs by PEDOT:PSS. By using the modified PEDOT:PSS of neutral pH as the over-coating layer, the long term shelf-life time, thermal and current stressing stabilities are all significantly improved without sacrifice of transparency, electrical conductivity and mechanical flexibility. Under both cases of thermal aging test at 210 °C for 20 min and 12 h continuous current stressing at a current density of 30 mA/cm², no obvious change of the conductivity is observed. The results clearly demonstrate that using the neutral-pH PEDOT:PSS as an over-coating layer can help to achieve flexible AgNW transparent conductive films with superior stability for flexible optoelectronic devices.     

Improved Operational Stability of Polymer Light‐Emitting Diodes Based on Silver Nanowire Electrode Through Pre‐Bias Conditioning Treatment

For the first time, highly efficient and flexible polymer light emitting diodes (PLEDs) based on silver nanowire (AgNW) electrode, with improved operational stability by simply applying pre‐bias conditioning treatment, are demonstrated. Reverse bias conditioning performed before J–V–L measurement of the PLEDs enables the rough AgNW networks to function properly as a bottom electrode by stabilizing current characteristics, and the devices continue to show consistent operational performances. Conditions of applied bias and thicknesses of active layer are controlled for optimization and it is found that high reverse voltage is required to obtain current stabilization. Adequate thickness of polymer is also necessary to avoid breakdown induced by reverse bias. The essential effect of pre‐bias conditioning on the improved performances of PLEDs is investigated, and it is found that morphological change of AgNW networks contribute to the improvement in device performance. Some of the AgNWs that appear to be pathway of leakage current are deformed, and surface roughness (RMS) of the AgNW film is decreased while the sheet resistance of the film is maintained when the reverse bias conditioning is applied. It is also revealed that pre‐bias conditioning is independent from directionality of the applied bias when utilizing insulating polymer sandwiched between two electrodes.     

Highly Stretchable Conductors Integrated with a Conductive Carbon Nanotube/Graphene Network and 3D Porous Poly(dimethylsiloxane)

Here, a novel and facile method is reported for manufacturing a new stretchable conductive material that integrates a hybrid three dimensional (3D) carbon nanotube (CNT)/reduced graphene oxide (rGO) network with a porous poly(dimethylsiloxane) (p‐PDMS) elastomer (pPCG). This reciprocal architecture not only alleviates the aggregation of carbon nanofillers but also significantly improves the conductivity of pPCG under large strains. Consequently, the pPCG exhibits high electrical conductivity with a low nanofiller loading (27 S m^?1 with 2 wt% CNTs/graphene) and a notable retention capability after bending and stretching. The simulation of the mechanical properties of the p‐PDMS model demonstrates that an extremely large applied strain (ε_appl) can be accommodated through local rotations and bending of cell walls. Thus, after a slight decrease, the conductivity of pPCG can continue to remain constant even as the strain increases to 50%. In general, this architecture of pPCG with a combination of a porous polymer substrate and 3D carbon nanofiller network possesses considerable potential for numerous applications in next‐generation stretchable electronics.