Rational Design of a Flexible CNTs@PDMS Film Patterned by Bio‐Inspired Templates as a Strain Sensor and Supercapacitor

Flexible devices integrated with sensing and energy storage functions are highly desirable due to their potential application in wearable electronics and human motion detection. Here, a flexible film is designed in a facile and low‐cost leaf templating process, comprising wrinkled carbon nanotubes (CNTs) as the conductive layer and patterned polydimethylsiloxane (PDMS) with bio‐inspired microstructure as a soft substrate. Assembled from wrinkled CNTs on patterned PDMS film, a strain sensor is realized to possess sensitive resistance response against various deformations, producing a resistance response of 0.34%, 0.14%, and 9.1% under bending, pressing, and 20% strain, respectively. Besides, the strain sensor can reach a resistance response of 3.01 when stretched to 44%. Furthermore, through the electro‐deposition of polyaniline, the CNTs film is developed into a supercapacitor, which exhibits a specific capacitance of 176 F g^?1 at 1 A g^?1 and a capacitance retention of 88% after 10 000 cycles. In addition, the fabricated supercapacitor shows super flexibility, delivering a capacitance retention of 98% after 180° bending for 100 cycles, 95% after 45° twisting for 100 cycles, and 98% after 100% stretching for 400 cycles. The superior capacitance stability demonstrates that the design of wrinkled CNTs‐based electrodes fixed by microstructures is beneficial to the excellent electrochemical performance.     

A Through-Thickness Arrayed Carbon Fibers Elastomer with Horizontal Segregated Magnetic Network for Highly Efficient Thermal Management and Electromagnetic Wave Absorption

Multifunctional thermal management materials with highly efficient electromagnetic wave (EMW) absorption performance are urgently required to tackle the heat dissipation and electromagnetic interference issues of high integrated electronics. However, the high thermal conductivity (λ) and outstanding EMW absorption performance are often incompatible with each other in a single material. Herein, a through-thickness arrayed NiCo₂O₄/graphene oxide/carbon fibers (NiCO@CFs) elastomer with integrated functionalities of high thermal conductivity, highly efficient EMW absorption, and excellent compressibility is reported. The NiCO@CFs elastomer realizes a high out-of-plane thermal conductivity of 15.55 W m⁻¹ K⁻¹, due to the through-thickness vertically aligned CFs framework. Moreover, the unique horizontal segregated magnetic network effectively reduces the electrical contact between the CFs, which significantly enhances impedance matching of NiCO@CFs elastomer. As a result, the vertically arrayed NiCO@CFs elastomer synchronously exhibits ultrabroad effective absorption bandwidth of 8.25 GHz (9.75–18 GHz) at a thickness of 2.4 mm, good impedance matching, and a minimum reflection loss (RL_min) of −55.15 dB. Given these outstanding findings, the multifunctional arrayed NiCO@CFs elastomer opens an avenue for applications in EMW absorption and thermal management. This strategy of constructing thermal/electrical/mechanical pathways provides a promising way for the high-performance multifunctional materials in electronic devices.     

Forming wrinkled stiff films on polymeric substrates at room temperature for stretchable interconnects applications

Periodically wrinkled stiff thin films on elastomeric substrates have been found extensive applications, such as in stretchable electronics. This paper presents a cost-effective and simple method to form wrinkled stiff SiO_x thin films on polydimethylsiloxane (PDMS) substrates at room temperature by ultraviolet/ozone (UV/O) radiation on pre-strained PDMS. Systemic studies have been conducted to understand the dependence of the wavy profile on the PDMS pre-strain, UV/O exposure time, and PDMS modulus. The mechanics analysis has been verified to be quantitatively or qualitatively accurate by experimental comparisons. The wrinkled SiO_x/PDMS system is stretchable and provides a wavy mold for stretchable electrodes. The constant electrical resistance during mechanical stretching shows the stretchability of this system.     

Cryo‐Transferred Ultrathin and Stretchable Epidermal Electrodes

A simple cryo‐transfer method to fabricate ultrathin, stretchable, and conformal epidermal electrodes based on a combination of silver nanowires (AgNWs) network and elastomeric polymers is developed. This method can temporarily enable the soft elastomers with much higher elastic modulus and dimensional contraction through exploiting their glass‐transition behaviors. During this process, a much higher Von Mises stress can be loaded on AgNWs than usual, and the generated strong grip force can facilitate the complete transfer of AgNWs. Afterward, the thawed AgNWs and elastomer composites quickly recover to their soft state at room temperature. The obtained ultrathin and soft electrode with a thickness of 8.4 µm and transmittance of 90.8% at a sheet resistance of 13.2 Ω sq^?1 can tolerate a stretching strain of 70% and 50 000 repeated bending cycles, which meets rigorous requirements of epidermal applications. The as‐prepared epidermal electrodes are effective and comfortable for electrophysiological signal monitoring, and while showing excellent performance exceeding the commercialized gel electrodes.     

Plasticizing Silk Protein for On‐Skin Stretchable Electrodes

Soft and stretchable electronic devices are important in wearable and implantable applications because of the high skin conformability. Due to the natural biocompatibility and biodegradability, silk protein is one of the ideal platforms for wearable electronic devices. However, the realization of skin‐conformable electronic devices based on silk has been limited by the mechanical mismatch with skin, and the difficulty in integrating stretchable electronics. Here, silk protein is used as the substrate for soft and stretchable on‐skin electronics. The original high Young's modulus (5–12 GPa) and low stretchability (<20%) are tuned into 0.1–2 MPa and > 400%, respectively. This plasticization is realized by the addition of CaCl₂ and ambient hydration, whose mechanism is further investigated by molecular dynamics simulations. Moreover, highly stretchable (>100%) electrodes are obtained by the thin‐film metallization and the formation of wrinkled structures after ambient hydration. Finally, the plasticized silk electrodes, with the high electrical performance and skin conformability, achieve on‐skin electrophysiological recording comparable to that by commercial gel electrodes. The proposed skin‐conformable electronics based on biomaterials will pave the way for the harmonized integration of electronics into human.     

Highly Conductive Ti3C2Tx MXene Hybrid Fibers for Flexible and Elastic Fiber‐Shaped Supercapacitors

Fiber‐shaped supercapacitors (FSCs) are promising energy storage solutions for powering miniaturized or wearable electronics. However, the scalable fabrication of fiber electrodes with high electrical conductivity and excellent energy storage performance for use in FSCs remains a challenge. Here, an easily scalable one‐step wet‐spinning approach is reported to fabricate highly conductive fibers using hybrid formulations of Ti₃C₂T_x MXene nanosheets and poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate. This approach produces fibers with a record conductivity of ≈1489 S cm^?1, which is about five times higher than other reported Ti₃C₂T_x MXene‐based fibers (up to ≈290 S cm^?1). The hybrid fiber at ≈70 wt% MXene shows a high volumetric capacitance (≈614.5 F cm^?3 at 5 mV s^?1) and an excellent rate performance (≈375.2 F cm^?3 at 1000 mV s^?1). When assembled into a free‐standing FSC, the energy and power densities of the device reach ≈7.13 Wh cm^?3 and ≈8249 mW cm^?3, respectively. The excellent strength and flexibility of the hybrid fibers allow them to be wrapped on a silicone elastomer fiber to achieve an elastic FSC with 96% capacitance retention when cyclically stretched to 100% strain. This work demonstrates the potential of MXene‐based fiber electrodes and their scalable production for fiber‐based energy storage applications.     

Visually Imperceptible Liquid‐Metal Circuits for Transparent,Stretchable Electronics with Direct Laser Writing

A material architecture and laser‐based microfabrication technique is introduced to produce electrically conductive films (sheet resistance = 2.95 Ω sq^?1; resistivity = 1.77 × 10^?6 Ω m) that are soft, elastic (strain limit >100%), and optically transparent. The films are composed of a grid‐like array of visually imperceptible liquid‐metal (LM) lines on a clear elastomer. Unlike previous efforts in transparent LM circuitry, the current approach enables fully imperceptible electronics that have not only high optical transmittance (>85% at 550 nm) but are also invisible under typical lighting conditions and reading distances. This unique combination of properties is enabled with a laser writing technique that results in LM grid patterns with a line width and pitch as small as 4.5 and 100 µm, respectively—yielding grid‐like wiring that has adequate conductivity for digital functionality but is also well below the threshold for visual perception. The electrical, mechanical, electromechanical, and optomechanical properties of the films are characterized and it is found that high conductivity and transparency are preserved at tensile strains of ≈100%. To demonstrate their effectiveness for emerging applications in transparent displays and sensing electronics, the material architecture is incorporated into a couple of illustrative use cases related to chemical hazard warning.     

Stretchable Organometal‐Halide‐Perovskite Quantum‐Dot Light‐Emitting Diodes

Stretchable light‐emitting diodes (LEDs) and electroluminescent capacitors have been reported to potentially bring new opportunities to wearable electronics; however, these devices lack in efficiency and/or stretchability. Here, a stretchable organometal‐halide‐perovskite quantum‐dot LED with both high efficiency and mechanical compliancy is demonstrated. The hybrid device employs an ultrathin (<3 µm) LED structure conformed on a surface‐wrinkled elastomer substrate. Its luminescent efficiency is up to 9.2 cd A^?1, which is 70% higher than a control diode fabricated on the rigid indium tin oxide/glass substrate. Mechanical deformations up to 50% tensile strain do not induce significant loss of the electroluminescent property. The device can survive 1000 stretch–release cycles of 20% tensile strain with small fluctuations in electroluminescent performance.     

Fabrication of Highly Stretchable Conductors via Morphological Control of Carbon Nanotube Network

Stretchable conductors, which can keep their excellent electrical conductivity while highly stretched, have been investigated extensively due to their wide range of applications in flexible and stretchable electronics, wearable displays, etc.; however, their preparation is often complicated and expensive. Herein, an efficient method to prepare high performance stretchable conductors through morphological control of conductive networks formed with carbon nanotubes (CNTs) in an elastomer matrix is reported. It is observed that an interface‐mediated method could be used to align randomly oriented filler during stretching and to induce buckling of CNTs during relaxation. Further morphological studies indicate the possible formation of a wavy CNT structure induced by cyclic pre‐straining. Subsequent thermal annealing is observed to collapse the oriented network and improve the local contacts between conductive networks. Through such a simple procedure, a conductivity of nearly 1000 S m^?1 and a stretchability of 200% can be achieved for composites containing 20 wt% CNTs. CNTs are observed to buckle over a large area in polymer bulk, and the combination of pre‐straining and thermal annealing modifies the conductive network in the elastomer matrix. As a general method, this could be used for easy fabrication of high‐performance stretchable conductors for arbitrary‐shaped objects on a large scale.     

Stretchable,Electrochemically-Stable Electrochromic Devices Based on Semi-Embedded Ag@Au Nanowire Network

Stretchable electrochromic (EC) devices that can adapt the irregular and dynamic human surfaces show promising applications in wearable display, adaptive camouflage, and visual sensation. However, challenges exist in lacking transparent conductive electrodes with both tensile and electrochemical stability to assemble the complex device structure and endure harsh electrochemical redox reactions. Herein, a wrinkled, semi-embedded Ag@Au nanowire (NW) networks are constructed on elastomer substrates to fabricate stretchable, electrochemically-stable conductive electrodes. The stretchable EC devices are then fabricated by sandwiching a viologen-based gel electrolyte between two conductive electrodes with the semi-embedded Ag@Au NW network. Because the inert Au layer inhibits the oxidation of Ag NWs, the EC device exhibits much more stable color changes between yellow and green than those with pure Ag NW networks. In addition, since the wrinkled semi-embedded structure is deformable and reversibly stretched without serious fractures, the EC devices still maintain excellent color-changing stability under 40% stretching/releasing cycles.     

Ultrastretchable Conductor Fabricated on Skin‐Like Hydrogel–Elastomer Hybrid Substrates for Skin Electronics

Printing technology can be used for manufacturing stretchable electrodes, which represent essential parts of wearable devices requiring relatively high degrees of stretchability and conductivity. In this work, a strategy for fabricating printable and highly stretchable conductors are proposed by transferring printed Ag ink onto stretchable substrates comprising Ecoflex elastomer and tough hydrogel layers using a water‐soluble tape. The elastic modulus of the produced hybrid film is close to that of the hydrogel layer, since the thickness of Ecoflex elastomer film coated on hydrogel is very thin (30 µm). Moreover, the fabricated conductor on hybrid film is stretched up to 1780% strain. The described transfer method is simpler than other techniques utilizing elastomer stamps or sacrificial layers and enables application of printable electronics to the substrates with low elastic moduli (such as hydrogels). The integration of printed electronics with skin‐like low‐modulus substrates can be applied to make wearable devices more comfortable for human skin.     

Constructing Carbon Nanotube Hybrid Fiber Electrodes with Unique Hierarchical Microcrack Structure for High-Voltage,Ultrahigh-Rate,and Ultralong-Life Flexible Aqueous Zinc Batteries

Flexible aqueous zinc batteries are promising candidates as safe power sources for fast-growing portable and wearable electronics. However, the low working voltage, poor rate capability, and cycling stability have greatly restricted their development and applications. Here, a new family of flexible bimetallic phosphide/carbon nanotube hybrid fiber electrodes with unique macroscopic microcrack structure and microscopic porous nanoflower structure is reported. The hierarchical microcrack structure not only facilitates the penetration of electrolyte for effective exposure of active sites, but also can serve as buffers to relieve the stress concentrations of the fiber electrode under deformations, enabling impressive electrochemical performance and mechanical flexibility. Particularly, the fabricated flexible aqueous zinc batteries demonstrate high working voltage plateau and specific capacity (≈1.7 V, 258.9 mAh g⁻¹ at 2 A g⁻¹), ultrahigh rate capability (135.8 mAh g⁻¹ at 50 A g⁻¹, fully charged in only 9.8 s) and impressive power density of 79 000 W kg⁻¹. Moreover, the flexible batteries show ultralong cycling life with 74.6% capacity retention after 20 000 cycles. The fiber batteries are also highly flexible and can be easily knitted into soft electronic textiles to power a smartphone, which are particularly promising for the next-generation of flexible and wearable electronics.     

Inside Front Cover: Buckled and Wavy Ribbons of GaAs for High‐Performance Electronics on Elastomeric Substrates (Adv. Mater. 21/2006)

Stretchable single‐crystalline GaAs nanoribbons and stretchable electronic devices fabricated with these ribbons are reported on p. 2857 by Sun, Rogers, and co‐workers. The inside cover shows an array of ‘wavy' GaAs nanoribbons (background) sitting on an elastomeric poly(dimethylsiloxane) (PDMS) support. Wavy and buckled ribbons integrated with metal electrodes (foreground inset) enable high‐performance, fully stretchable electronics, i.e., metal–semiconductor field‐effect transistors.     

Layer‐by‐Layer Assembled Oxide Nanoparticle Electrodes with High Transparency,Electrical Conductivity,and Electrochemical Activity by Reducing Organic Linker‐Induced Oxygen Vacancies

Solution‐processable transparent conducting oxide (TCO) nanoparticle (NP)–based electrodes are limited by their low electrical conductivity, which originates from the low level of oxygen vacancies within NPs and the contact resistance between neighboring NPs. Additionally, these electrodes suffer from the troublesome trade‐off between electrical conductivity and optical transmittance and the restricted shape of substrates (i.e., only flat substrates). An oxygen‐vacancy‐controlled indium tin oxide (ITO) NP‐based electrode is introduced using carbon‐free molecular linkers with strong chemically reducing properties. Specifically, ITO NPs are layer‐by‐layer assembled with extremely small hydrazine monohydrate linkers composed of two amine groups, followed by thermal annealing. This approach markedly improves the electrical conductivity of ITO NP‐based electrodes by significantly increasing the level of oxygen vacancies and decreasing the interparticle distance (i.e., contact resistance) without sacrificing optical transmittance. The prepared electrodes surpass the optical/electrical performance of TCO NP‐based electrodes reported to date. Additionally, the nanostructured ITO NP films can be applied to more complex geometric substrates beyond flat substrates, and furthermore exhibit a prominent electrochemical activity. This approach can provide an important basis for developing a wide range of highly functional transparent conducting electrodes.     

Kirigami‐Inspired Nanoconfined Polymer Conducting Nanosheets with 2000% Stretchability

Stretchable conductors are essential components of wearable electronics. However, such materials typically sacrifice their electronic conductivity to achieve mechanical stretchability and elasticity. Here, the nanoconfinement and air/water interfacial assembly is explored to grow freestanding mechanical endurance conducting polymer nanosheets that can be stretched up to 2000% with simultaneously high electrical conductivity, inspired by kirigami. Such stretchable conductors show remarkable electronic and mechanical reversibility and reproducibility under more than 1000 cycle durability tests with 2000% deformability, which can be accurately predicted using finite element modeling. The conductivity of nanoconfined freestanding conductor nanosheets increases by three orders of magnitude from 2.2 × 10^?3 to 4.002 S cm^?1 is shown, due to the charge‐transfer complex formation between polymer chain and halogen, while the electrical conductance of the stretchable kirigami nanosheets can be maintained over the entire strain regime. The nanoconfined polymer nanosheets can also act as a sensor capable of sensing the pressure with high durability and real‐time monitoring.     

An Efficiently Doped PEDOT:PSS Ink Formulation via Metastable Liquid−Liquid Contact for Capillary Flow-Driven,Hierarchically and Highly Conductive Films

With commercial electronics transitioning toward flexible devices, there is a growing demand for high-performance polymers such as poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS). Previous breakthroughs in promoting the conductivity of PEDOT:PSS, which mainly stem from solvent-treatment and transfer-printing strategies, remain as inevitable challenges due to the inefficient, unstable, and biologically incompatible process. Herein, a scalable fabrication of conducting PEDOT:PSS inks is reported via a metastable liquid−liquid contact (MLLC) method, realizing phase separation and removal of excess PSS simultaneously. MLLC-doped inks are further used to prepare ring-like films through a compromise between the coffee-ring effect and the Marangoni vortex during evaporation of droplets. The specific control over deposition conditions allows for tunable ring-like morphologies and preferentially interconnected networks of PEDOT:PSS nanofibrils, resulting in a high electrical conductivity of 6,616 S cm⁻¹ and excellent optical transparency of the film. The combination of excellent electrical properties and the special morphology enables it to serve as electrodes for touch sensors with gradient pressure sensitivity. These findings not only provide new insight into developing a simple and efficient doping method for commercial PEDOT:PSS ink, but also offer a promising self-assembled deposition pattern of organic semiconductor films, expanding the applications in flexible electronics, bioelectronics as well as photovoltaic devices.     

Roll‐to‐Roll Production of Graphene Hybrid Electrodes for High‐Efficiency,Flexible Organic Photoelectronics

Despite nearly two decades of research, the absence of ideal, flexible, and transparent electrodes has been the biggest bottleneck for realizing flexible and printable electronics via roll‐to‐roll (R2R) method. A fabrication of poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate):graphene:ethyl cellulose (PEDOT:PSS:G:EC) hybrid electrodes by R2R process, which allows for the elimination of strong acid treatment. The high‐performance flexible printable electrode includes a transmittance (T) of 78% at 550 nm and a sheet resistance of 13 Ω sq⁻¹ with excellent mechanical stability. These features arise from the PSS interacting strongly with the ethyoxyl groups from EC promoting a favorable phase separation between PEDOT and PSS chains, and the highly uniform and conductive G:EC enable rearrangement of the PEDOT chains with more expanded conformation surrounded by G:EC via the π–π interaction between G:EC and PEDOT. The hybrid electrodes are fully functional as universal electrodes for outstanding flexible electronic applications. Organic solar cells based on the hybrid electrode exhibit a high power conversion efficiency of 9.4% with good universality for active layer. Moreover, the organic light‐emitting diodes and photodetector devices hold the same level to or outperform those based on indium tin oxide flexible transparent electrodes.     

High-stability conducting polymer-based conformal electrodes for bio-/iono-electronics

Compared to conventional rigid electronics, polymer-based soft electronics conformal to organisms of irregular shapes have emerged as the next-generation devices, especially benefiting long-term bio-interface interactions that avoid mechanical mismatch and consequent adverse immune responses. Highly conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) has become a promising candidate for building soft conductors/electrodes due to its good conductance, tunable mechanical stiffness, good biocompatibility and facile fabrication into various structures. However, their high instability towards alkaline, reductants and applied voltage has not yet been fully addressed, which inevitably leads to deteriorated performance in complex physiological environments or weather conditions (e.g., humidity). Such intolerances are rooted in unstable electronic/molecular structures of PEDOT caused by de-doping. Besides the low electrical stability, PEDOT:PSS films also exhibit an impaired overall conductance due to its phase separation into PSS-rich and PEDOT-rich domains. Herein, a general and effective coating strategy is proposed, based on a mechanism of simultaneous molecular rejection and electron conjugation, to improve the stability and boost the conductance. Specifically, a reduced-graphene-oxide (rGO) thin layer can not only protect PEDOT: PSS from being de-doped by alkali, bio-reductants and applied voltage through molecular rejection, to maintain its conductivity and ensure stable functions, but also further boost the overall conductance through a bridging effect with its large conjugated domain. This strategy is compatible with various material fabrication techniques, including blade-coating, dip-coating and extrusion-based printing techniques, enabling the fabrication of conductors/electrodes with different structures. Finally, the advantages of excellent stability and high conformability of the composite films as soft conductors have been demonstrated through practical applications in tissue stimulation, electrophysiological recording and proprioceptive hydrogel skins, exhibiting great promise in bio/iono-electronics and human–machine interactions.     

Intertwined Nanocarbon and Manganese Oxide Hybrid Foam for High‐Energy Supercapacitors

Rapid charging and discharging supercapacitors are promising alternative energy storage systems for applications such as portable electronics and electric vehicles. Integration of pseudocapacitive metal oxides with single‐structured materials has received a lot of attention recently due to their superior electrochemical performance. In order to realize high energy‐density supercapacitors, a simple and scalable method is developed to fabricate a graphene/MWNT/MnO₂ nanowire (GMM) hybrid nanostructured foam, via a two‐step process. The 3D few‐layer graphene/MWNT (GM) architecture is grown on foamed metal foils (nickel foam) via ambient pressure chemical vapor deposition. Hydrothermally synthesized α‐MnO₂ nanowires are conformally coated onto the GM foam by a simple bath deposition. The as‐prepared hierarchical GMM foam yields a monographical graphene foam conformally covered with an intertwined, densely packed CNT/MnO₂ nanowire nanocomposite network. Symmetrical electrochemical capacitors (ECs) based on GMM foam electrodes show an extended operational voltage window of 1.6 V in aqueous electrolyte. A superior energy density of 391.7 Wh kg^?1 is obtained for the supercapacitor based on the GMM foam, which is much higher than ECs based on GM foam only (39.72 Wh kg^?1). A high specific capacitance (1108.79 F g^?1) and power density (799.84 kW kg^?1) are also achieved. Moreover, the great capacitance retention (97.94%) after 13 000 charge–discharge cycles and high current handability demonstrate the high stability of the electrodes of the supercapacitor. These excellent performances enable the innovative 3D hierarchical GMM foam to serve as EC electrodes, resulting in energy‐storage devices with high stability and power density in neutral aqueous electrolyte.     

纳米纤维素-聚吡咯/天然橡胶柔性导电弹性体的制备与性能

以纤维素纳米纤丝（Cellulose nanofibrils,CNFs）为生物模板,将聚吡咯（Polypyrrole,PPy）原位聚合在CNFs表面,再将CNF-PPy复合物均匀分散到天然橡胶（Natural rubber,NR）弹性基体中,制备了具有高柔韧性的纳米纤维素-聚吡咯/天然橡胶（CNF-PPy/NR）导电弹性体。结果表明：CNFs可协助PPy在NR基体中形成三维导电网络结构,并提高弹性体的力学性能和导电性能,有效降低其逾渗阈值。当添加质量比为5%（以橡胶质量为基准,下同）的CNF和20%的PPy时,CNF-PPy/NR的拉伸强度可达（8.97±0.92）MPa,分别约为PPy/NR及纯NR的1.56倍和9.54倍,电导率可达（0.134±0.063）S/m;在0.3 A/g的电流密度下,比电容可达96 F/g,并在1.0 A/g电流密度下循环充放电1 200次后,比电容仍可保持其初始值的72%。此导电弹性体具有良好的力学强度和电学性能,有望应用于柔性有机电子器件领域。