Highly Conductive,Flexible, Polyurethane‐Based Adhesives for Flexible and Printed Electronics

Flexible interconnects are one of the key elements in realizing next‐generation flexible electronics. While wire bonding interconnection materials are being deployed and discussed widely, adhesives to support flip‐chip and surface‐mount interconnections are less commonly used and reported. A polyurethane (PU)‐based electrically conductive adhesive (ECA) is developed to meet all the requirements of flexible interconnects, including an ultralow bulk resistivity of ≈1.0 × 10^?5 Ω cm that is maintained during bending, rolling, and compressing, good adhesion to various flexible substrates, and facile processing. The PU‐ECA enables various interconnection techniques in flexible and printed electronics: it can serve as a die‐attach material for flip‐chip, as vertical interconnect access (VIA)‐filling and polymer bump materials for 3D integration, and as a conductive paste for wearable radio‐frequency devices.     

Recent Progress of Conductive Hydrogel Fibers for Flexible Electronics: Fabrications,Applications, and Perspectives

Flexible conductive materials with intrinsic structural characteristics are currently in the spotlight of both fundamental science and advanced technological applications due to their functional preponderances such as the remarkable conductivity, excellent mechanical properties, and tunable physical and chemical properties, and so on. Typically, conductive hydrogel fibers (CHFs) are promising candidates owing to their unique characteristics including light weight, high length-to-diameter ratio, high deformability, and so on. Herein, a comprehensive overview of the cutting-edge advances the CHFs involving the architectural features, function characteristics, fabrication strategies, applications, and perspectives in flexible electronics are provided. The fundamental design principles and fabrication strategies are systematically introduced including the discontinuous fabrication (the capillary polymerization and the draw spinning) and the continuous fabrication (the wet spinning, the microfluidic spinning, 3D printing, and the electrospinning). In addition, their potential applications are crucially emphasized such as flexible energy harvesting devices, flexible energy storage devices, flexible smart sensors, and flexible biomedical electronics. This review concludes with a perspective on the challenges and opportunities of such attractive CHFs, allowing for better understanding of the fundamentals and the development of advanced conductive hydrogel materials.     

Room‐Temperature Printing of Organic Thin‐Film Transistors with π‐Junction Gold Nanoparticles

Printing semiconductor devices under ambient atmospheric conditions is a promising method for the large‐area, low‐cost fabrication of flexible electronic products. However, processes conducted at temperatures greater than 150 °C are typically used for printed electronics, which prevents the use of common flexible substrates because of the distortion caused by heat. The present report describes a method for the room‐temperature printing of electronics, which allows thin‐film electronic devices to be printed at room temperature without the application of heat. The development of π‐junction gold nanoparticles as the electrode material permits the room‐temperature deposition of a conductive metal layer. Room‐temperature patterning methods are also developed for the Au ink electrodes and an active organic semiconductor layer, which enables the fabrication of organic thin‐film transistors through room‐temperature printing. The transistor devices printed at room temperature exhibit average field‐effect mobilities of 7.9 and 2.5 cm² V^?1 s^?1 on plastic and paper substrates, respectively. These results suggest that this fabrication method is very promising as a core technology for low‐cost and high‐performance printed electronics.     

Tunable Structural Color Surfaces with Visually Self‐Reporting Wettability

Functional materials with wettability of specific surfaces are important for many areas. Here, a new lubricant‐infused elastic inverse opal is presented with tunable and visually “self‐reporting” surface wettability. The elastic inverse opal films are used to lock in the infused lubricating fluid and construct slippery surfaces to repel droplets of various liquids. The films are stretchable, and the lubricating fluid can penetrate the pores under stretching, leaving the surface layer free of lubrication; the resultant undulating morphology of the inverse opal scaffold topography can reversibly pin droplets on the fluidic film rather than the solid substrate. This mechanical stimulation process provides an effective means of dynamically tuning the surface wettability and the optical transparency of the inverse opal films. In particular, as the adjustments are accompanied by simultaneous deformation of the periodic macroporous structure, the inverse opal films can self‐report on their surface status through visible structural color changes. These features make such slippery structural color materials highly versatile for use in diverse applications.     

Designing Multicolor Micropatterns of Inverse Opals with Photonic Bandgap and Surface Plasmon Resonance

Structural coloration provides unique features over chemical coloration, such as nonfading, color tunability, and high color brightness, rendering it useful in various optical applications. To develop the structural colors, two different mechanisms of coloration–photonic bandgap (PBG) and surface plasmon resonance (SPR)–have been separately utilized. In this work, a new method is suggested to create structurally colored micropatterns by regioselectively employing SPR in a single film of inverse opal with PBG. The inverse opals are prepared by thermal embedding of opal into a negative photoresist and its subsequent removal. The inverse opals have a hexagonal array of open pores on the surface which serves as a template to make SPR‐active nanostructures through a directional deposition of gold, a perforated gold film and an array of curved gold disks are formed. With a shadow mask lithographically prepared, the gold is regioselectively deposited on the surface of the inverse opal, which results in two distinct regions of gold‐free inverse opal with PBG and gold nanostructure with SPR. As PBG and SPR develop their own structural colors respectively, the resultant micropatterns exhibit pronounced dual colors. More importantly, the micropatterns show the distinguished optical response for evaporation of volatile liquids that occupy the pores.     

Paper‐Like,Thin, Foldable,and Self‐Healable Electronics Based on PVA/CNC Nanocomposite Film

The facile fabrication of thin and foldable self‐healing electronics on a poly(vinyl alcohol)/cellulose nanocrystal (PVA/CNC) composite film is reported. The self‐healing property of the PVA/CNC nanocomposite film can be activated by spraying water on the film surface, via dynamic formation of hydrogen bonding. The self‐healing efficiency of PVA/CNC is influenced by the content of CNC in the film, pH of the spraying solution, and the temperature. Via vacuum filtration and pattern transfer techniques, both a supercapacitor and a temperature sensor are fabricated on the same PVA/CNC film using gold nanosheet (AuNS) and polyaniline/multiwalled nanotube (PANI/MWCNT) electrodes. The fabricated supercapacitor with a gel‐type electrolyte exhibits a high electrochemical performance, and the thermoresistive temperature sensor shows a linear sensitivity with a fast response. Both devices exhibit superior mechanical stability and self‐healing property over 100 repetitive folding and five repetitive healing cycles, respectively, retaining the device performance owing to the percolated network of the conductive materials. This work demonstrates that our paper‐like thin PVA/CNC film‐based self‐healable devices can serve as highly durable and deformable electronics with longevity.     

Flexible Breathable Nanomesh Electronic Devices for On‐Demand Therapy

Flexible electronics are drawing tremendous interest for various applications in wearable healthcare biomonitoring, on‐demand therapy, and human–machine interactions. However, conventional plastic substrates with uncomfortableness, mechanical mismatches, and impermeability have limited the application of flexible on‐skin electronic devices for healthcare biomonitoring and on‐demand therapy. Herein, flexible breathable electronic devices with the capabilities of real‐time temperature sensing and timely on‐demand anti‐infection therapy at wound sites are presented. These devices are assembled from a crosslinked electrospun moxifloxacin hydrochloride (MOX)‐loaded thermoresponsive polymer nanomesh film with a conductive pattern. The conductive polymer nanomesh film demonstrates excellent flexibility, reliable breathability, and robust environmental stability. Furthermore, the assembled temperature sensor displays a linear relationship between the electrical resistance and temperature, potentially enabling real‐time biomonitoring of tissue temperature at the wound site. Smart artificial electronic skins (E‐skins) are assembled from the thermoresponsive polymer nanomesh film for spatial touching sensing mapping of temperature changes. Furthermore, the flexible temperature sensor is coupled with a wireless transmitter for real‐time wireless temperature monitoring. Notably, the thermoresponsive polymer nanomesh film can also be assembled as a highly efficient flexible heater to trigger the on‐demand release of antibiotics loaded in the fibers to eliminate bacterial colonization in the wound site once infection has occurred.     

Super‐ and Ultrathin Organic Field‐Effect Transistors: from Flexibility to Super‐ and Ultraflexibility

Physically flexible electronics offer a wide range of benefits, including the development of next‐generation consumer electronics and healthcare products. The advancement of physical flexibility, typically achieved by the reduction of the total device thickness, including substrates and encapsulation layers, shows great promise for skin‐laminated electronics. Organic electronics—devices relying on carbon‐based materials—offer many advantages over their inorganic counterparts, including the following: significantly lower fabrication temperatures resulting in alternative fabrication techniques, including inkjet and roll‐to‐roll printing, enabling low‐cost and large‐area fabrication; biocompatibility; and spectacular physical flexibility. This article presents a review, spanning the last two decades, of organic field‐effect transistors with the total thickness of just a few microns as well as devices demonstrated in this decade with a total thickness of few hundred of nanometers. A handful of demonstrations of other organic electronic thin film devices are also presented.     

Self-Healing Titanium Dioxide Nanocapsules-Graphene/Multi-Branched Polyurethane Hybrid Flexible Film with Multifunctional Properties toward Wearable Electronics

The integration of self-healing capabilities into flexible electronics arouses extensive attention. The application of self-healing electronics with multifunctional properties in a variety of exceptional environments has been identified to be significantly challenging and not yet proven to be fully viable thus far. In the present study, the self-healing octadecane loaded titanium dioxide nanocapsules (OTNs)-graphene/multi-branched polyurethane (PU) hybrid flexible multifunctional film is successfully prepared. The prepared film exhibits a novel self-repair capability that consists of disulfide bonds in the leading chains for efficient self-healing of PU damage, as well as multiple amino groups in the branches for damage between OTNs-graphene and PU. Impacted by the constructed self-healing system and well-dispersed OTNs-graphene, the prepared flexible film demonstrates a prominent performance in piezoresistive sensing and a desirable outcome of ultraviolet protection properties, which can effectively prolong its service life, especially when used outdoors. Moreover, the film exhibits thermal insulating properties, capable of offering a suitable route for thermal protection of bio-integrated wearable electronic devices system. Thus, this self-healing multifunctional film is promising in wearable electronics, human–machine interaction, artificial intelligence devices, etc.     

All‐Printed Flexible and Stretchable Electronics with Pressing or Freezing Activatable Liquid‐Metal–Silicone Inks

Liquid‐metal (LM)‐based flexible and stretchable electronics have attracted widespread interest in wearable computing, human–machine interaction, and soft robotics. However, many current examples are one‐off prototypes, whereas future implementation requires mass production. To address this critical challenge, an integrated multimaterial 3D printing process composed of direct ink writing (DIW) of sealing silicone elastomer and special LM‐silicone (LMS) inks for manufacturing high‐performance LM‐based flexible and stretchable electronics is presented. The LMS ink is a concentrated mixture of LM microdroplets and silicone elastomer and exhibits excellent printability for DIW printing. Guided by a verified theoretical model, a printing process with high resolution and high speed can be easily implemented. Although LMS is not initially conductive, it can be activated by pressing or freezing. Activated LMS possesses good conductivity and significant electrical response to strain. Owing to LMS's unique structure, LMS‐embedded flexible electronics exhibit great damage mitigation, in that no leaking occurs even when damaged. To demonstrate the flexibility of this process in fabricating LM‐based flexible electronics, multilayer soft circuits, strain sensors, and data gloves are printed and investigated. Notably, utilizing LMS's unique activating property, some functional circuits such as one‐time pressing/freezing‐on switch can be printed without any structural design.     

Skin‐Inspired Antibacterial Conductive Hydrogels for Epidermal Sensors and Diabetic Foot Wound Dressings

Recently, artificial intelligence research has driven the development of stretchable and flexible electronic systems. Conductive hydrogels are a class of soft electronic materials that have emerging applications in wearable and implantable biomedical devices. However, current conductive hydrogels possess fundamental limitations in terms of their antibacterial performance and a mechanical mismatch with human tissues, which severely limits their applications in biological interfaces. Here, inspired by animal skin, a conductive hydrogel is fabricated from a supramolecular assembly of polydopamine decorated silver nanoparticles (PDA@Ag NPs), polyaniline, and polyvinyl alcohol, namely PDA@Ag NPs/CPHs. The resultant hydrogel has many desirable features, such as tunable mechanical and electrochemical properties, eye‐catching processability, good self‐healing ability as well as repeatable adhesiveness. Remarkably, PDA@Ag NPs/CPHs exhibit broad antibacterial activity against Gram‐negative and Gram‐positive bacteria. The potential application of this versatile hydrogel is demonstrated by monitoring large‐scale movements of the human body in real time. In addition, PDA@Ag NPs/CPHs have a significant therapeutic effect on diabetic foot wounds by promoting angiogenesis, accelerating collagen deposition, inhibiting bacterial growth, and controlling wound infection. To the best of the authors' knowledge, this is the first time that conductive hydrogels with antibacterial ability are developed for use as epidermal sensors and diabetic foot wound dressing.     

Designing Multicolored Photonic Micropatterns through the Regioselective Thermal Compression of Inverse Opals

Colloidal assemblies develop pronounced structural colors due to the selective diffraction of light. Micropatterns with multiple structural colors are appealing for the use in a variety of photonic applications. Here, a lithographic approach is reported, which provides a high level of control over the size, shape, and color of a micropattern using the anisotropic shrinkage of inverse opals made of a negative photoresist heated to high temperatures. Shrinkage occurs uniformly across the thickness of the film, leading to a blueshift in the structural color while maintaining a high reflectivity across the full visible spectrum. The rate of shrinkage is determined by the annealing temperature and the photoresist crosslinking density. The rate can, therefore, be spatially modulated by applying UV radiation through a photomask to create multicolor micropatterns from single‐colored inverse opals. The lateral dimensions of the micropattern features can be as small as the thickness of the inverse opal.     

Interactively Full‐Color Changeable Electronic Fiber Sensor with High Stretchability and Rapid Response

Smart interactive electronic devices can dynamically respond to and visualize environmental stimuli. Inspired by the rapid color changes of natural creatures, an interactive electronic fiber sensor with high stretchability and tunable coloration is presented. It is based on an ingenious multi‐sheath design on a piezoresistive electronic fiber coupled with a mechanochromic photonic crystal microtubule. It has the unique capabilities of sensing and visualizing its deformation simultaneously, by reconstructing conductive paths and regulating the lattice spacing of the photonic sheath. In particular, it exhibits dynamic color switching spanning the full visible region (from red to blue), fast optical/electrical response (≈80 ms), and a large working range (0–200%), allowing its application as a user‐interactive sensor for dynamically monitoring large joint movements and muscle microvibrations of the human body in real time. This investigation provides a general platform for emerging interactive devices, which are promising for applications in wearable electronics, human–machine interactions, and intelligent robots.     

Hexagonal Boron Nitride–Enhanced Optically Transparent Polymer Dielectric Inks for Printable Electronics

Solution‐processable thin‐film dielectrics represent an important material family for large‐area, fully‐printed electronics. Yet, in recent years, it has seen only limited development, and has mostly remained confined to pure polymers. Although it is possible to achieve excellent printability, these polymers have low (≈2–5) dielectric constants (ε_r). There have been recent attempts to use solution‐processed 2D hexagonal boron nitride (h‐BN) as an alternative. However, the deposited h‐BN flakes create porous thin‐films, compromising their mechanical integrity, substrate adhesion, and susceptibility to moisture. These challenges are addressed by developing a “one‐pot” formulation of polyurethane (PU)‐based inks with h‐BN nano‐fillers. The approach enables coating of pinhole‐free, flexible PU+h‐BN dielectric thin‐films. The h‐BN dispersion concentration is optimized with respect to exfoliation yield, optical transparency, and thin‐film uniformity. A maximum ε_r ≈ 7.57 is achieved, a two‐fold increase over pure PU, with only 0.7 vol% h‐BN in the dielectric thin‐film. A high optical transparency of ≈78.0% (≈0.65% variation) is measured across a 25 cm² area for a 10 μm thick dielectric. The dielectric property of the composite is also consistent, with a measured areal capacitance variation of <8% across 64 printed capacitors. The formulation represents an optically transparent, flexible thin‐film, with enhanced dielectric constant for printed electronics.     

A Skin‐Inspired Substrate with Spaghetti‐Like Multi‐Nanofiber Network of Stiff and Elastic Components for Stretchable Electronics

Mimicking the skin's non‐linear self‐limiting mechanical characteristics is of great interest. Skin is soft at low strain but becomes stiff at high strain and thereby can protect human tissues and organs from high mechanical loads. Herein, the design of a skin‐inspired substrate is reported based on a spaghetti‐like multi‐nanofiber network (SMNN) of elastic polyurethane (PU) nanofibers (NFs) sandwiched between stiff poly(vinyldenefluoride‐co‐trifluoroethylene) (P(VDF‐TrFE)) NFs layers embedded in polydimethylsiloxane elastomer. The elastic moduli of the stretchable skin‐inspired substrate can be tuned in a range that matches well with the mechanical properties of skins by adjusting the loading ratios of the two NFs. Confocal imaging under stretching indicates that PU NFs help maintain the stretchability while adding stiff P(VDF‐TrFE) NFs to control the self‐limiting characteristics. Interestingly, the Au layer on the substrate indicates a negligible change in the resistance under cyclic (up to 7000 cycles at 35% strain) and dynamic stretching (up to 35% strain), which indicates the effective absorption of stress by the SMNN. A stretchable chemoresistive gas sensor on the skin‐inspired substrate also demonstrates a reasonable stability in NO₂ sensing response under strain up to 30%. The skin‐inspired substrate with SMNN provides a step toward ultrathin stretchable electronics.     

Microflotronics: A Flexible,Transparent, Pressure‐Sensitive Microfluidic Film

There is an increasing demand for sensitive, flexible, and low‐cost pressure sensing solutions for health monitoring, wearable sensing, robotic and prosthetic applications. Here, the first flexible and pressure‐sensitive microfluidic film is reported, referred to as a microflotronic, with high transparency and seamless integratability with the state‐of‐the‐art microelectronics. The microflotronic film represents the initial effort to utilize a continuous microfluidic layer as the sensing elements for large‐area dynamic pressure mapping applications, and meanwhile an ultrahigh sensitivity of 0.45 kPa^?1 has been achieved in a compact, flexible, and transparent packaging. The response time of the device is in the millisecond range, which is at least an order of magnitude faster than that of its conventional flexible solid‐state counterparts. In addition, the fabrication process of the device is fully compatible with the industrial‐scale manufacturing of capacitive touchscreen devices and liquid‐crystal displays. The overall device packaging can be as thin as 200 μm with an optical transparency greater than 80%. Several practical applications were successfully demonstrated, including surface topology mapping and dynamic blood pressure monitoring. The microflotronic devices offer an alternative approach to the solid‐state pressure sensors, by offering an unprecedented sensitivity and ultrafast response time in a completely transparent, flexible and adaptive platform.     

Wearable and Implantable Devices for Cardiovascular Healthcare: from Monitoring to Therapy Based on Flexible and Stretchable Electronics

Cardiovascular disease is the leading cause of death and has dramatically increased in recent years. Continuous cardiac monitoring is particularly important for early diagnosis and prevention, and flexible and stretchable electronic devices have emerged as effective tools for this purpose. Their thin, soft, and deformable features allow intimate and long‐term integration with biotissues, which enables continuous, high‐fidelity, and sometimes large‐area cardiac monitoring on the skin and/or heart surface. In addition to monitoring, intimate contact is also crucial for high‐precision therapies. Combined with tissue engineering, soft bioelectronics have also demonstrated the capability to repair damaged cardiac tissues. This review highlights the recent advances in wearable and implantable devices based on flexible and stretchable electronics for cardiovascular monitoring and therapy. First, wearable/implantable soft bioelectronics for cardiovascular monitoring (e.g., the electrocardiogram, blood pressure, and oxygen saturation level) are reviewed. Then, advances in cardiovascular therapy based on soft bioelectronics (e.g., mesh pacing, ablation, robotic sleeves, and electronic stents) are discussed. Finally, device‐assisted tissue engineering therapy (e.g., functional electronic scaffolds and in vitro cardiac platforms) is discussed.     

Water‐Based Isotropically Conductive Adhesives: Towards Green and Low‐Cost Flexible Electronics

This paper reports the first high‐performance water‐based isotropically conductive adhesives (WBICAs) – a promising material for both electrical interconnects and printed circuits for ultralow‐cost flexible/foldable printed electronics. Through combining surface iodination and in situ reduction treatment, the electrically conductivity of the WBICAs are dramatically improved (8 × 10^‐5 Ω cm with 80 wt% of silver); moreover, their reliability (stable for at least 1440 h during 85 °C/85% RH aging) meets the essential requirements for microelectronic applications. Prototyped applications in carrying light emitting diode (LED) arrays and radio frequency identification (RFID) antennas on flexible substrates were demonstrated, which showed satisfactory performances. Moreover, their water‐based character may render them more environmentally benign (no volatile organic chemicals involved in the printing and machine maintenance processes), more convenient in processing (reducing the processing steps), and energy economic (thermally sintering the silver fillers and curing the resin is not necessary unlike conventional ICAs). Therefore, they are especially advantageous for mass‐fabricating flexible electronic devices when coupled with paper and other low‐cost substrate materials such as PET, PI, wood, rubber, and textiles.     

Seriography‐Guided Reduction of Graphene Oxide Biopapers for Wearable Sensory Electronics

Novel nacre‐mimic bio‐nanocomposites, such as graphene‐based laminates, are pushing the boundaries of strength and toughness as flexible engineering materials. Translating these material advances to functional flexible electronics requires methods for generating print‐scalable microcircuits (conductive elements surrounded by dielectric) into these strong, tough, lightweight bio‐nanocomposites. Here, a new paradigm for printing flexible electronics by employing facile, eco‐friendly seriography to confine the reduction of graphene oxide biopapers reinforced by silk interlayers is presented. Well‐defined, micropatterned regions on the biopaper are chemically reduced, generating a 10⁶ increase in conductivity (up to 10⁴ S m^?1). Flexible, robust graphene‐silk circuits are showcased in diverse applications such as resistive moisture sensors and capacitive proximity sensors. Unlike conductive (i.e., graphene‐ or Ag nanoparticle‐loaded) inks printed onto substrates, seriography‐guided reduction does not create mechanically weak interfaces between dissimilar materials and does not require the judicious formation of ink. The unimpaired functionality of printed‐in graphene‐silk microcircuits after thousands of punitive folding cycles and chemical attack by harsh solvents is demonstrated. This novel approach provides a low‐cost, portable solution for printing micrometer‐scale conductive features uniformly across large areas (>hundreds of cm²) in layered composites for applications including wearable health monitors, electronic skin, rollable antennas, and conformable displays.     

Recent Advances in Pen‐Based Writing Electronics and their Emerging Applications

The emerging demand for cost‐effective, easily accessible, and rapid prototyping electronics fabrication calls for novel techniques to design and manufacture electronic components and devices for wearable functional sensing, on‐skin medical monitoring, and body‐worn energy conversion. Inspired by daily hand‐writing, innovative and ubiquitously available pens can be employed to write conductive patterns on multiple substrates; such a low‐cost, fast, and user‐friendly direct writing paradigm has recently aroused remarkable research interest as a promising electronics prototyping strategy. In this review, state‐of‐art advances in techniques for direct writing of electronics are presented, and pros and cons of each fabrication route are discussed. Emerging applications of pen‐based writing electronics are also summarized. Based on these, final conclusions, limitations and challenges, as well as ongoing perspectives are illustrated.