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.     

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.     

Shape-Engineerable Silk Fibroin Papers for Ideal Substrate Alternatives of Plastic Electronics

Plastic-based electronics fill the gaps in conventional rigid silicon-based devices toward the applications in soft interfaces. However, people in the future should also consider their potential environmental impact if tons of non-degradable plastics are applied. Silk fibroin is a superior substrate alternative for the development of “green” electronics; whereas, the brittleness of silk films is still a major limitation impeding their practical use. Different from the widely reported polyphasic composite approaches, here a trace-ion-assisted plasticization strategy is developed, and shape-engineerable pure silk fibroin paper (PSFP) is prepared for the first time, which can be engraved and crumpled like a sheet of paper in the dry state. The PSFPs exhibit higher tensile fracture energy (14.4 ± 4 kJ m⁻²) than any typical plastic-electronic-substrates as far as it is known. The intrinsic brittleness of pure silk films is overcome, and the PSFP can be easily engineered to form periodic meshes, electronic prototypes, and kirigami-based devices, which are beyond the reported regenerated silk films or silk composite films. Moreover, the scrape coating method employed here is simple, highly repeatable, and suitable for scaled production of low-cost PSFP continuously. Collectively, the PSFP is generalizable to various shapes and devices, represents an ideal substrate alternative to plastic electronics.     

Ultrafast Laser Pulses Enable One‐Step Graphene Patterning on Woods and Leaves for Green Electronics

Fast, simple, cost‐efficient, eco‐friendly, and design‐flexible patterning of high‐quality graphene from abundant natural resources is of immense interest for the mass production of next‐generation graphene‐based green electronics. Most electronic components have been manufactured by repetitive photolithography processes involving a large number of masks, photoresists, and toxic etchants; resulting in slow, complex, expensive, less‐flexible, and often corrosive electronics manufacturing processes to date. Here, a one‐step formation and patterning of highly conductive graphene on natural woods and leaves by programmable irradiation of ultrafast high‐photon‐energy laser pulses in ambient air is presented. Direct photoconversion of woods and leaves into graphene is realized at a low temperature by intense ultrafast light pulses with controlled fluences. Green graphene electronic components of electrical interconnects, flexible temperature sensors, and energy‐storing pseudocapacitors are fabricated from woods and leaves. This direct graphene synthesis is a breakthrough toward biocompatible, biodegradable, and eco‐friendlily manufactured green electronics for the sustainable earth.     

Cutting Edge Use of Conductive Patterns in Nanocellulose-Based Green Electronics

Green electronics made from degradable materials have recently attracted special attention, because electronic waste (e-waste) represents a serious threat to the environment and to human health worldwide. Among the novel materials used for sustainable technologies, nanocelluloses containing at least 1D in the nanoscale range (1–100 nm) have been widely exploited for various industrial applications owing to their inherent properties, such as biodegradability, mechanical strength, thermal stability, and optical transparency. This review highlights recent advances in research on the development of patterns for conductive material on nanocellulose substrates for use in high-performance green electronics. The advantages of nanocellulose substrates compared to conventional paper substrates for advanced green electronics are discussed. Importantly, this review emphasizes various fabrication strategies for producing conductive patterns on different types of nanocellulose-based substrates, such as cellulose nanofiber (CNF), (2,2,6,6-tetramethylpiperidin-1-yl)oxyl(TEMPO)-oxidized CNF, regenerated cellulose, and bacterial cellulose. In the latter part of this review, emerging engineering applications for green electronics such as circuits, transistors/antennas, sensors, energy storage systems, and electrochromic devices are further discussed.     

Liquid Metal Droplets Wrapped with Polysaccharide Microgel as Biocompatible Aqueous Ink for Flexible Conductive Devices

Nanometerization of liquid metal in organic systems can facilitate deposition of liquid metals onto substrates and then recover its conductivity through sintering. Although having broader potential applications, producing stable aqueous inks of liquid metals keeps challenging because of rapid oxidation of liquid metal when exposing to water and oxygen. Here, a biocompatible aqueous ink is produced by encapsulating alloy nanodroplets of gallium and indium (EGaIn) into microgels of marine polysaccharides. During sonicating bulk EGaIn in aqueous alginate solution, alginate not only facilitates the downsizing process via coordination of their carboxyl groups with Ga ions but also forms microgel shells around EGaIn droplets. Due to the deceasing oxygen‐permeability of microgel shells, aqueous ink of EGaIn nanodroplets can maintain colloidal and chemical stability for a period of >7 d. Crosslinked alginate‐gel with tunable thickness can retard the generation and release of toxic cations, thereby affording high biocompatibility. The soft alginate shells also enable to recover electric conductivity of EGaIn layers by “mechanical sintering” for applications in microcircuits, electric‐thermal actuators, and wearable sensors, offering huge potential for electronic tattoos, artificial limbs, electric skins, etc.     

Printed Solar Cells and Energy Storage Devices on Paper Substrates

Paper is a flexible material, commonly used for information storage, writing, packaging, or specialized purposes. It also has strong appeal as a substrate in the field of flexible printed electronics. Many applications, including safety, merchandising, smart labels/packing, and chemical/biomedical sensors, require an energy source to power operation. Here, progress regarding development of photovoltaic and energy storage devices on cellulosic substrates, where one or more of the main material layers are deposited via solution processing or printing, is reviewed. Paper can be used simply as the flexible substrate or, exploiting its porous fiber‐like nature, as an active film by infiltration or copreparation with electronic materials. Solar cells with efficiencies of up to 9% on opaque substrates and 13% on transparent substrates are demonstrated. Recent developments in paper‐based supercapacitors and batteries are also reviewed with maximum achieved capacity of 1350 mF cm^?2 and 2000 mAh g^?1, respectively. Analyzing the literature, it becomes apparent that more work needs to be carried out in continuing to improve peak performance, but especially stability and the application of printing techniques, even roll‐to‐roll processing, over large areas. Paper is not only environmentally friendly and recyclable, but also thin, flexible, lightweight, biocompatible, and inexpensive.     

Highly Stretchable,Global, and Distributed Local Strain Sensing Line Using GaInSn Electrodes for Wearable Electronics

For identifying human or finger movement, it is necessary to sense subtle movements at multiple points, including the local strain and global deformation simultaneously; however, this has not yet been realized. Therefore, a highly stretchable, global, and distributed local strain sensing electrode made of GaInSn and polydimethylsiloxane is developed for wearable devices. To investigate the electrical properties of multiple sections of the GaInSn electrode when stretching, tensile, cyclic, and three‐point‐bending tests are performed. The results demonstrate that the electrode can withstand a strain up to 50% and has little hysteresis without any delay. Moreover, the distributed local strain and global strain can be simultaneously measured using just a single electrode line. Finally, a prototype of a data glove as an application of the strain sensing line is manufactured, and it is demonstrated that the folding state of fingers could be identified. The proposed technology may allow the creation of a lightweight master hand manipulator or 3D data entry device.     

Novel Eco‐Friendly Starch Paper for Use in Flexible,Transparent, and Disposable Organic Electronics

An eco‐friendly biodegradable starch paper is introduced for use in next‐generation disposable organic electronics without the need for a planarizing layer. The starch papers are formed by starch gelatinization using a very small amount of 0.5 wt% polyvinyl alcohol (PVA), a polymer that bound to the starch, and 5 wt% of a crosslinker that bound to the PVA to improve mechanical properties. This process minimizes the additions of synthetic materials. The resultant starch paper provides a remarkable mechanical strength and stability under repeated movements. Robustness tests using various chemical solvents are conducted by immersing the starch paper for 6 h. Excellent nonpolar solvent stabilities are observed. They are important for the manufacture of organic electronics that use nonpolar solution processes. The applicability of the starch paper as a flexible substrate is tested by fabricating flexible organic transistors using pentacene, dinaphtho[2,3‐b:2′,3′‐f]thieno[3,2‐b]thiophene, and poly(dimethyl‐triarylamine) using both vacuum and solution processes. Electrically well‐behaved device performances are identified. Finally, the eco‐friendly biodegradability is verified by subjecting the starch paper to complete degradation by fungi in fishbowl water over 24 d. These developments illuminate new research areas in the field of biodegradable green electronics, enabling the development of extremely low‐cost electronics.     

Bio‐Inspired Stretchable,Adhesive, and Conductive Structural Color Film for Visually Flexible Electronics

The rapid progress in flexible electronic devices has attracted immense interest in many applications, such as health monitoring devices, sensory skins, and implantable apparatus. Here, inspired by the adhesion features of mussels and the color shift mechanism of chameleons, a novel stretchable, adhesive, and conductive structural color film is presented for visually flexible electronics. The film is generated by adding a conductive carbon nanotubes polydopamine (PDA) filler into an elastic polyurethane (PU) inverse opal scaffold. Owing to the brilliant flexibility and inverse opal structure of the PU layer, the film shows stable stretchability and brilliant structural color. Besides, the catechol groups on PDA impart the film with high tissue adhesiveness and self‐healing capability. Notably, because of its responsiveness, the resultant film is endowed with color‐changing ability that responds to motions, which can function as dual‐signal soft human‐motion sensors for real‐time color‐sensing and electrical signal monitoring. These features make the bio‐inspired hydrogel‐based electronics highly potential in the flexible electronics field.     

绿色电子制造及绿色电子封装材料

阐述了绿色电子制造(包括电子封装)概念起源、定义以及基本内涵和范畴,并从电子封装用互连材料、被连接材料和封装后清洗过程这三个方面全面阐述了绿色电子封装的主要内容,重点评述了目前绿色电子封装材料(包括无铅钎料、钎剂、焊膏和导电胶等)的研究现状和面临的问题.最后,展望了绿色电子制造及绿色电子封装材料的未来发展趋势.     

All-Printed Green Micro-Supercapacitors Based on a Natural-derived Ionic Liquid for Flexible Transient Electronics

The fabrication and characterization of green, flexible, and ultra-thin supercapacitors that are able to operate above 1.5 V is reported, using an all-printed fabrication process. The devices are produced by aqueous spray casting of a natural-derived electrolyte ionogel composed by 2-hydroxyethyl cellulose and by the ionic liquid choline lactate, while the electrodes are composed of highly porous nanostructured carbon films deposited by supersonic cluster beam deposition (SCBD). The obtained supercapacitors (device thickness < 10 μm) are stable to bending and they possess power values up to 120 kW kg^–1. The combination of aqueous spray casting and SCBD constitutes a versatile, scalable, and eco-friendly fabrication process able to directly print interconnected elements suitable for transient electronic systems.     

Liquid Metal‐Based Transient Circuits for Flexible and Recyclable Electronics

Transient electronics, arising electronic devices with dissolvable or degradable features on demand, is still at an early stage of development due to the limited choices of materials and strategies. Herein, a facile fabrication method for transient circuits by the combination of room‐temperature liquid metals (RTLMs) as the electronic circuit and water‐soluble poly(vinyl alcohol) (PVA) as the packaging material is reported. The as‐made transient circuits exhibit remarkable durability and stable electric performance upon bending and twisting, while possessing short transience times, owing to the excellent solubility of PVA substrates and the intrinsic flexibility of RTLM patterns. Moreover, the RTLM‐based transient circuit shows an extremely high recycling efficiency, up to 96% of the employed RTLM can be recovered. As such, the economic and environmental viability of transient electronics increases substantially. To validate this concept, the surface patterning of RTLMs with complicated shapes is demonstrated, and a transient antenna is subsequently applied for passive near‐field communication tag and a transient capacitive touch sensor. The application of the RTLM‐based transient circuit for sequentially turning off an array of light‐emitting‐diode lamps is also demonstrated. The present RTLM‐based PVA‐encapsulated circuits substantially expand the scope of transient electronics toward flexible and recyclable transient systems.     

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.     

Calcium‐Modified Silk as a Biocompatible and Strong Adhesive for Epidermal Electronics

With the increasing interest and demand for epidermal electronics, a strong interface between a sensor and a biological surface is essential, yet achieving such interface is still a challenge. Here, a calcium (Ca)‐modified biocompatible silk fibroin as a strong adhesive for epidermal electronics is proposed and the physical principles behind its interfacial and adhesive properties are reported. A strong adhesive characteristic (>800 N m^?1) is observed because of the increase in both viscoelastic property and mechanical interlocking through the incorporation of Ca ions. Furthermore, additional key characteristics of the Ca‐modified silk: reusability, stretchability, biocompatibility, and conductivity, are reported. These characteristics enable a wide range of applications as demonstrated in four epidermal electronic systems: capacitive touch sensor, resistive strain sensor, hydrogel‐based drug delivery, and electrocardiogram monitoring sensor. As a reusable, biocompatible, conductive, and strong adhesive with water‐degradability, the Ca‐modified silk adhesive is a promising candidate for the next‐generation adhesive for epidermal biomedical sensors.     

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.     

Experimental and Theoretical Studies of Serpentine Microstructures Bonded To Prestrained Elastomers for Stretchable Electronics

Stretchable electronic devices that exploit inorganic materials are attractive due to their combination of high performance with mechanical deformability, particularly for applications in biomedical devices that require intimate integration with human body. Several mechanics and materials schemes have been devised for this type of technology, many of which exploit deformable interconnects. When such interconnects are fully bonded to the substrate and/or encapsulated in a solid material, useful but modest levels of deformation (<30–40%) are possible, with reversible and repeatable mechanics. Here, the use of prestrain in the substrate is introduced, together with interconnects in narrow, serpentine shapes, to yield significantly enhanced (more than two times) stretchability, to more than 100%. Fracture and cyclic fatigue testing on structures formed with and without prestrain quantitatively demonstrate the possible enhancements. Finite element analyses (FEA) illustrates the effects of various material and geometric parameters. A drastic decrease in the elastic stretchability is observed with increasing metal thickness, due to changes in the buckling mode, that is, from local wrinkling at small thicknesses to absence of such wrinkling at large thicknesses, as revealed by experiment. An analytic model quantitatively predicts the wavelength of this wrinkling, and explains the thickness dependence of the buckling behaviors.     

2D Nanomaterial Arrays for Electronics and Optoelectronics

Two‐dimensional (2D) materials, benefitting from their unique planar structure and various appealing electronic properties, have attracted much attention for novel electronic and optoelectronic applications. As a basis for practical devices, the study of micro/nano‐2D material arrays based on coupling effects and synergistic effects is critical to the functionalization and integration of 2D materials. Moreover, micro/nano‐2D material arrays are compatible with traditional complementary metal oxide semiconductor (CMOS) electronics, catering well to high‐integration, high‐sensitivity, and low‐cost sensing and imaging systems. This review presents some recent studies on 2D material arrays in sequence from their novel preparations to high‐integration applications as well as explorations on dimension tuning. A first focus is on various typical fabrication methods for 2D material arrays, including photolithography, 2D printing, seeded growth, van der Waals epitaxial growth, and self‐assembly. Then, the applications of 2D material arrays, such as field effect transistors, photodetectors, pressure sensors, as well as flexible electronic devices of photodetectors and strain sensors, are elaborately introduced. Furthermore, the recent burgeoning exploration of mixed‐dimensional heterostructure arrays including 0D/2D, 1D/2D, and 3D/2D is discussed. Ultimately, conclusions and an outlook based on the current developments in this promising field are presented.