Porous Conductive Textiles for Wearable Electronics.

Over the years, researchers have made significant strides in the development of novel flexible/stretchable and conductive materials, enabling the creation of cutting-edge electronic devices for wearable applications. Among these, porous conductive textiles (PCTs) have emerged as an ideal material platform for wearable electronics, owing to their light weight, flexibility, permeability, and wearing comfort. This Review aims to present a comprehensive overview of the progress and state of the art of utilizing PCTs for the design and fabrication of a wide variety of wearable electronic devices and their integrated wearable systems. To begin with, we elucidate how PCTs revolutionize the form factors of wearable electronics. We then discuss the preparation strategies of PCTs, in terms of the raw materials, fabrication processes, and key properties. Afterward, we provide detailed illustrations of how PCTs are used as basic building blocks to design and fabricate a wide variety of intrinsically flexible or stretchable devices, including sensors, actuators, therapeutic devices, energy-harvesting and storage devices, and displays. We further describe the techniques and strategies for wearable electronic systems either by hybridizing conventional off-the-shelf rigid electronic components with PCTs or by integrating multiple fibrous devices made of PCTs. Subsequently, we highlight some important wearable application scenarios in healthcare, sports and training, converging technologies, and professional specialists. At the end of the Review, we discuss the challenges and perspectives on future research directions and give overall conclusions. As the demand for more personalized and interconnected devices continues to grow, PCT-based wearables hold immense potential to redefine the landscape of wearable technology and reshape the way we live, work, and play.

Fully Printable and Reconfigurable Hufu-type Electroluminescent Devices for Visualized Encryption.

Hufu, serving as evidence of imperial authorization in ancient China, comprises two parts in the form of tiger-shaped tallies that only become effective when matched. Drawing inspiration from the concept of Hufu, a reconfigurable electroluminescent (EL) device is designed by separating conventional integral devices into two parts that contain the EL layer (part A) and the transparent electrode (part B), respectively. The key to realizing such strategy is employing an adhesive and stretchable polymer gel composite as the transparent electrodes for the EL devices. The polymer gel composite facilitates robust yet reversible contact between the EL layer and transparent electrode, enabling high-performance and stretchable EL devices that can be readily disassembled and reassembled: the EL devices can maintain ≈81% of their initial luminance after 1000 times of repeated disassembly and reassembly. Moreover, the precursor ink of the polymer gel composite is compatible with a wide variety of coating and printing technologies, such as spin-coating, inkjet printing, dispensing, and brush painting. Importantly, the reconfigurable feature of the devices opens up a new path to encryption display systems, and as a proof-of-concept, EL encrypted password, and content-changeable digital clock are demonstrated.

Rapid self-assembly of self-healable and transferable liquid metal epidermis.

Healable electronic skins, an essential component for future soft robotics, implantable bioelectronics, and smart wearable systems, necessitate self-healable and pliable materials that exhibit functionality at intricate interfaces. Although a plethora of self-healable materials have been developed, the fabrication of highly conformal biocompatible functional materials on complex biological surfaces remains a formidable challenge. Inspired by regenerative properties of skin, we present the self-assembled transfer-printable liquid metal epidermis (SALME), which possesses autonomous self-healing capabilities at the oil-water interface. SALME comprises a layer of surfactant-grafted liquid metal nanodroplets that spontaneously assemble at the oil-water interface within a few seconds. This unique self-assembly property facilitates rapid restoration (<10 s) of SALME following mechanical damage. In addition to its self-healing ability, SALME exhibits excellent shear resistance and can be seamlessly transferred to arbitrary hydrophilic/hydrophobic curved surfaces. The transferred SALME effectively preserves submicron-scale surface textures on biological substrates, thus displaying tremendous potential for future epidermal bioelectronics.

Wet-Adaptive Electronic Skin.

Skin electronics provides remarkable opportunities for non-invasive and long-term monitoring of a wide variety of biophysical and physiological signals that are closely related to health, medicine, and human-machine interactions. Nevertheless, conventional skin electronics fabricated on elastic thin films are difficult to adapt to the wet microenvironments of the skin: Elastic thin films are non-permeable, which block the skin perspiration; Elastic thin films are difficult to adhere to wet skin; Most skin electronics are difficult to work underwater. Here, a Wet-Adaptive Electronic Skin (WADE-skin) is reported, which consists of a next-to-skin wet-adhesive fibrous layer, a next-to-air waterproof fibrous layer, and a stretchable and permeable liquid metal electrode layer. While the electronic functionality is determined by the electrode design, this WADE-skin simultaneously offers superb stretchability, wet adhesion, permeability, biocompatibility, and waterproof property. The WADE-skin can rapidly adhere to human skin after contact for a few seconds and stably maintain the adhesion over weeks even under wet conditions, without showing any negative effect to the skin health. The use of WADE-skin is demonstrated for the stable recording of electrocardiogram during intensive sweating as well as underwater activities, and as the strain sensor for the underwater operation of virtual reality-mediated human-machine interactions.

Stretchable and Self-Healable Fiber-Shaped Conductors Suitable for Harsh Environments.

Fiber-shaped conductors with high electrical conductivity, stretchability, and durability have attracted increasing attention due to their potential for integration into arbitrary wearable forms. However, these fiber conductors still suffer from low reliability and short life span, particularly in harsh environments. Herein, a conductive, environment-tolerant, stretchable, and healable fiber conductor (CESH), which consists of a self-healable and stretchable organohydrogel fiber core, a conductive and buckled silver nanowire coating, and a self-healable and waterproof protective sheath, is reported. Such a multilayer core-sheath design not only offers high stretchability (≈2400%), high electrical conductivity (1.0 × 106 S m-1 ), outstanding self-healing ability and durability, but also possesses unprecedented tolerance in harsh environments including wide working temperature (-60-20 °C), arid (≈10 % RH (RH: room humidity)), and underwater conditions. As proof-of-concept demonstrations, CESHs are integrated into various wearable formats as interconnectors to steadily perform the electric function under different mechanical deformations and harsh conditions. Such a new type of multifunctional fiber conductors can bridge the gap in stretchable and self-healing fiber technologies by providing ultrastable electrical conductance and excellent environmental tolerance, which can greatly expand the range of applications for fiber conductors.

Elasto-Plastic Design of Ultrathin Interlayer for Enhancing Strain Tolerance of Flexible Electronics.

The ability to tolerate large strains during various degrees of deformation is a core issue in the development of flexible electronics. Commonly used strategies nowadays to enhance the strain tolerance of thin film devices focus on the optimization of the device architecture and the increase of bonding at the materials interface. In this paper, we propose a strategy, namely elasto-plastic design of an ultrathin interlayer, to boost the strain tolerance of flexible electronics. We demonstrate that insertion of an ultrathin, stiff (high Young's modulus) and elastic (high yield strain) interlayer between an upper rigid film/device and a soft substrate, regardless of the substrate thickness or the interfacial bonding, can significantly reduce the actual strain applied on the film/device when the substrate is bent. Being independent of existing strategies, the elasto-plastic design strategy offers an effective method to enhance the device flexibility without redesigning the device structure or altering the material interface.

Destructive-Treatment-Free Rapid Polymer-Assisted Metal Deposition for Versatile Electronic Textiles.

Highly conductive, durable, and breathable metal-coated textiles are critical building block materials for future wearable electronics. In order to enhance the metal adhesion on the textile surface, existing solution-based approaches to preparing these materials require time-consuming presynthesis and/or premodification processes, typically in the order of tens of minutes to hours, on textiles prior to metal plating. Herein, we report a UV-induced rapid polymer-assisted metal deposition (r-PAMD) that offers a destructive-treatment-free process to deposit highly conductive metals on a wide variety of textile materials, including cotton, polyester, nylon, Kevlar, glass fiber, and carbon cloth. In comparison to the state of the arts, r-PAMD significantly shortens the modification time to several minutes and is compatible with the roll-to-roll fabrication manner. Moreover, the deposited metals show outstanding adhesion, which withstands rigorous flexing, abrasion, and machine washing tests. We demonstrate that these metal-coated textiles are suitable for applications in two vastly different fields, being wearable and washable sensors, and lithium batteries.

Controllable Heterogenous Seeding-Induced Crystallization for High-Efficiency FAPbI3 -Based Perovskite Solar Cells Over 24.

The addition of small seeding particles into a supersaturated solution is one among the most effective approaches to obtain high-quality semiconductor materials via increased crystallization rates. However, limited study is conducted on this approach for the fabrication of perovskite solar cells. Here, a new strategy-"heterogenous seeding-induced crystallization (hetero-SiC)" to assist the growth of FAPbI3 -based perovskite is proposed. In this work, di-tert-butyl(methyl)phosphonium tetrafluoroborate is directly introduced into the precursor, which forms a low-solubility complex with PbI2 . The low-solubility complex can serve as the seed to induce crystallization of the perovskite during the solvent-evaporation process. Various in situ measurement tools are used to visualize the hetero-SiC process, which is shown to be an effective way of manipulating the nucleation and crystal growth of perovskites. The hetero-SiC process greatly improves the film quality, reduces film defects, and suppresses nonradiative recombination. A hetero-SIC proof-of-concept device exhibits outstanding performance with 24.0% power conversion efficiency (PCE), well over the control device with 22.2% PCE. Additionally, hetero-SiC perovskite solar cell (PSC) stability under light illumination is enhanced and the PSC retains 84% of its initial performance after 1400 h of light illumination.

Sensitive, High-Speed, and Broadband Perovskite Photodetectors with Built-In TiO2 Metalenses.

Monolithic integration of nanostructured metalenses with broadband light transmission and good charge transport can simultaneously enhance the sensitivity, speed, and efficiency of photodetectors. The realization of built-in broadband metalenses in perovskite photodetectors, however, has been largely challenged by the limited choice of materials and the difficulty in nanofabrication. Here a new type of broadband-transmitting built-in TiO2 metalens (meta-TiO2 ) is devised, which is readily fabricated by one-step and lithograph-free glancing angle deposition. The meta-TiO2 , which comprises of sub-100 nm TiO2 nanopillars randomly spaced with a wide range of sub-wavelength distances in 5-200 nm, shows high transmittance of light in the wavelength range of 400-800 nm. The meta-TiO2 also serves as an efficient electron transporting layer to prevent the exciton recombination and facilitate the photoinduced electron extraction and transport. Replacing the conventional mesoporous TiO2 with the meta-TiO2 comprehensively leads to enhancing the detection speed by three orders of magnitude to a few hundred nanoseconds, improving the responsivity and detectivity by one order of magnitude to 0.5 A W-1 and 1013 Jones, respectively, and extending the linear dynamic range by 50% to 120 dB.

Polymer-Assisted Metallization of Mammalian Cells.

Developing biotemplating techniques to translate microorganisms and cultured mammalian cells into metallic biocomposites is of great interest for biosensors, electronics, and energy. The metallization of viruses and microbial cells is successfully demonstrated via a genetic engineering strategy or electroless deposition. However, it is difficult to transform mammalian cells into metallic biocomposites because of the complicated genes and the delicate morphological features. Herein, "polymer-assisted cell metallization" (PACM) is reported as a general method for the transformation of mammalian cells into metallic biocomposites. PACM includes a first step of in situ polymerization of functional polymer on the surface and in the interior of the mammalian cells, and a subsequent electroless deposition of metal to convert the polymer-functionalized cells into metallic biocomposites, which retain the micro- and nanostructures of the mammalian cells. This new biotemplating method is compatible with different cell types and metals to yield a wide variety of metallic biocomposites with controlled structures and properties.

Multifunctional Crosslinking-Enabled Strain-Regulating Crystallization for Stable, Efficient α-FAPbI3 -Based Perovskite Solar Cells.

α-Formamidinium lead triiodide (α-FAPbI3 ) represents the state-of-the-art for perovskite solar cells (PSCs) but experiences intrinsic thermally induced tensile strain due to a higher phase-converting temperature, which is a critical instability factor. An in situ crosslinking-enabled strain-regulating crystallization (CSRC) method with trimethylolpropane triacrylate (TMTA) is introduced to precisely regulate the top section of perovskite film where the largest lattice distortion occurs. In CSRC, crosslinking provides in situ perovskite thermal-expansion confinement and strain regulation during the annealing crystallization process, which is proven to be much more effective than the conventional strain-compensation (post-treatment) method. Moreover, CSRC with TMTA successfully achieves multifunctionality simultaneously: the regulation of tensile strain, perovskite defects passivation with an enhanced open-circuit voltage (VOC  = 50 mV), and enlarged perovskite grain size. The CSRC approach gives significantly enhanced power conversion efficiency (PCE) of 22.39% in α-FAPbI3 -based PSC versus 20.29% in the control case. More importantly, the control PSCs' instability factor-residual tensile strain-is regulated into compression strain in the CSRC perovskite film through TMTA crosslinking, resulting in not only the best PCE but also outstanding device stability in both long-term storage (over 4000 h with 95% of initial PCE) and light soaking (1248 h with 80% of initial PCE) conditions.

Bottom-Up Quasi-Epitaxial Growth of Hybrid Perovskite from Solution Process-Achieving High-Efficiency Solar Cells via Template​-Guided Crystallization.

Epitaxial growth gives the highest-quality crystalline semiconductor thin films for optoelectronic devices. Here, a universal solution-processed bottom-up quasi-epitaxial growth of highly oriented α-formamidinium lead triiodide (α-FAPbI3 ) perovskite film via a two-step method is reported, in which the crystal orientation of α-FAPbI3 film is precisely controlled through the synergetic effect of methylammonium chloride and the large-organic cation butylammonium bromide. In situ GIWAXS visualizes the BA-related intermediate phase formation at the bottom of film, which serves as a guiding template for the bottom-up quasi-epitaxial growth in the subsequent annealing process. The template-guided epitaxially grown BAFAMA perovskite film exhibits increased crystallinity, preferred crystallographic orientation, and reduced defects. Moreover, the BAFAMA perovskite solar cells demonstrate decent stability, maintaining 95% of their initial power conversion efficiency after 2600 h ambient storage, and 4-time operation condition lifetime enhancement.

Efficient Flexible Perovskite Solar Cells Using Low-Cost Cu Top and Bottom Electrodes.

Perovskite solar cells (PSCs) are promising technology for flexible photovoltaic applications because of the low cost and good flexibility of the halide perovskite materials. Nevertheless, the use of transparent conductive oxides (TCOs) and noble metals (e.g., Au and Ag) as PSC electrodes is very costly, and TCOs are too brittle for flexible applications. How to fabricate flexible PSCs (FPSCs) with cost-effective and soft electrode materials remains to be a big challenge. Herein, we report the first study of FPSCs using low-cost Cu electrodes. Both the transparent bottom electrode and the opaque top electrode are fabricated with Cu. FPSCs made with such Cu electrodes acquire a champion efficiency of 13.58% (Jsc of 17.79 mA cm-2, Voc of 1.031 V, and FF of 74.07%), which retains over 90% after 1000 cycles of bending at a small radius of curvature of 5 mm. The device shows negligible changes in Voc and FF after storage for 10 weeks without encapsulation.

Solution-Processed Transparent Electrodes for Emerging Thin-Film Solar Cells.

Solution-processed solar cells are appealing because of the low manufacturing cost, the good compatibility with flexible substrates, and the ease of large-scale fabrication. Whereas solution-processable active materials have been widely adopted for the fabrication of organic, dye-sensitized, and perovskite solar cells, vacuum-deposited transparent conducting oxides (TCOs) such as indium tin oxide, fluorine-doped tin oxide, and aluminum-doped tin oxide are still the most frequently used transparent electrodes (TEs) for solar cells. These TCOs not only significantly increase the manufacturing cost of the device, but also are too brittle for future flexible and wearable applications. Therefore, developing solution-processed TEs for solar cells is of great interest. This paper provides a detailed discussion on the recent development of solution-processed TEs, including the chemical synthesis of the electrode materials, the solution-based technologies for the electrode fabrication, the optical and electrical properties of the solution-processed TEs, and their applications on solar cells.

Polymer-Assisted Metal Deposition (PAMD) for Flexible and Wearable Electronics: Principle, Materials, Printing, and Devices.

The rapid development of flexible and wearable electronics favors low-cost, solution-processing, and high-throughput techniques for fabricating metal contacts, interconnects, and electrodes on flexible substrates of different natures. Conventional top-down printing strategies with metal-nanoparticle-formulated inks based on the thermal sintering mechanism often suffer from overheating, rough film surface, low adhesion, and poor metal quality, which are not desirable for most flexible electronic applications. In recent years, a bottom-up strategy termed as polymer-assisted metal deposition (PAMD) shows great promise in addressing the abovementioned challenges. Here, a detailed review of the development of PAMD in the past decade is provided, covering the fundamental chemical mechanism, the preparation of various soft and conductive metallic materials, the compatibility to different printing technologies, and the applications for a wide variety of flexible and wearable electronic devices. Finally, the attributes of PAMD in comparison with conventional nanoparticle strategies are summarized and future technological and application potentials are elaborated.

Scanning Nanowelding Lithography for Rewritable One-Step Patterning of Sub-50 nm High-Aspect-Ratio Metal Nanostructures.

The development of a new nanolithographic strategy, named scanning nanowelding lithography (SNWL), for the one-step fabrication of arbitrary high-aspect-ratio nanostructures of metal is reported in this study. Different from conventional pattern transfer and additive printing strategies which require subtraction or addition of materials, SNWL makes use of a sharp scanning tip to reshape metal thin films or existing nanostructures into desirable high-aspect-ratio patterns, through a cold-welding effect of metal at the nanoscale. As a consequence, SNWL can easily fabricate, in one step and at ambient conditions, sub-50 nm metal nanowalls with remarkable aspect ratio >5, which are found to be strong waveguide of light. More importantly, SNWL outweighs the existing strategies in terms of the unique ability to erase the as-made nanostructures and rewrite them into other shapes and orientations on-demand. Taking advantages of the serial and rewriting capabilities of SNWL, the smart information storage-erasure of Morse codes is demonstrated. SNWL is a promising method to construct arbitrary high-aspect-ratio nanostructure arrays that are highly desirable for biological, medical, optical, electronic, and information applications.

Chemical formation of soft metal electrodes for flexible and wearable electronics.

Flexible and wearable electronics is one major technology after smartphones. It shows remarkable application potential in displays and informatics, robotics, sports, energy harvesting and storage, and medicine. As an indispensable part and the cornerstone of these devices, soft metal electrodes (SMEs) are of great significance. Compared with conventional physical processes such as vacuum thermal deposition and sputtering, chemical approaches for preparing SMEs show significant advantages in terms of scalability, low-cost, and compatibility with the soft materials and substrates used for the devices. This review article provides a detailed overview on how to chemically fabricate SMEs, including the material preparation, fabrication technologies, methods to characterize their key properties, and representative studies on different wearable applications.

Photoreactive and Metal-Platable Copolymer Inks for High-Throughput, Room-Temperature Printing of Flexible Metal Electrodes for Thin-Film Electronics.

Photoreactive and metal-platable copolymer inks are reported for the first time to allow high-throughput printing of high-performance flexible electrodes at room temperature. This new copolymer ink accommodates various types of printing technologies, such as soft lithography molding, screen printing, and inkjet printing. Electronic devices including resistors, sensors, solar cells, and thin-film transistors fabricated with these printed electrodes show excellent electrical performance and mechanical flexibility.

Bio-Inspired Chemical Fabrication of Stretchable Transparent Electrodes.

Stretchable and transparent electrodes are fabricated by chemical deposition of metal thin films on natural veins of leaves at ambient conditions. These vein-based transparent electrodes show excellent electro-optical property (0.9 Ω sq(-1) at 83% T) even at 50% tensile strains, ideal for flexible and stretchable optoelectronic devices.

Full-solution processed flexible organic solar cells using low-cost printable copper electrodes.

Full-solution-processed flexible organic solar cells (OSCs) are fabricated using low-cost and high-quality printable Cu electrodes, which achieve a power conversion efficiency as high as 2.77% and show remarkable stability upon 1000 bending cycles. This device performance is thought to be the best among all full-solution-processed OSCs reported in the literature using the same active materials. This printed Cu electrode is promising for application in roll-to-roll fabrication of flexible OSCs.