All‐Carbon‐Electrode‐Based Endurable Flexible Perovskite Solar Cells

Endured, low‐cost, and high‐performance flexible perovskite solar cells (PSCs) featuring lightweight and mechanical flexibility have attracted tremendous attention for portable power source applications. However, flexible PSCs typically use expensive and fragile indium–tin oxide as transparent anode and high‐vacuum processed noble metal as cathode, resulting in dramatic performance degradation after continuous bending or thermal stress. Here, all‐carbon‐electrode‐based flexible PSCs are fabricated employing graphene as transparent anode and carbon nanotubes as cathode. All‐carbon‐electrode‐based flexible devices with and without spiro‐OMeTAD (2,2′,7,7′‐tetrakis‐(N,N‐di‐p‐methoxyphenylamine)‐9,9′‐spirobifluorene) hole conductor achieve power conversion efficiencies (PCEs) of 11.9% and 8.4%, respectively. The flexible carbon‐electrode‐based solar cells demonstrate superior robustness against mechanical deformation in comparison with their counterparts fabricated on flexible indium–tin oxide substrates. Moreover, all carbon‐electrode‐based flexible PSCs also show significantly enhanced stability compared to the flexible devices with gold and silver cathodes under continuous light soaking or 60 °C thermal stress in air, retaining over 90% of their original PCEs after 1000 h. The promising durability and stability highlight that flexible PSCs are fully compatible with carbon materials and pave the way toward the realization of rollable and low‐cost flexible perovskite photovoltaic devices.     

Rational Design of Nanostructured Electrode Materials toward Multifunctional Supercapacitors

As an intermediate step during energy usage, supercapacitors with superior power density, long‐term cycling stability, and moderate energy density have attracted immense interest as a facile route to use energy in a clean, efficient, and versatile manner in smart grid applications, as well as portable devices and other applications. Currently, the major drawback of supercapacitors is the low energy density. Electrode materials are the key components determining the cell performance. Great research efforts are made to develop nanostructured electrode materials with high performance. On the other hand, integrating supercapacitors with other applications have led to the emergence of many new types of multifunctional supercapacitors, which are attractive for a myriad of applications. The current understanding on charge/discharge mechanisms of electric double layer capacitors and pseudo‐capacitors is discussed along with recent development in designing nanostructured electrode materials by structure/morphology engineering, doping, and crystal structure controlling. Achievements in multifunctional supercapacitors like flexible supercapacitors, all‐solid‐state supercapacitors, self‐healing supercapacitors, electrochromic supercapacitors, self‐chargeable supercapacitors, and supercapacitors integrated with sensors are illustrated. Finally, opportunities and challenges in developing high performance and multifunctional supercapacitors are proposed.     

Flexible All‐Solid‐State Supercapacitors of High Areal Capacitance Enabled by Porous Graphite Foams with Diverging Microtubes

The practical applications of wearable electronics rely on the successful development of flexible and integrable energy devices with small footprints. This work reports a completely new type of graphite foam made of strategically created superstructures with covalently attached diverging microtubes, and their applications as electrode supports for binder‐free and additive‐free flexible supercapacitors. Because of the enhanced volumetric surface areas compared to conventional graphite foams, a high loading of pseudocapacitive materials (Mn₃O₄, 3.91 mg cm^?2, 78 wt%) is achieved. The supercapacitors provide areal capacitances as high as 820 mF cm^?2 at 1 mV s^?1, while still maintaining high rate capability and 88% retention of capacitance after 3000 continuous charging and discharging cycles. When assembled as all‐solid‐state flexible symmetric supercapacitors, they offer one of the highest full‐cell capacitances (191 mF cm^?2) among similar manganese oxide/graphene foams, and retain 80% capacitance after 1000 mechanical cycles. The potential of such flexible supercapacitors is also manifested by directly powering electric nanomotors that can trace along letters “U” and T,” which is the first demonstration of flexible supercapacitors for wireless/portable nanomanipulation systems. This work could inspire a new paradigm in designing and creating 3D porous micro/nanosuperstructures for an array of self‐powered electronic and nanomechanical applications.     

Recent Developments of Planar Micro‐Supercapacitors: Fabrication,Properties, and Applications

The increasing development of wearable, portable, implantable, and highly integrated electronic devices has led to an increasing demand for miniaturization of energy storage devices. In recent years, supercapacitors, as an energy storage device, have received enormous attention owing to their excellent properties of quick charge and discharge, high power density, and long life cycle with minimal maintenance. Micro‐supercapacitors (MSCs) as a promising candidate for miniaturized energy storage components have undergone considerable theoretical and experimental investigations. Particularly, planar MSCs with a 2D architecture design have more attractive application prospects due to their flexible design and excellent electrochemical performance. However, the major drawbacks of MSCs are their intrinsically low energy density. For this reason, researchers have conducted much investigation to improve their energy density in order to promote their practical application. Herein, the recent development and progress of planar MSCs from the scope of the substrates, electrode materials, fabrication methods, electrochemical properties, and applications are discussed. Finally, the currently existing challenges and developments associated with planar MSCs are also discussed. All in all, planar MSCs have great application potential in various fields of electrochemical energy storage, self‐powered wireless sensors, and stimuli‐responsive and photoresponsive, alternating current line filtering.     

Highly Conductive Ordered Mesoporous Carbon Based Electrodes Decorated by 3D Graphene and 1D Silver Nanowire for Flexible Supercapacitor

Ordered mesoporous carbon (OMC) is considered one of the most promising materials for electric double layer capacitors (EDLC) given its low‐cost, high specific surface area, and easily accessed ordered pore channels. However, pristine OMC electrode suffers from poor electrical conductivity and mechanical flexibility, whose specific capacitance and cycling stability is unsatisfactory in flexible devices. In this work, OMC is coated on the surface of highly conductive three‐dimensional graphene foam, serving as both charge collector and flexible substrate. Upon further decoration with silver nanowires (Ag NWs), the novel architecture of Ag NWs/3D‐graphene foam/OMC (Ag‐GF‐OMC) exhibits exceptional electrical conductivity (up to 762 S cm^?1) and mechanical robustness. The Ag‐GF‐OMC electrodes in flexible supercapacitors reach a specific capacitance as high as 213 F g^?1, a value five‐fold higher than that of the pristine OMC electrode. Moreover, these flexible electrodes also exhibit excellent long‐term stability with >90% capacitance retention over 10 000 cycles, as well as high energy and power density (4.5 Wh kg^?1 and 5040 W kg^?1, respectively). This study provides a new procedure to enhance the device performance of OMC based supercapacitors, which is a promising candidate for the application of flexible energy storage devices.     

Self‐Powered Electronics by Integration of Flexible Solid‐State Graphene‐Based Supercapacitors with High Performance Perovskite Hybrid Solar Cells

To develop high‐capacitance flexible solid‐state supercapacitors and explore its application in self‐powered electronics is one of ongoing research topics. In this study, self‐stacked solvated graphene (SSG) films are reported that have been prepared by a facile vacuum filtration method as the free‐standing electrode for flexible solid‐state supercapacitors. The highly hydrated SSG films have low mass loading, high flexibility, and high electrical conductivity. The flexible solid‐state supercapacitors based on SSG films exhibit excellent capacitive characteristics with a high gravimetric specific capacitance of 245 F g^?1 and good cycling stability of 10 000 cycles. Furthermore, the flexible solid‐state supercapacitors are integrated with high performance perovskite hybrid solar cells (pero‐HSCs) to build self‐powered electronics. It is found that the solid‐state supercapacitors can be charged by pero‐HSCs and discharged from 0.75 V. These results demonstrate that the self‐powered electronics by integration of the flexible solid‐state supercapacitors with pero‐HSCs have great potential applications in storage of solar energy and in flexible electronics, such as portable and wearable personal devices.     

Advances on Emerging Materials for Flexible Supercapacitors: Current Trends and Beyond

The progressive size reduction of electronic components is experiencing bottlenecks in shrinking charge storage devices like batteries and supercapacitors, limiting their development into wearable and flexible zero‐pollution technologies. The inherent long cycle life, rapid charge–discharge patterns, and power density of supercapacitors rank them superior over other energy storage devices. In the modern market of zero‐pollution energy devices, currently the lightweight formula and shape adaptability are trending to meet the current requirement of wearables. Carbon nanomaterials have the potential to meet this demand, as they are the core of active electrode materials for supercapacitors and texturally tailored to demonstrate flexible and stretchable properties. With this perspective, the latest progress in novel materials from conventional carbons to recently developed and emerging nanomaterials toward lightweight stretchable active compounds for flexi‐wearable supercapacitors is presented. In addition, the limitations and challenges in realizing wearable energy storage systems and integrating the future of nanomaterials for efficient wearable technology are provided. Moreover, future perspectives on economically viable materials for wearables are also discussed, which could motivate researchers to pursue fabrication of cheap and efficient flexible nanomaterials for energy storage and pave the way for enabling a wide‐range of material‐based applications.     

Large-Area Flexible Organic Solar Cells with a Robust Silver Nanowire-Polymer Composite as Transparent Top Electrode

Upscaling of efficient flexible organic solar cells (OSCs) is still a challenging task, where flexible transparent electrode is a key limiting factor. Silver nanowires (AgNWs) are widely used as flexible transparent electrodes to fabricate efficient small-area flexible OSCs, but the high surface roughness of AgNWs electrodes causes large leakage current and performance deterioration in large-area OSCs. In this study, it is reported that a strategy of switching the bottom AgNWs electrode and the top Ag film electrode to avoid the detrimental effect of the high surface roughness of AgNWs electrodes. Mechanical robustness of the AgNWs has been enhanced by introducing a cross-linked poly(sodium 4-styrenesulfonate) layer. The AgNWs-polymer transparent film is fabricated by water transfer printing as the top electrode. 21 cm² flexible organic modules containing 10 sub-cells are fabricated and delivered power conversion efficiencies of 12.3% with the design of switched electrodes.     

Flexible Solid‐State Supercapacitors with Enhanced Performance from Hierarchically Graphene Nanocomposite Electrodes and Ionic Liquid Incorporated Gel Polymer Electrolyte

High energy density, durability, and flexibility of supercapacitors are required urgently for the next generation of wearable and portable electronic devices. Herein, a novel strategy is introduced to boost the energy density of flexible soild‐state supercapacitors via rational design of hierarchically graphene nanocomposite (GNC) electrode material and employing an ionic liquid gel polymer electrolyte. The hierarchical graphene nanocomposite consisting of graphene and polyaniline‐derived carbon is synthesized as an electrode material via a scalable process. The meso/microporous graphene nanocomposites exhibit a high specific capacitance of 176 F g^?1 at 0.5 A g^?1 in the ionic liquid 1‐ethyl‐3‐methylimidazolium tetrafluoroborate (EMIBF₄) with a wide voltage window of 3.5 V, good rate capability of 80.7% in the range of 0.5–10 A g^?1 and excellent stability over 10 000 cycles, which is attributed to the superior conductivity (7246 S m^?1), and quite large specific surface area (2416 m² g^?1) as well as hierarchical meso/micropores distribution of the electrode materials. Furthermore, flexible solid‐state supercapacitor devices based on the GNC electrodes and gel polymer electrolyte film are assembled, which offer high specific capacitance of 180 F g^?1 at 1 A g^?1, large energy density of 75 Wh Kg^?1, and remarkable flexible performance under consecutive bending conditions.     

Non-Monotonic Capacitance Change of Layered Ti3C2Tx MXene Film Structures under Increasing Compressive Stress

The progress in advanced electronic devices has imposed a great demand for developing flexible electrochemical power devices, which requires a comprehensive understanding of the mechanical–electrochemical coupling behavior of various energy storage materials. Unlike a monotonic capacitance increase of carbon-based double-layer supercapacitors, MXene-based flexible supercapacitors demonstrate a non-monotonic, i.e., “increase-then-decrease” capacitance behavior under the pressure range of 8488 kPa. This non-monotonic capacitance response to pressure is intrinsic to the MXene film as its charge storage is primarily determined by the surface activity, which can be readily affected by pressure-induced dissociation of functionalities, as well as the charge transporting kinetics as limited by the inherent layered structure. The findings described in this study not only expand the knowledge of mechanical–electrochemical coupling to layered MXenes under pressure, but also give a vital design guideline for flexible/stretchable MXene-based energy storage devices or other electronics.     

Ultralight and Binder‐Free All‐Solid‐State Flexible Supercapacitors for Powering Wearable Strain Sensors

Flexible energy storage devices play a pivotal role in realizing the full potential of flexible electronics. This work presents high‐performance, all‐solid‐state, flexible supercapacitors by employing an innovative multilevel porous graphite foam (MPG). MPGs exhibit superior properties, such as large specific surface area, high electric conductivity, low mass density, high loading efficiency of pseudocapacitive materials, and controlled corrugations for accommodating mechanical strains. When loaded with pseudocapacitive manganese oxide (Mn₃O₄), the MPG/Mn₃O₄ (MPGM) composites achieve a specific capacitance of 538 F g^?1 (1 mV s^?1) and 260 F g^?1 (1 mV s^?1) based on the mass of pure Mn₃O₄ and entire electrode composite, respectively. Both are among the best of Mn₃O₄‐based supercapacitors. The MPGM is mechanically robust and can go through 1000 mechanical bending cycles with only 1.5% change in electric resistance. When integrated as all‐solid‐state symmetric supercapacitors, they offer a full cell specific capacitance as high as 53 F g^?1 based on the entire electrode and retain 80% of capacitance after 1000 continuous mechanical bending cycles. Furthermore, the all‐solid‐state flexible supercapacitors are incorporated with strain sensors into self‐powered flexible devices for detection of both coarse and fine motions on human skins, i.e., those from finger bending and heart beating.     

Low‐Resistant Electrical and Robust Mechanical Contacts of Self‐Attachable Flexible Transparent Electrodes with Patternable Circuits

Flexible, transparent, conductive electrodes are key elements of emerging flexible electronic and energy devices. Such electrodes should form an intimate physical contact with various active components of flexible devices to ensure stable, low‐resistant electrical contacts. However, contact formation techniques are based largely on conventional soldering, conductive pastes, mechanical clamping, and thin film deposition. These generally result in damaged, contaminated, bulky, and uncontrollable contact interfaces. A self‐attachable, flexible, transparent, and conductive electrode that is based on a distinctive design of regular grid patterns into which bioinspired adhesive architectures and percolating Ag nanowires are integrated is proposed. Based on this integrated design, the proposed electrode forms reliable, low‐resistant electrical contacts; strong mechanical adhesive contacts; and ultra‐clean, damage‐free contact interfaces with active device components by attaching onto the components without using additional conductive pastes, mechanical pressing, or vacuum deposition processes. The contact interfaces of the electrode and device components remain stable even when the electrode is extremely bent. Moreover, specific electronic circuits can be generated on the electrode surface by a selective deposition of Ag nanowires. This enables simple interconnections of diverse electronic components on its surface.     

Enhancing the Capacitive Storage Performance of Carbon Fiber Textile by Surface and Structural Modulation for Advanced Flexible Asymmetric Supercapacitors

The exploration of high‐energy anodes with good mechanical properties is highly attractive for flexible asymmetric supercapacitors (ASCs) but challenging. Owing to the excellent conductivity and superior mechanical flexibility, carbon fiber textile (CFT) holds great promise as a substrate/current‐collector for fabricating flexible electrodes. Yet, it is rarely used as a flexible active electrode in terms of its low electrochemical reactivity and small accessible area. In this work, an effective surface and structural modulation strategy is developed to directly tune CFT into a highly active anode for flexible ASCs by creating hierarchical pores and numerous pseudocapacitive oxygenic groups. Arising from large surface and increased active sites, the as‐prepared activated porous CFT (APCFT) electrode not only achieves a large capacitance (1.2 F cm^?2 at 4 mA cm^?2) and fast kinetics but also shows satisfying cycling durability (no capacitance decay after 25 000 cycles). More importantly, an advanced flexible ASC device with an impressive energy density of 4.70 mWh cm^?3 is successfully assembled by employing this APCFT as an anode, outperforming most recently reported ASC devices. This dual modification strategy may throw light on the rational design of new generation advanced carbon electrodes for high‐performance flexible supercapacitors.     

Spatially resolved photocurrent mapping of efficient organic solar cells fabricated on a woven mesh electrode

Flexible organic photovoltaic devices may soon find applications in various fields, such as portable electronics or building‐integrated photovoltaics, occupying market niches that are currently not covered by the prevailing photovoltaic technology based on silicon and other inorganic materials. For these applications, there is an urgent need to replace the commonly used indium tin oxide by transparent and electrically conductive materials that can be processed cost‐effectively by large‐area compatible printing and coating processes. Here, we fabricated P3HT/PCBM organic solar cells with a power conversion efficiency of 3.1% on a flexible, transparent and conductive woven fabric electrode. The electrode is produced by a roll‐to‐roll process and consists of a polymer‐embedded fibre/metal wire grid. Metal wires protrude as little as 5 µm from the electrode plane, providing electrical contact points on a smooth surface suitable for thin film deposition. The use of spatially resolved photocurrent mapping experiments showed a high level of detailed information, with the unexpected indication that there probably exists a maximum in the cell performance versus mesh size opening and that woven fabric electrodes with largest geometrical open area do not necessarily perform better. Copyright © 2012 John Wiley & Sons, Ltd.     

Current Technology of Supercapacitors: A Review

A supercapacitor is a solid-state device that can store electrical energy in the form of charges. It represents an advancement in the field of energy storage, as it overcomes many of the shortcomings of batteries. This paper presents an overview of the various types of supercapacitors, electrode materials, and electrolytes, and the future of supercapacitors. Due to their high storage capacity, supercapacitors are commonly used in portable electronic devices such as MP3 players and mobile phones, and in hybrid vehicles and other applications. In electrical and hybrid vehicles, supercapacitors are increasingly used as provisional energy storage for regenerative braking. Various materials are used in electrodes to boost the performance of the supercapacitor. This review presents details regarding the materials and electrolyte, and the improvements in the field of supercapacitors.     

Sustainable 3D Structural Binder for High-Performance Supercapacitor by Biosynthesis Process

Flexible supercapacitors represent an attractive technology for the next generation of wearable consumer electronics as power sources but usually suffer from relatively low energy density. It is highly desired to construct high-performance electrodes for the practical applications of supercapacitors. Here, inspired by the natural structure of the spider web, an elaborate design of binder is reported through a biosynthesis process to construct flexible electrodes with both excellent mechanical properties and electrochemical performance. Through this strategy, a spider-web-inspired 3D structural binder enables large ion-accessible surface area and high packing density of active electrode material as well as efficient ion transport pathways. As a result, a high areal capacitance of 4.62 F cm^-2 and a high areal energy density of 0.18 mW h cm^-2 is achieved in the composite electrodes and symmetric supercapacitors, respectively, demonstrating a promising potential to construct flexible energy storage devices for diverse practical applications.     

Additive Functionalization and Embroidery for Manufacturing Wearable and Washable Textile Supercapacitors

Electronic textiles require rechargeable power sources that are highly integrated with textiles and garments, thereby providing outstanding durability and washability. In contrast, present power sources fabricated using conventional ex situ strategies are difficult to integrate with clothing and can degrade during garment washing. Here, a new manufacturing strategy named additive functionalization and embroidery manufacturing (AFEM) is reported, which enables textile‐based supercapacitors (TSCs) to be directly fabricated on woven, knitted, and nonwoven fabrics. The additive principle of AFEM allows developing TSCs with different types of electrode materials, device architectures, pattern designs, and array connections. High‐machine‐speed, programmable‐design industrial embroidering equipment is used to fabricate TSCs with high areal energy storage and power capabilities, which are retained during many cycles of severe mechanical deformation and industrial laundering with waterproof encapsulation.     

Rational Design of Electrode Materials for Advanced Supercapacitors: From Lab Research to Commercialization

Supercapacitors can harvest electrical energy from intermittent sources and transfer it quickly, but their specific energy must be raised if they are applied to efficiently power wearable and flexible electronics, as well as larger equipment. However, the remaining big gap between the lab research and practical applications seriously hinders the further progress of advanced supercapacitors, especially for electrode materials. Consequently, from a commercial/usable perspective, a clear guideline from lab research to commercialization is highly desired for bringing advanced supercapacitors from basic research into reality. This review focuses on the key factors of advanced supercapacitors from lab research to commercialization and summarizes recent progress in the field of supercapacitors as well as outlines key perspectives for future research. First, the several energy storage mechanisms are illustrated for building better supercapacitors. Then, the up-to-date key achievements and progresses of smart methods toward high-energy supercapacitors and effective strategies for commercial-level mass-loading as well as high packing density electrodes are summarized and commented upon. Also, integrated systems of supercapacitors and application fields of commercial supercapacitors are also highlighted. Subsequently, future research directions are presented here to guide research toward the commercialization of advanced supercapacitors.     

Solid‐State Hybrid Fibrous Supercapacitors Produced by Dead‐End Tube Membrane Ultrafiltration

The development of flexible supercapacitors with high volumetric performance is critically important for portable electronics applications, which are severely volume limited. Here, dead‐end tube membrane (DETM) ultrafiltration is used to produce densely compacted carbon‐nanotube/graphene fibrous films as solid‐state supercapacitor electrodes. DETM is widely used in the water purification industry, but to date its use has not been explored for making supercapacitor electrode materials. Compared with vacuum‐assisted filtration, dead‐end filtration of the mixture through a porous membrane is carried out under much higher pressure, and thus the solvent can be gotten rid of much faster, with less energy consumption and in an environmentally friendly manner. More importantly, phase separation of the solid constituents in the mixture, due to concentration increase, can be suppressed in DETM. Therefore, highly uniform and densely compacted supercapacitor electrodes can be obtained with very high volumetric energy and power density. The volumetric energy density in this work (≈2.7 mWh cm^‐3) is at a higher level than all the all‐solid‐state fibrous supercapacitors reported to date. This can be attributed to the DETM process used, which produces a densely compacted network structure without compromising the availability of electrochemically active surface area.     

Wearable Force Touch Sensor Array Using a Flexible and Transparent Electrode

Transparent electrodes have been widely used for various electronics and optoelectronics, including flexible ones. Many nanomaterial‐based electrodes, in particular 1D and 2D nanomaterials, have been proposed as next‐generation transparent and flexible electrodes. However, their transparency, conductivity, large‐area uniformity, and sometimes cost are not yet sufficient to replace indium tin oxide (ITO). Furthermore, the conventional ITO is quite rigid and susceptible to mechanical fractures under deformations (e.g., bending, folding). In this study, the authors report new advances in the design, fabrication, and integration of wearable and transparent force touch (touch and pressure) sensors by exploiting the previous efforts in stretchable electronics as well as novel ideas in the transparent and flexible electrode. The optical and mechanical experiment, along with simulation results, exhibit the excellent transparency, conductivity, uniformity, and flexibility of the proposed epoxy‐copper‐ITO (ECI) multilayer electrode. By using this multi‐layered ECI electrode, the authors present a wearable and transparent force touch sensor array, which is multiplexed by Si nanomembrane p‐i‐n junction‐type (PIN) diodes and integrated on the skin‐mounted quantum dot light‐emitting diodes. This novel integrated system is successfully applied as a wearable human–machine interface (HMI) to control a drone wirelessly. These advances in novel material structures and system‐level integration strategies create new opportunities in wearable smart displays.