Printable Fabrication of Nanocoral‐Structured Electrodes for High‐Performance Flexible and Planar Supercapacitor with Artistic Design

Planar supercapacitors with high flexibility, desirable operation safety, and high performance are considered as attractive candidates to serve as energy‐storage devices for portable and wearable electronics. Here, a scalable and printable technique is adopted to construct novel and unique hierarchical nanocoral structures as the interdigitated electrodes on flexible substrates. The as‐fabricated flexible all‐solid‐state planar supercapacitors with nanocoral structures achieve areal capacitance up to 52.9 mF cm^?2, which is 2.5 times that of devices without nanocoral structures, and this figure‐of‐merit is among the highest in the literature for the same category of devices. More interestingly, due to utilization of the inkjet‐printing technique, excellent versatility on electrode‐pattern artistic design is achieved. Particularly, working supercapacitors with artistically designed patterns are demonstrated. Meanwhile, the high scalability of such a printable method is also demonstrated by fabrication of large‐sized artistic supercapacitors serving as energy‐storage devices in a wearable self‐powered system as a proof of concept.     

Recent Advances in Fiber Supercapacitors: Materials,Device Configurations,and Applications

Fiber supercapacitors (SCs), with their small size and weight, excellent flexibility and deformability, and high capacitance and power density, are recognized as one of the most robust power supplies available for wearable electronics. They can be woven into breathable textiles or integrated into different functional materials to fit curved surfaces for use in day-to-day life. A comprehensive review on recent important development and progress in fiber SCs is provided, with respect to the active electrode materials, device configurations, functions, integrations. Active electrode materials based on different electrochemical mechanisms and intended to improve performance including carbon-based materials, metal oxides, and hybrid composites, are first summarized. The three main types of fiber SCs, namely parallel, twist, and coaxial structures, are then discussed, followed by the exploration of some functions including stretchability and self-healing. Miniaturized integration of fiber SCs to obtain flexible energy fibers and integrated sensing systems is also discussed. Finally, a short conclusion is made, combining with comments on the current challenges and potential solutions in this field.     

Layered Transition Metal Dichalcogenide-Based Nanomaterials for Electrochemical Energy Storage

The rapid development of electrochemical energy storage (EES) systems requires novel electrode materials with high performance. A typical 2D nanomaterial, layered transition metal dichalcogenides (TMDs) are regarded as promising materials used for EES systems due to their large specific surface areas and layer structures benefiting fast ion transport. The typical methods for the preparation of TMDs and TMD-based nanohybrids are first summarized. Then, in order to improve the electrochemical performance of various kinds of rechargeable batteries, such as lithium-ion batteries, lithium–sulfur batteries, sodium-ion batteries, and other types of emerging batteries, the strategies for the design and fabrication of layered TMD-based electrode materials are discussed. Furthermore, the applications of layered TMD-based nanomaterials in supercapacitors, especially in untraditional supercapacitors, are presented. Finally, the existing challenges and promising future research directions in this field are proposed.     

Flexible/Stretchable Supercapacitors with Novel Functionality for Wearable Electronics

With the miniaturization of personal wearable electronics, considerable effort has been expended to develop high-performance flexible/stretchable energy storage devices for powering integrated active devices. Supercapacitors can fulfill this role owing to their simple structures, high power density, and cyclic stability. Moreover, a high electrochemical performance can be achieved with flexible/stretchable supercapacitors, whose applications can be expanded through the introduction of additional novel functionalities. Here, recent advances in and future prospects for flexible/stretchable supercapacitors with innate functionalities are covered, including biodegradability, self-healing, shape memory, energy harvesting, and electrochromic and temperature tolerance, which can contribute to reducing e-waste, ensuring device integrity and performance, enabling device self-charging following exposure to surrounding stimuli, displaying the charge status, and maintaining the performance under a wide range of temperatures. Finally, the challenges and perspectives of high-performance all-in-one wearable systems with integrated functional supercapacitors for future practical application are discussed.     

Printable Fabrication of a Fully Integrated and Self‐Powered Sensor System on Plastic Substrates

Wearable and portable devices with desirable flexibility, operational safety, and long cruising time, are in urgent demand for applications in wireless communications, multifunctional entertainments, personal healthcare monitoring, etc. Herein, a monolithically integrated self‐powered smart sensor system with printed interconnects, printed gas sensor for ethanol and acetone detection, and printable supercapacitors and embedded solar cells as energy sources, is successfully demonstrated in a wearable wristband fashion by utilizing inkjet printing as a proof‐of‐concept. In such a “wearable wristband”, the harvested solar energy can either directly drive the sensor and power up a light‐emitting diode as a warning signal, or can be stored in the supercapacitors in a standby mode, and the energy released from supercapacitors can compensate the intermittency of light illumination. To the best of our knowledge, the demonstration of such a self‐powered sensor system integrated onto a single piece of flexible substrate in a printable and additive manner has not previously been reported. Particularly, the printable supercapacitors deliver an areal capacitance of 12.9 mF cm^?2 and the printed SnO₂ gas sensor shows remarkable detection sensitivity under room temperature. The printable strategies for device fabrication and system integration developed here show great potency for scalable and facile fabrication of a variety of wearable devices.     

Overcoming the Trade-Off between Optical Transmittance and Areal Capacitance of Transparent Supercapacitors for Practical Application

It is substantially challenging for transition metal oxide nanoparticle (NP)-based electrodes for supercapacitors to achieve high transparency and large capacity simultaneously due to the inherent trade-off between optical transmittance (T) and areal capacitance (C_A). This study demonstrates how this trade-off limitation can be overcome by replacing some electrode NPs with transparent tin oxide (SnO₂) NPs. Although SnO₂ NPs are non-capacitive, they provide effective paths for charge transport, which simultaneously increase the C_A and T_550nm of the manganese oxide (Mn₃O₄) NP electrode from 11.7 to 13.4 mF cm⁻² and 82.1% to 87.4%, respectively, when 25 wt% of Mn₃O₄ are replaced by SnO₂. The obtained C_A values at a given T are higher than those of the transparent electrodes previously reported. An energy storage window fabricated using the mixed-NP electrodes exhibits the highest energy density among transparent supercapacitors previously reported. The improved energy density enables the window to operate various electronic devices for a considerable amount of time, demonstrating its applicability in constructing a reliable and space-efficient building-integrated power supply system.     

“Salting out” in Hofmeister Effect Enhancing Mechanical and Electrochemical Performance of Amide-based Hydrogel Electrolytes for Flexible Zinc-Ion Battery

With the development of flexible and wearable electronic devices, it is a new challenge for polymer hydrogel electrolytes to combine high mechanical flexibility and electrochemical performance into one membrane. In general, the high content of water in hydrogel electrolyte membranes always leads to poor mechanical strength, and limits their applications in flexible energy storage devices. In this work, based on the “salting out” phenomenon in Hofmeister effect, a kind of gelatin-based hydrogel electrolyte membrane is fabricated with high mechanical strength and ionic conductivity by soaking pre-gelated gelatin hydrogel in 2 m ZnSO₄ aqueous. Among various gelatin-based electrolyte membranes, the gelatin-ZnSO₄ electrolyte membrane delivers the “salting out” property of Hofmeister effect, which improves both the mechanical strength and electrochemical performance of gelatin-based electrolyte membranes. The breaking strength reaches 1.5 MPa. When applied to supercapacitors and zinc-ion batteries, it can sustain over 7500 and 9300 cycles for repeated charging and discharging processes. This study provides a very simple and universal method to prepare polymer hydrogel electrolytes with high strength, toughness, and stability, and its applications in flexible energy storage devices provide a new idea for the construction of secure and stable flexible and wearable electronic devices.     

Scalable Manufacturing of Environmentally Stable All-Solid-State Plant Protein-Based Supercapacitors with Optimal Balance of Capacitive Performance and Mechanically Robust

The development of advanced biomaterial with mechanically robust and high energy density is critical for flexible electronics, such as batteries and supercapacitors. Plant proteins are ideal candidates for making flexible electronics due to their renewable and eco-friendly natures. However, due to the weak intermolecular interactions and abundant hydrophilic groups of protein chains, the mechanical properties of protein-based materials, especially in bulk materials, are largely constrained, which hinders their performance in practical applications. Here, a green and scalable method is shown for the fabrication of advanced film biomaterials with high mechanical strength (36.3 MPa), toughness (21.25 MJ m⁻³), and extraordinary fatigue-resistance (213 000 times) by incorporating tailor-made core–double-shell structured nanoparticles. Subsequently, the film biomaterials combine to construct an ordered, dense bulk material by stacking-up and hot-pressing techniques. Surprisingly, the solid-state supercapacitor based on compacted bulk material shows an ultrahigh energy density of 25.8 Wh kg⁻¹, which is much higher than those previously reported advanced materials. Notably, the bulk material also demonstrates long-term cycling stability, which can be maintained under ambient condition or immersed in H₂SO₄ electrolyte for more than 120 days. Thus, this research improves the competitiveness of protein-based materials for real-world applications such as flexible electronics and solid-state supercapacitors.