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A supercapacitor is a potential electrochemical energy storage device with high‐power density (PD) for driving flexible, smart, electronic devices. In particular, flexible supercapacitors (FSCs) have reliable mechanical and electrochemical properties and have become an important part of wearable, smart, electronic devices. It is noteworthy that the flexible electrode, electrolyte, separator and current collector all play key roles in overall FSCs. In this review, the unique mechanical properties, structural designs and fabrication methods of each flexible component are systematically classified, summarized and discussed based on the recent progress of FSCs. Further, the practical applications of FSCs are delineated, and the opportunities and challenges of FSCs in wearable technologies are proposed. The development of high‐performance FSCs will greatly promote electricity storage toward more practical and widely varying fields. However, with the development of portable equipment, simple FSCs cannot satisfy the needs of integrated and intelligent flexible wearable devices for long durations. It is anticipated that the combining an FSC and a flexible power source such as flexible solar cells is an effective strategy to solve this problem. This review also includes some discussions of flexible self‐powered devices. In this review, the unique mechanical properties, structural designs, and fabrication methods of each flexible component are systematically classified, summarized, and discussed based on the recent progress of flexible supercapacitors (FSCs). Further, the practical applications of FSCs are delineated, and the opportunities and challenges of FSCs in wearable technologies are proposed.

Ion doping is an effective strategy for achieving high‐performance flexible Cu2ZnSn(S,Se)4 (CZTSSe) solar cells by defect regulations. Here, a Li&Na co‐doped strategy is applied to synergistically regulate defects in CZTSSe bulks. The quality absorbers with the uniformly distributed Li and Na elements are obtained using the solution method, where the acetates (LiAc and NaAc) are as additives. The concentration of the harmful CuZn anti‐site defects is decreased by 8.13% after Li incorporation, and that of the benign NaZn defects is increased by 36.91% after Na incorporation. Synergistic Li&Na co‐doping enhances the carrier concentration and reduces the interfacial defects concentration by one order of magnitude. As a result, the flexible CZTSSe solar cell achieves a power conversion efficiency (PCE) of 10.53% with certified 10.12%. Because of the high PCE and the homogeneous property, the Li&Na co‐doped device is fabricated to a large area (2.38 cm2) and obtains 9.41% PCE. The co‐doping investigation to synergistically regulate defects provides a new perspective for efficient flexible CZTSSe solar cells. The Li&Na co‐doped strategy is applied to synergistically regulate defects in CZTSSe bulks using the cheap and non‐toxic LiAc and NaAc as additives. The synergistic co‐doping effectively passivates harmful defects and increases shallow‐level defects. The flexible CZTSSe device achieves 10.53% efficiency (certified 10.12%) in the area (0.21 cm2) and 9.41% efficiency in large area (2.38 cm2).

A self-folding method that can fold a thick (~10 μm) metal layer with a large curvature (>1 mm−1) and is resistant to repetitive folding deformation is proposed. Given the successful usage of hinged origami/kirigami structures forms in deployable structures, they show strong potential for application in stretchable electronic devices. There are, however, two key difficulties in applying origami/kirigami methods to stretchable electronic devices. The first is that a thick metal layer used as the conductive layer of electronic devices is too hard for self-folding as it is. Secondly, a thick metal layer breaks on repetitive folding deformation at a large curvature. To overcome these difficulties, this paper proposes a self-folding method using hinges on a thick metal layer by applying a meander structure. Such a structure can be folded at a large curvature even by weak driving forces (such as those produced by self-folding) and has mechanical resistance to repetitive folding deformation due to the local torsional deformation of the meander structure. To verify the method, the large curvature self-folding of thick metal layers and their mechanical resistance to repetitive folding deformation is experimentally demonstrated. In addition, an origami/kirigami hybrid stretchable electronic device with light-emitting diodes (LEDs) is fabricated using a double-tiling structure called the perforated extruded Miura-ori.

Recently, some studies have addressed the use of a folded substrate to realize stretchable electronic devices including stretchable thermoelectric generators (TEGs). However, the utilization of the folded substrate as a heat radiation fin has not been achieved. Herein, we have proposed the construction of a TEG with an origami-like folded structure substrate called an “origami-fin” that can achieve a high heat radiation performance and is also highly stretchable. The origami-fin increases the stretchability of the TEG by bending a non-stretchable material into a folded shape, and it also works as a heat radiator because of its large surface area compared to that of a flat structure. We evaluated the heat radiation performance of the origami-fin and the stability of the performance when it was stretched. The results demonstrate that the origami-fin works as a heat radiator and enhances the output of the TEG, while also exhibiting a high stretchability with only a slight output reduction.

Multiferroic materials with flexibility are expected to make great contributions to flexible electronic applications, such as sensors, memories, and wearable devices. In this work, super‐flexible freestanding BiMnO3 membranes with simultaneous ferroelectricity and ferromagnetism are synthesized using water‐soluble Sr3Al2O6 as the sacrificial buffer layer. The super‐flexibility of BiMnO3 membranes is demonstrated by undergoing an ≈180° folding during an in situ bending test, which is consistent with the results of first‐principles calculations. The piezoelectric signal under a bending radius of ≈500 µm confirms the stable existence of electric polarization in freestanding BiMnO3 membranes. Moreover, the stable ferromagnetism of freestanding BiMnO3 membranes is demonstrated after 100 times bending cycles with a bending radius of ≈2 mm. 5.1% uniaxial tensile strain is achieved in freestanding BiMnO3 membranes, and the piezoresponse force microscopy (PFM) phase retention behaviors confirm that the ferroelectricity of membranes can survive stably up to the strain of 1.7%. These super‐flexible membranes with stable ferroelectricity and ferromagnetism pave ways to the realizations of multifunctional flexible electronics. As flexible device have become vital in the forefront of technology, the maintenance of multifunctional performances under high flexion is highly desired. Here, the synthesis of super‐flexible freestanding BiMnO3 membranes with stable ferroelectricity and ferromagnetism simultaneously by pulsed laser deposition using recently promising water‐soluble Sr3Al2O6 as the sacrificial layer is reported.

The flexibility of thermoelectric generators (TEGs) is important for low-contact thermal resistance to curved heat sources. However, approaches that depend on soft materials, which are used in most existing studies, have the problem of low performance in terms of the substrate’s thermal conductivity and the thermoelectric conversion efficiency of the thermoelectric (TE) elements. In this study, we propose a method to fabricate “Origami-TEG”, a TEG with an origami structure that enables both flexibility and the usage of high-performance rigid materials by self-folding. By applying the principle of the linkage mechanism to self-folding, we realized a fabrication process in which the TE element-mounting process and the active-material-addition process were separated in time. The fabricated origami-TEG showed similar internal resistance and maximum output power when attached to heat sources with flat and curved surfaces. Furthermore, it exhibited high-performance stability against both stretching and bending deformations.

We propose a paper solar cell based on carbon nanotube (CNT)-composite papers. To fabricate this cell, we use dye-sensitized solar cells (DSCs) for generating power through the redox reaction of dyes in conjunction with CNT-composite papers, which are composite materials containing CNTs and pulp (raw paper material) that can be fabricated easily by using a method based on the Japanese washi papermaking technique. The demand for CNT applications is expected to increase due to their high conductivity and metallic or semiconducting characteristics. This CNT-composite paper can also have metallic or semiconducting characteristics based on the contained CNTs in the composite paper. We previously fabricated a DSC that generates electricity by using CNT-composite papers stacked in a typical DSC structure. However, the conversion efficiency of this DSC was just 0.188%, which is not practical. To overcome this low power generation issue, we tried improving the DSC structure by applying electrodes to the CNT-composite papers in grid patterns for efficient current collection and applying an optimally mixed dye for efficient electron excitation. Results showed that the conversion efficiency improved to 0.58%. Moreover, we demonstrated that using a mixed dye can improve the conversion efficiency of the paper DSC. We expect these types of CNT-composite papers to be used as material for new DSCs.

Tactile displays have been extensively studied for several decades. However, owing to their bulkiness and stiffness, it has been difficult to integrate these displays with information devices to enable tactile communication between the devices and their users. This paper proposes a novel sheet-type electrovibration tactile display that consists of poly(3,4-ethylenedioxythiophene) polystyrene sulfonate conductive layers and an insulation layer of polydimethylsiloxane. The tactile display is sufficiently thin and flexible for attaching onto various surfaces. In this study, the tactile display was micro-fabricated and characterized through experiments. The experimental results indicated that the tactile display exhibited good durability under bending and that it could present various tactile sensations depending on the type of voltage waveform. In addition, the effect of using a combination of electrovibration and thermal stimuli was also demonstrated. The sheet-type display was attached onto a Peltier element; the thinness of the structure enabled the display to conform to the element and ensure good heat transfer. In the experiment, subjects were asked to scan the display with their fingertips. The results showed that multiple tactile stimuli were also successfully perceived by the subjects.

HighlightsThe MXene-boosted rapid gelling expedites the assembly of flexible thermocell arrays, overcoming the typical constraint of complicated device fabrication processes.The hydrogel electrolyte can sustain stable thermoelectrochemical performance under various challenging conditions, including large, repeated, and sustained deformations, and multiple cut-healing cycles.The as-assembled thermocell array exhibits device-level self-healing capability and high adaptability to human body, efficiently harvesting low-grade heat for wearable applications.The evolution of wearable technology has prompted the need for adaptive, self-healable, and energy-autonomous energy devices. This study innovatively addresses this challenge by introducing an MXene-boosted hydrogel electrolyte, which expedites the assembly process of flexible thermocell (TEC) arrays and thus circumvents the complicated fabrication of typical wearable electronics. Our findings underscore the hydrogel electrolyte's superior thermoelectrochemical performance under substantial deformations and repeated self-healing cycles. The resulting hydrogel-based TEC yields a maximum power output of 1032.1 nW under the ΔT of 20 K when being stretched to 500% for 1000 cycles, corresponding to 80% of its initial state; meanwhile, it sustains 1179.1 nW under the ΔT of 20 K even after 60 cut-healing cycles, approximately 92% of its initial state. The as-assembled TEC array exhibits device-level self-healing capability and high adaptability to human body. It is readily applied for touch-based encrypted communication where distinct voltage signals can be converted into alphabet letters; it is also employed as a self-powered sensor to in-situ monitor a variety of body motions for complex human actions. The swift assembly approach, combined with the versatile functionality of the TEC device, paves the way for future advancements in wearable electronics targeting at fitness monitoring and human–machine interfaces.

Polyvinyl alcohol (PVA)-based hydrogels have attracted significant attention due to their excellent biocompatibility, tunable mechanical properties, and ability to form stable three-dimensional networks. This comprehensive review explores the recent advancements in PVA-based hydrogels, focusing on their unique properties, fabrication strategies, and multifunctional applications. Firstly, it discusses various facile synthesis techniques, including freeze/thaw cycles, chemical cross-linking, and enhancement strategies, which have led to enhanced mechanical strength, elasticity, and responsiveness to external stimuli. These improvements have expanded the applicability of PVA-based hydrogels in critical areas such as biomedical, environmental treatment, flexible electronics, civil engineering, as well as other emerging applications. Additionally, the integration of smart functionalities, such as self-healing capabilities and multi-responsiveness, is also examined. Despite progress, challenges remain, including optimizing mechanical stability under varying conditions and addressing potential toxicity of chemical cross-linkers. The review concludes by outlining future perspectives, emphasizing the potential of PVA-based hydrogels in emerging fields like regenerative medicine, environmental sustainability, and advanced manufacturing. It underscores the importance of interdisciplinary collaboration in realizing the full potential of these versatile materials to address pressing societal challenges.