Flexible Lead‐Free Perovskite Oxide Multilayer Film Capacitor Based on (Na0.8K0.2)0.5Bi0.5TiO3/Ba0.5Sr0.5(Ti0.97Mn0.03)O3 for High‐Performance Dielectric Energy Storage

Flexible thin film dielectric capacitors with high energy storage density and a fast charging–discharging rate have attracted increasing attention as the development of microelectronics progresses toward flexibility and miniaturization. In this work, an all‐inorganic thin film dielectric capacitor with a multilayer structure based on (Na_0.8K_0.2)_0.5Bi_0.5TiO₃ and Ba_0.5Sr_0.5(Ti_0.97Mn_0.03)O₃ is designed and synthesized on a mica substrate. By optimizing the periodic number (N), concomitantly enhanced breakdown strength and large polarization difference are achieved in the film with N = 6, which contributes to the large energy density (W_rec) of 91 J cm^?3, high efficiency (η) of 68%, and fast discharging rate of 47.6 µs. The obtained energy density is the highest value up to now in flexible dielectric capacitors, including lead‐free and lead‐based inorganic films as well as organic dielectric films. Moreover, no obvious deterioration of the energy storage performance is observed in the wide ranges of working temperature (?50–200 °C), operating frequency (500 Hz to 30 kHz), and fatigue cycles (1–10⁸). Besides, the W_rec and η are ultra‐stable under various bending radii (R = 12–2 mm) and even after 10⁴ bending cycles at R = 4 mm, demonstrating an outstanding mechanical bending endurance. This excellent performance will allow the capacitor thrive in flexible microenergy storage systems.     

Self‐Supported Tin Sulfide Porous Films for Flexible Aluminum‐Ion Batteries

High‐performance flexible batteries are promising energy storage devices for portable and wearable electronics. Currently, the major obstacle to develop flexible batteries is the shortage of flexible electrodes with excellent electrochemical performance. Another challenge is the limited progress in the flexible batteries beyond Li‐ion because of a safety concern for the Li‐based electrochemical system. In this work, a self‐supported tin sulfide (SnS) porous film (PF) is fabricated as a flexible cathode material in an Al‐ion battery, which delivers a high specific capacity of 406 mAh g^?1. A capacity decay rate of 0.03% per cycle is achieved, indicating a good stability. The self‐supported and flexible SnS film also shows an outstanding electrochemical performance and stability during dynamic and static bending tests. In situ transmission electron microscopy demonstrates that the porous structure of SnS is beneficial for minimizing the volume expansion during charge/discharge. This leads to an improved structural stability and superior long‐term cyclability.     

An Efficient Ultra‐Flexible Photo‐Charging System Integrating Organic Photovoltaics and Supercapacitors

Flexible and biocompatible integrated photo‐charging devices consisting of photovoltaic cells and energy storage units can provide an independent power supply for next‐generation wearable electronics or biomedical devices. However, current flexible integrated devices exhibit low total energy conversion and storage efficiency and large device thickness, hindering their applicability towards efficient and stable self‐powered systems. Here, a highly efficient and ultra‐thin photo‐charging device with a total efficiency approaching 6% and a thickness below 50 µm is reported, prepared by integrating 3‐µm‐thick organic photovoltaics on 40 µm‐thick carbon nanotube/polymer‐based supercapacitors. This flexible photo‐charging capacitor delivers much higher performance compared with previous reports by tuning the electrochemical properties of the composite electrodes, which reduce the device thickness to 1/8 while improving the total efficiency by 15%. The devices also exhibit a superior operational stability (over 96% efficiency retention after 100 charge/discharge cycles for one week) and mechanical robustness (94.66% efficiency retention after 5000 times bending at a radius of around 2 mm), providing a high‐power and long‐term operational energy source for flexible and wearable electronics.     

Ultrafast All‐Solid‐State Coaxial Asymmetric Fiber Supercapacitors with a High Volumetric Energy Density

Fiber‐supercapacitors (FSCs) are promising energy storage devices that can complement or even replace microbatteries in miniaturized portable and wearable electronics. Currently, a major challenge for FSCs is achieving ultrahigh volumetric energy and power densities simultaneously, especially when the charge/discharge rates exceed 1 V s^?1. Herein, an Au‐nanoparticle‐doped‐MnO_x@CoNi‐alloy@carbon‐nanotube (Au–MnO_x@CoNi@CNT) core/shell nanocomposite fiber electrode is designed, aiming to boost its charge/discharge rate by taking advantage of the superconductive CoNi alloy network and the greatly enhanced conductivity of the Au doped MnO_x active materials. An all‐solid‐state coaxial asymmetric FSC (CAFSC) prototype device made by wrapping this fiber with a holey graphene paper (HGP) exhibits excellent performance at rates up to 10 V s^?1, which is the highest charge rate demonstrated so far for FSCs based on pseudocapacitive materials. Furthermore, our fully packaged CAFSC delivers a volumetric energy density of ≈15.1 mW h cm^?3, while simultaneously maintaining a high power density of 7.28 W cm^?3 as well as a long cycle life (90% retention after 10 000 cycles). This value is the highest among all reported FSCs, even better than that of a typical 4 V/500 µA h thin‐film lithium battery.     

Alkaline Polymer Membrane‐Based Ultrathin,Flexible, and High‐Performance Solid‐State Zn‐Air Battery

The increasing demand for portable and wearable electronics requires lightweight, thin, and highly flexible power sources, for example, flexible zinc‐air batteries (ZABs). The so‐far reported flexible ZAB devices mostly remain bulky, with a design consisting of two relatively thick substrates (e.g., carbon cloths and/or metal foams) and a gel electrolyte‐coated separator in between. Herein, an ultrathin (≈0.2 mm) solid‐state ZAB with high flexibility and performance is introduced by directly forming self‐standing active layers on each surface of an alkaline polymer membrane through an ink‐casting/hot‐pressing approach. A Fe/N‐doped 3D carbon with hierarchic pores and an interconnected network structure is used as cathode electrocatalyst, so that the backing gas‐diffusion layer (e.g., carbon cloth) can be abandoned. What is further, a microstructure‐modulating method to significantly increase the FeN₄ active sites for oxygen reduction reaction is developed, thus significantly boosting the performance of the ZAB. The assembled solid‐state ZAB manifests remarkable peak power density of 250 mW cm^?3 and high capacity of 150.4 mAh cm^?3 at 8.3 mA cm^?3, as well as excellent flexibility. The new design should provide valuable opportunity to the portable and wearable electronics.     

Yolk–Shell NiS2 Nanoparticle‐Embedded Carbon Fibers for Flexible Fiber‐Shaped Sodium Battery

Fiber‐shaped rechargeable batteries hold promise as the next‐generation energy storage devices for wearable electronics. However, their application is severely hindered by the difficulty in fabrication of robust fiber‐like electrodes with promising electrochemical performance. Herein, yolk–shell NiS₂ nanoparticles embedded in porous carbon fibers (NiS₂?PCF) are successfully fabricated and developed as high‐performance fiber electrodes for sodium storage. Benefiting from the robust embedded structure, 3D porous and conductive carbon network, and yolk–shell NiS₂ nanoparticles, the as‐prepared NiS₂?PCF fiber electrode achieves a high reversible capacity of about 679 mA h g^?1 at 0.1 C, outstanding rate capability (245 mA h g^?1 at 10 C), and ultrastable cycle performance with 76% capacity retention over 5000 cycles at 5 C. Notably, a flexible fiber‐shaped sodium battery is assembled, and high reversible capacity is kept at different bending states. This work offers a new electrode‐design paradigm toward novel carbon fiber electrodes embedded with transition metal oxides/sulfides/phosphides for application in flexible energy storage devices.     

All‐Solid‐State Fiber Supercapacitors with Ultrahigh Volumetric Energy Density and Outstanding Flexibility

Fiber supercapacitors (FSCs) represent a promising class of energy storage devices that can complement or even replace microbatteries in miniaturized portable and wearable electronics. One of their main limitations, however, is the low volumetric energy density when compared with those of rechargeable batteries. Considering the energy density of FSC is proportional to CV² (E = 1/2 CV², where C is the capacitance and V is the operating voltage), one would explore high operating voltage as an effective strategy to promote the volumetric energy density. In the present work, an all‐solid‐state asymmetric FSC (AFSC) with a maximum operating voltage of 3.5 V is successfully achieved, by employing an ionic liquid (IL) incorporated gel‐polymer as the electrolyte (EMIMTFSI/PVDF‐HFP). The optimized AFSC is based on MnO_x@TiN nanowires@carbon nanotube (NWs@CNT) fiber as the positive electrode and C@TiN NWs@CNT fiber as the negative electrode, which gives rise to an ultrahigh stack volumetric energy density of 61.2 mW h cm^?3, being even comparable to those of commercially planar lead‐acid batteries (50–90 mW h cm^?3), and an excellent flexibility of 92.7% retention after 1000 blending cycles at 90°. The demonstration of employing the ILs‐based electrolyte opens up new opportunities to fabricate high‐performance flexible AFSC for future portable and wearable electronic devices.     

Aqueous Solution‐Processable Small Molecular Metal‐Chelate Complex Electrolyte for Flexible All‐Solid State Energy Storage Devices

A small molecular metal‐chelate complex, tris(8‐hydroxyquinoline‐5‐sulfonic acid) aluminum (AlQSA₃), that has three sulfonic acid groups per molecule leading to an excellent solubility in water is reported as a liquid‐free perfect solid‐state electrolyte for flexible film‐type all‐solid‐state energy storage devices. The AlQSA₃ material is synthesized by one‐step reaction of aluminum triisopropoxide and 8‐hydroxyquinoline‐5‐sulfonic acid. The aqueous solutions of AlQSA₃ are applied to fabricate flexible film‐type all‐solid state electric double layer capacitors with indium‐tin oxide thin film electrodes. The ion conductivity of the AlQSA₃ film reaches 0.116 mS cm^?1, while a pronounced hysteresis are obtained in the cyclic voltammetry measurement. The AlQSA₃ film capacitors exhibit an output voltage of 1.5 V at 20 μA cm^?2, which is considerably stable by the repeated operation. In particular, the peak output voltage is well kept even after 180° bending for 500 times in the case of the flexible AlQSA₃ film capacitors.     

Mn‐Rich P′2‐Na0.67[Ni0.1Fe0.1Mn0.8]O2 as High‐Energy‐Density and Long‐Life Cathode Material for Sodium‐Ion Batteries

Herein, P′2‐type Na_0.67[Ni_0.1Fe_0.1Mn_0.8]O₂ is introduced as a promising new cathode material for sodium‐ion batteries (SIBs) that exhibits remarkable structural stability during repetitive Na⁺ de/intercalation. The O? Ni? O? Mn? O? Fe? O bond in the octahedra of transition‐metal layers is used to suppress the elongation of the Mn? O bond and to improve the electrochemical activity, leading to the highly reversible Na storage mechanism. A high discharge capacity of ≈220 mAh g^?1 (≈605 Wh kg^?1) is delivered at 0.05 C (13 mAg^?1) with a high reversible capacity of ≈140 mAh g^?1 at 3 C and excellent capacity retention of 80% over 200 cycles. This performance is associated with the reversible P′2–OP4 phase transition and small volume change upon charge and discharge (≈3%). The nature of the sodium storage mechanism in a full cell paired with a hard carbon anode reveals an unexpectedly high energy density of ≈542 Wh kg^?1 at 0.2 C and good capacity retention of ≈81% for 500 cycles at 1 C (260 mAg^?1).     

Flexible and High‐Loading Lithium–Sulfur Batteries Enabled by Integrated Three‐In‐One Fibrous Membranes

Lithium–sulfur batteries are appealing as high‐energy storage systems and hold great application prospects in wearable and portable electronics. However, severe shuttle effects, low sulfur conductivity, and especially poor electrode mechanical flexibility restrict sulfur utilization and loading for practical applications. Herein, high‐flux, flexible, electrospun fibrous membranes are developed, which succeed in integrating three functional units (cathode, interlayer, and separator) into an efficient composite. This structure helps to eliminate negative interface effects, and effectively drives synergistic boosts to polysulfide confinement, electron transfer, and lithium‐ion diffusion. It delivers a high initial capacity of 1501 mA h g^?1 and a discharge capacity of 933 mA h g^?1 after 400 cycles, with slow capacity attenuation (0.069% per cycle). Even under high sulfur loading (13.2 mg cm^?2, electrolyte/sulfur ratio = 6 mL g^?1) or in an alternative folded state, this three‐in‐one membrane still exhibits high areal capacity (11.4 mA h cm^?2) and exceptional application performance (powering an array of over 30 light‐emitting diodes (LEDs)), highlighting its huge potential in high‐energy flexible devices.     

Highly‐Safe and Ultra‐Stable All‐Flexible Gel Polymer Lithium Ion Batteries Aiming for Scalable Applications

With the development of flexible electronics, flexible lithium ion batteries (LIBs) have received great attention. Previously, almost all reported flexible components had shortcomings related to poor mechanical flexibility, low energy density, and poor safety, which led to the failure of scalable applications. This study demonstrates a fully flexible lithium ion battery using LiCoO₂ as the cathode, Li₄Ti₅O₁₂ as the anode, and graphene film as the flexible current collector. The graphene oxide modified gel polymer electrolyte exhibits higher ionic conductivity than a conventional liquid electrolyte and improves the safety of the flexible battery. The optimum design of the flexible graphene battery exhibits super electrochemical performance, with a 2.3 V output voltage plateau and a satisfactory capacity of 143.0 mAh g^?1 at 1 C. The mass energy density and power density are both ≈1.4 times higher than a standard electrode using metal foils as current collectors. No capacity loss is observed after 100 thousand cycles of mechanical bending. More importantly, even in the clipping state, this flexible gel polymer battery can still demonstrate a stable and safe electrochemical performance. This work may lead to a promising strategy of high‐performance scalable LIBs for the next‐generation flexible electronics.     

All‐Manganese‐Based Binder‐Free Stretchable Lithium‐Ion Batteries

Advanced electrode materials with bendability and stretchability are critical for the rapid development of fully flexible/stretchable lithium‐ion batteries. However, the sufficiently stretchable lithium‐ion battery is still underdeveloped that is one of the biggest challenges preventing from realizing fully deformable power sources. Here, a low‐temperature hydrothermal synthesis of a cathode material for stretchable lithium‐ion battery is reported by the in situ growth of LiMn₂O₄ (LMO) nanocrystals inside 3D carbon nanotube (CNT) film networks. The LMO/CNT film composite has demonstrated the chemical bonding between the LMO active materials and CNT scaffolds, which is the most important characteristic of the stretchable electrodes. When coupled with a wrinkled MnO_x /CNT film anode, a binder‐free, all‐manganese‐based stretchable full battery cell is assembled which delivers a high average specific capacity of ≈97 mA h g^?1 and stabilizes after over 300 cycles with an enormous strain of 100%. Furthermore, combining with other merits such as low cost, natural abundance, and environmentally friendly, the all‐manganese design is expected to accelerate the practical applications of stretchable lithium‐ion batteries for fully flexible and biomedical electronics.     

Superior Energy‐Storage Capacitors with Simultaneously Giant Energy Density and Efficiency Using Nanodomain Engineered BiFeO3‐BaTiO3‐NaNbO3 Lead‐Free Bulk Ferroelectrics

Dielectric capacitors are receiving a great deal of attention for advanced pulsed power owing to their high power density and quick charge/discharge rate. However, the energy density is limited and the efficiency and the thermal stability are also not ideal, which has been a longstanding obstacle to developing desirable dielectric materials. These concerns have are addressed herein by fabricating nanodomain‐engineered BiFeO₃‐BaTiO₃‐NaNbO₃ bulk ferroelectrics, integrating a high‐spontaneous‐polarization gene, wide band gaps, and a heterogeneous nanodomain structure, generating record‐excellent comprehensive performance of giant energy‐storage density W_rec ≈8.12 J cm^?3, high efficiency η ≈90% and excellent thermal stability (±10%, ?50 to 250 °C) and ultrafast discharge rate (t_0.9 < 100 ns). Significantly enhanced dielectric breakdown strength of BiFeO₃‐based solid solutions is mainly attributed to the substitution of NaNbO₃, which provides an increased band gap, refined grain size, and increased resistivity. The formation of nanoscale domains as evidenced by piezoresponse force microscopy and transmission electron microscopy enables nearly hysteresis‐free polarization‐field response and temperature‐insensitive dielectric response. In comparison with antiferroelectric capacitors, the current work provides a new solution to successfully design next‐generation pulsed power capacitors by fully utilizing relaxor ferroelectrics in energy‐storage efficiency and thermal stability.     

Rational Construction of Self‐Standing Sulfur‐Doped Fe2O3 Anodes with Promoted Energy Storage Capability for Wearable Aqueous Rechargeable NiCo‐Fe Batteries

Aqueous rechargeable Ni‐Fe batteries featuring an ultra‐flat discharge plateau, low cost, and outstanding safety characteristics show promising prospects for application in wearable energy storage. In particular, fiber‐shaped Ni‐Fe batteries will enable textile‐based energy supply for wearable electronics. However, the development of fiber‐shaped Ni‐Fe batteries is currently challenged by the performance of fibrous Fe‐based anode materials. In this context, this study describes the fabrication of sulfur‐doped Fe₂O₃ nanowire arrays (S‐Fe₂O₃ NWAs) grown on carbon nanotube fibers (CNTFs) as an innovative anode material (S‐Fe₂O₃ NWAs/CNTF). Encouragingly, first‐principle calculations reveal that S‐doping in Fe₂O₃ can dramatically reduce the band gap from 2.34 to 1.18 eV and thus enhance electronic conductivity. The novel developed S‐Fe₂O₃ NWAs/CNTF electrode is further demonstrated to deliver a very high capacity of 0.81 mAh cm^?2 at 4 mA cm^?2. This value is almost sixfold higher than that of the pristine Fe₂O₃ NWAs/CNTF electrode. When a cathode containing zinc‐nickel‐cobalt oxide (ZNCO)@Ni(OH)₂ NWAs heterostructures is used, 0.46 mAh cm^?2 capacity and 67.32 mWh cm^?3 energy density are obtained for quasi‐solid‐state fiber‐shaped NiCo‐Fe batteries, which outperform most state‐of‐the‐art fiber‐shaped aqueous rechargeable batteries. These findings offer an innovative and feasible route to design high‐performance Fe‐based anodes and may inspire new development for the next‐generation wearable Ni‐Fe batteries.     

High‐Performance Fiber‐Shaped All‐Solid‐State Asymmetric Supercapacitors Based on Ultrathin MnO2 Nanosheet/Carbon Fiber Cathodes for Wearable Electronics

Flexible fiber‐shaped supercapacitors have shown great potential in portable and wearable electronics. However, small specific capacitance and low operating voltage limit the practical application of fiber‐shaped supercapacitors in high energy density devices. Herein, direct growth of ultrathin MnO₂ nanosheet arrays on conductive carbon fibers with robust adhesion is exhibited, which exhibit a high specific capacitance of 634.5 F g^?1 at a current density of 2.5 A g^?1 and possess superior cycle stability. When MnO₂ nanosheet arrays on carbon fibers and graphene on carbon fibers are used as a positive electrode and a negative electrode, respectively, in an all‐solid‐state asymmetric supercapacitor (ASC), the ASC displays a high specific capacitance of 87.1 F g^?1 and an exceptional energy density of 27.2 Wh kg^?1. In addition, its capacitance retention reaches 95.2% over 3000 cycles, representing the excellent cyclic ability. The flexibility and mechanical stability of these ASCs are highlighted by the negligible degradation of their electrochemical performance even under severely bending states. Impressively, as‐prepared fiber‐shaped ASCs could successfully power a photodetector based on CdS nanowires without applying any external bias voltage. The excellent performance of all‐solid‐state ASCs opens up new opportunity for development of wearable and self‐powered nanodevices in near future.     

Blood‐Capillary‐Inspired,Free‐Standing,Flexible, and Low‐Cost Super‐Hydrophobic N‐CNTs@SS Cathodes for High‐Capacity,High‐Rate,and Stable Li‐Air Batteries

With the rising demand for flexible and wearable electronic devices, flexible power sources with high energy densities are required to provide a sustainable energy supply. Theoretically, rechargeable, flexible Li‐O₂/air batteries can provide extremely high specific energy densities; however, the high costs, complex synthetic methods, and inferior mechanical properties of the available flexible cathodes severely limit their practical applications. Herein, inspired by the structure of human blood capillary tissue, this study demonstrates for the first time the in situ growth of interpenetrative hierarchical N‐doped carbon nanotubes on the surface of stainless‐steel mesh (N‐CNTs@SS) for the fabrication of a self‐supporting, flexible electrode with excellent physicochemical properties via a facile and scalable one‐step strategy. Benefitting from the synergistic effects of the high electronic conductivity and stable 3D interconnected conductive network structure, the Li‐O₂ batteries obtained with the N‐CNTs@SS cathode exhibit superior electrochemical performance, including a high specific capacity (9299 mA h g^?1 at 500 mA g^?1), an excellent rate capability, and an exceptional cycle stability (up to 232 cycles). Furthermore, as‐fabricated flexible Li‐air batteries containing the as‐prepared flexible super‐hydrophobic cathode show excellent mechanical properties, stable electrochemical performance, and superior H₂O resistibility, which enhance their potential to power flexible and wearable electronic devices.     

Nature Driven Bio‐Piezoelectric/Triboelectric Nanogenerator as Next‐Generation Green Energy Harvester for Smart and Pollution Free Society

Electronics wastes (e‐wastes) are the major concern in the rapid expansion of smart/wearable/portable electronics in modern high‐tech society. Informal processing and enormous gathering of e‐wastes can lead to adverse human/animal health effects and environmental pollution worldwide. Currently, these issues are a big headache and require the scientific community to develop effective green energy harvesting technologies using biodegradable/biocompatible materials. Piezoelectric/triboelectric nanogenerators (PNGs/TNGs) are considered one of the most promising renewable green energy sources for the conversion of mechanical/biomechanical energies into electricity. However, organic/inorganic material based PNGs/TNGs are very much incompatible, and considered e‐wastes for their non‐biodegradability. This review covers potential uses of biodegradable/biocompatible materials which are wasted every day as nature driven material based bio‐nanogenerators with a particular focus on their applications in flexible PNGs/TNGs fabrication. Structural investigation and possible working principles are described first in order to outline the basic mechanism of bio‐inspired materials behind energy harvesting. Then, energy harvesting abilities and the mechanical sensing of bio‐inspired integrated flexible devices are discussed under various mechanical/biomechanical activities. Finally, their potential applications in various flexible, wearable, and portable electronic fields are demonstrated. These bio‐inspired energy harvesting devices can make huge changes in fields as diverse as portable electronics, in vitro/in vivo biomedical applications, and many more.     

Reaching the Energy Density Limit of Layered O3‐NaNi0.5Mn0.5O2 Electrodes via Dual Cu and Ti Substitution

Although being less competitive energy density‐wise, Na‐ion batteries are serious alternatives to Li‐ion ones for applications where cost and sustainability dominate. O3‐type sodium layered oxides could partially overcome the energy limitation, but their practical use is plagued by a reaction process that enlists numerous phase changes and volume variations while additionally being moisture sensitive. Here, it is shown that the double substitution of Ti for Mn and Cu for Ni in O3‐NaNi_0.5?yCu_yMn_{0.5? z}Ti_zO₂ can alleviate most of these issues. Among this series, electrodes with specific compositions are identified that can reversibly release and uptake ≈0.9 sodium per formula unit via a smooth voltage‐composition profile enlisting minor lattice volume changes upon cycling as opposed to ΔV/V≈23% in the parent NaNi_0.5Mn_0.5O₂ while showing a greater resistance against moisture. The positive attributes of substitution are rationalized by structure considerations supported by density functional theory (DFT) calculations. Electrodes with sustained capacities of ≈180 mAh g^?1 are successfully implemented into 18 650 Na‐ion cells having greater performances, energy density‐wise (≈250 Wh L^?1), than today's Na₃V₂(PO₄)₂F₃/HC Na‐ion technology which excels in rate capabilities. These results constitute a step forward in increasing the practicality of Na‐ion technology with additional opportunities for applications in which energy density prevails over rate capability.     

Thermally Chargeable Solid‐State Supercapacitor

Ubiquitous low‐grade thermal energy, which is typically wasted without use, can be extremely valuable for continuously powering electronic devices such as sensors and wearable electronics. A popular choice for waste heat recovery has been thermoelectric energy conversion, but small output voltage without energy‐storing capability necessitates additional components such as a voltage booster and a capacitor. Here, a novel method of simultaneously generating a large voltage from a temperature gradient and storing electrical energy without losing the benefit of solid‐state no‐moving part devices like conventional thermoelectrics is reported. Thermally driven ion diffusion is used to greatly increase the output voltage (8 mV K^?1) with polystyrene sulfonic acid (PSSH) film. Polyaniline‐coated electrodes containing graphene and carbon nanotube sandwich the PSSH film where thermally induced voltage‐enabled electrochemical reactions, resulting in a charging behavior without an external power supply. With a small temperature difference (5 K) possibly created over wearable energy harvesting devices, the thermally chargeable supercapacitor produce 38 mV with a large areal capacitance (1200 F m^?2). It is anticipated that the attempt with thermally driven ion diffusion behaviors initiates a new research direction in thermal energy harvesting.     

Scalable Water‐Based Production of Highly Conductive 2D Nanosheets with Ultrahigh Volumetric Capacitance and Rate Capability

Highly conductive and ultrathin 2D nanosheets are of importance for the development of portable electronics and electric vehicles. However, scalable production and rational design for highly electronic and ionic conductive 2D nanosheets still remain a challenge. Herein, an industrially adoptable fluid dynamic exfoliation process is reported to produce large quantities of ionic liquid (IL)‐functionalized metallic phase MoS₂ (m‐MoS₂) and defect‐free graphene (Gr) sheets. Hybrid 2D–2D layered films are also fabricated by incorporating Gr sheets into compact m‐MoS₂ films. The incorporated IL functionalities and Gr sheets prevent aggregation and restacking of the m‐MoS₂ sheets, thereby creating efficient and rapid ion and electron pathways in the hybrid films. The hybrid film with a high packing density of 2.02 g cm^?3 has an outstanding volumetric capacitance of 1430.5 F cm^?3 at 1 A g^?1 and an extremely high rate capability of 80% retention at 1000 A g^?1. The flexible supercapacitor assembled using a polymer‐gel electrolyte exhibits excellent resilience to harsh electrochemical and mechanical conditions while maintaining an impressive rate performance and long cycle life. Successful achievement of an ultrahigh volumetric energy density (1.14 W h cm^?3) using an organic electrolyte with a wide cell voltage of ≈3.5 V is demonstrated.