Sulfidation of NiMn‐Layered Double Hydroxides/Graphene Oxide Composites toward Supercapacitor Electrodes with Enhanced Performance

Supercapacitors can deliver high‐power density and long cycle stability, but the limited energy density due to poor electronic and ionic conductivity of the supercapacitor electrode has been a bottleneck in many applications. A strategy to prepare microflower‐like NiMn‐layered double hydroxides (LDH) with sulfidation is delineated to reduce the charge transfer resistance of supercapacitor electrode and realize faster reversible redox reactions with notably enhanced specific capacitance. The incorporation of graphite oxide (GO) in NiMn LDH during sulfidation leads to simultaneous reduction of GO with enhanced conductivity, lessened defects, and doping of S into the graphitic structure. Cycling stability of the sulfidized composite electrode is enhanced due to the alleviation of phase transformation during electrochemical cycling test. As a result, this sulfidation product of LDH/GO (or LDHGOS) can reach a high‐specific capacitance of 2246.63 F g^?1 at a current density of 1 A g^?1, and a capacitance of 1670.83 F g^?1 is retained at a high‐current density of 10 A g^?1, exhibiting an outstanding capacitance and rate performance. The cycling retention of the LDHGOS electrode is also extended to ≈ 67% after 1500 cycles compared to only ≈44% of the pristine NiMn LDH.     

General Controlled Sulfidation toward Achieving Novel Nanosheet‐Built Porous Square‐FeCo2S4‐Tube Arrays for High‐Performance Asymmetric All‐Solid‐State Pseudocapacitors

A significant advance toward the design and fabrication of a novel hierarchical supercapacitor electrode consisting of FeCo₂S₄‐tubes with well‐defined square cross‐section and intersecting nanosheets built porous shells on a 3D porous Ni backbone via controlled sulfidation is reported. This general method allows template‐free synthesis of metal sulfides tubular structures with polygonal cross‐sections and also fine control over the nanostructure leading to both maximized porosity and saturation sulfidation. New insights into concentration and time dependent sulfidation reaction kinetics are proposed. The FeCo₂S₄ electrode achieves a specific capacitance reaching 2411 F g^‐1 at 5 mA cm^‐2 and good rate capability, which are superior over those for nanotube arrays of other ternary transition metal sulfides. This is attributed to rich redox reactions, the highly porous but robust architecture as well as high electrical conductivity. Especially such porous shells effectively avoid “dead volume”, thus improve the utilization ratio of the electrode material. Asymmetric solid‐state device applying the FeCo₂S₄ as positive electrode and N‐doped graphene hydrogel film as negative electrode has a high cell voltage of 1.6 V and thus delivers considerably higher energy density of 76.1 W h kg^‐1 (at 755 W kg^‐1) than those reported for similar devices.     

Wearable High‐Performance Supercapacitors Based on Silver‐Sputtered Textiles with FeCo2S4–NiCo2S4 Composite Nanotube‐Built Multitripod Architectures as Advanced Flexible Electrodes

To achieve high‐performance wearable supercapacitors (SCs), a new class of flexible electrodes with favorable architectures allowing large porosity, high conductivity, and good mechanical stability is strongly needed. Here, this study reports the rational design and fabrication of a novel flexible electrode with nanotube‐built multitripod architectures of ternary metal sulfides' composites (FeCo₂S₄–NiCo₂S₄) on a silver‐sputtered textile cloth. Silver sputtering is applicable to almost all kinds of textiles, and S^2? concentration is optimized during sulfidation process to achieve such architectures and also a complete sulfidation assuring high conductivity. New insights into concentration‐dependent sulfidation mechanism are proposed. The additive‐free FeCo₂S₄–NiCo₂S₄ electrode shows a high specific capacitance of 1519 F g^?1 at 5 mA cm^?2 and superior rate capability (85.1% capacitance retention at 40 mA cm^?2). All‐solid‐state SCs employing these advanced electrodes deliver high energy density of 46 W h kg^?1 at 1070 W kg^?1 as well as achieve remarkable cycling stability retaining 92% of initial capacitance after 3000 cycles at 10 mA cm^?2, and outstanding reliability with no capacitance degradation under large twisting. These are attributed to the components' synergy assuring rich redox reactions, high conductivity as well as highly porous but robust architectures. An almost linear increase in capacitance with devices' area indicates possibility to meet various energy output requirements. This work provides a general, low‐cost route to wearable power sources.     

Achieving High Rate Performance in Layered Hydroxide Supercapacitor Electrodes

Layered hydroxides (LHs) are promising supercapacitor electrode materials with high specific capacitances. However, they generally exhibit poor energy storage ability at high current densities due to their insulating nature. Nickel‐cobalt‐aluminum LHs are synthesized and chemically treated to form LHs with enhanced conductivity that results in greatly enhanced rate performances. The key role of chemical treatment is to enable the partial conversion of Co²⁺ to a more conductive Co³⁺ state that stimulates charge transfers. Simultaneously, the defects on the LHs caused by the selective etching of Al promoted the electrolyte diffusion within LHs. As a result, the LHs show a high specific capacitance of 738 F g^?1 at 30 A g^?1, which is 57.2% of 1289 F g^?1 at 1 A g^?1. The strategy provides a facile and effective method to achieve high performance LHs for supercapacitor electrode materials.     

Ultrathin and Porous Ni3S2/CoNi2S4 3D‐Network Structure for Superhigh Energy Density Asymmetric Supercapacitors

3D‐networked, ultrathin, and porous Ni₃S₂/CoNi₂S₄ on Ni foam (NF) is successfully designed and synthesized by a simple sulfidation process from 3D Ni–Co precursors. Interestingly, the edge site‐enriched Ni₃S₂/CoNi₂S₄/NF 3D‐network is realized by the etching‐like effect of S^2? ions, which made the surfaces of Ni₃S₂/CoNi₂S₄/NF with a ridge‐like feature. The intriguing structural/compositional/componental advantages endow 3D‐networked‐free‐standing Ni₃S₂/CoNi₂S₄/NF electrodes better electrochemical performance with specific capacitance of 2435 F g^?1 at a current density of 2 A g^?1 and an excellent rate capability of 80% at 20 A g^?1. The corresponding asymmetric supercapacitor achieves a high energy density of 40.0 W h kg^?1 at an superhigh power density of 17.3 kW kg^?1, excellent specific capacitance (175 F g^?1 at 1A g^?1), and electrochemical cycling stability (92.8% retention after 6000 cycles) with Ni₃S₂/CoNi₂S₄/NF as the positive electrode and activated carbon/NF as the negative electrode. Moreover, the temperature dependences of cyclic voltammetry curve polarization and specific capacitances are carefully investigated, and become more obvious and higher, respectively, with the increase of test temperature. These can be attributed to the components' synergetic effect assuring rich redox reactions, high conductivity as well as highly porous but robust architectures. This work provides a general, low‐cost route to produce high performance electrode materials for portable supercapacitor applications on a large scale.     

Controlled Growth of NiMoO4 Nanosheet and Nanorod Arrays on Various Conductive Substrates as Advanced Electrodes for Asymmetric Supercapacitors

Hierarchical NiMoO₄ architectures assembled from well‐aligned uniform nanosheets or nanorods are successfully grown on various conductive substrates using a facile and effective general approach. Importantly, the nanostructures of NiMoO₄ can be easily controlled to be nanosheets or nanorods by using different solvents. By virtue of their intriguing structure features, NiMoO₄ nanosheets as integrated additive‐free electrodes for supercapacitors manifest higher Faradaic capacitance than NiMoO₄ nanorods. Moreover, an asymmetric supercapacitor (ASC) is constructed using the as‐prepared NiMoO₄ nanosheets as the positive electrode and activated carbon (AC) as the negative electrode. The optimized ASC with an extended operating voltage range of 0–1.7 V displays excellent electrochemical performance with a high energy density of 60.9 Wh kg^?1 at a power density of 850 W kg^?1 in addition to superior rate capability. Furthermore, the NiMoO₄//AC ASC device exhibits remarkable cycling stability with 85.7% specific capacitance retention after 10 000 cycles. The results show that these NiMoO₄‐based nanostructures are promising for high‐energy supercapacitors.     

Vanadium Oxide Nanowire–Carbon Nanotube Binder‐Free Flexible Electrodes for Supercapacitors

Vanadium pentoxide (V₂O₅) layered nanostructures are known to have very stable crystal structures and high faradaic activity. The low electronic conductivity of V₂O₅ greatly limits the application of vanadium oxide as electrode materials and requires combining with conducting materials using binders. It is well known that the organic binders can degrade the overall performance of electrode materials and need carefully controlled compositions. In this study, we develop a simple method for preparing freestanding carbon nanotube (CNT)‐V₂O₅ nanowire (VNW) composite paper electrodes without using binders. Coin cell type (CR2032) supercapacitors are assembled using the nanocomposite paper electrode as the anode and high surface area carbon fiber electrode (Spectracarb 2225) as the cathode. The supercapacitor with CNT‐VNW composite paper electrode exhibits a power density of 5.26 kW Kg^?1 and an energy density of 46.3 Wh Kg^?1. (Li)VNWs and CNT composite paper electrodes can be fabricated in similar manner and show improved overall performance with a power density of 8.32 kW Kg^?1 and an energy density of 65.9 Wh Kg^?1. The power and energy density values suggest that such flexible hybrid nanocomposite paper electrodes may be useful for high performance electrochemical supercapacitors.     

Nanostructured Ternary Electrodes for Energy‐Storage Applications

A three‐component, flexible electrode is developed for supercapacitors over graphitized carbon fabric, utilizing γ‐MnO₂ nanoflowers anchored onto carbon nanotubes (γ‐MnO₂/CNT) as spacers for graphene nanosheets (GNs). The three‐component, composite electrode doubles the specific capacitance with respect to GN‐only electrodes, giving the highest‐reported specific capacitance (308 F g^?1) for symmetric supercapacitors containing MnO₂ and GNs using a two‐electrode configuration, at a scan rate of 20 mV s^?1. A maximum energy density of 43 W h kg^?1 is obtained for our symmetric supercapacitors at a constant discharge‐current density of 2.5 A g^?1 using GN–(γ‐MnO₂/CNT)‐nanocomposite electrodes. The fabricated supercapacitor device exhibits an excellent cycle life by retaining ≈90% of the initial specific capacitance after 5000 cycles.     

Functional Pillared Graphene Frameworks for Ultrahigh Volumetric Performance Supercapacitors

Supercapacitors, also known as electrochemical capacitors, can provide much faster charge–discharge, greater power density, and cyclability than batteries, but they are still limited by lower energy densities (or the amount of energy stored per unit volume). Here, a novel strategy for the synthesis of functional pillared graphene frameworks, in which graphene fragments in‐between graphene sheets, through simple thermal‐treatment of ozone (O₃)‐treated graphene oxide at very low temperature of 200 °C is reported. Due to its high packing density, high content of stable oxygen species, and continues ion transport network in‐between graphene sheets, the functional pillared‐graphene framework delivers not only high gravimetric capacitance (353 F g^?1 based on the mass of the active material) and ultrahigh volumetric capacitance (400 F cm^?3 based on total mass of electrode material) in aqueous electrolyte but also excellent cyclic stability with 104% of its initial capacitance retention after 10 000 cycles. Moreover, the assembled symmetric supercapacitor achieves as high as 27 Wh L^?1 of volumetric energy density at a power density of 272 W L^?1. This novel strategy holds great promise for future design of high volumetric capacitance supercapacitors.     

Antimonene Engineered Highly Deformable Freestanding Electrode with Extraordinarily Improved Energy Storage Performance

Advanced 2D materials have spurred great interest as a new paradigm in pursuing improved energy storage performance. Herein, for the first time, antimonene is utilized as an effective active component for constructing highly deformable and editable freestanding film electrodes, as the basis of a supercapacitor with record‐breaking electrode performance. The insertion of antimonene is able to improve the environmental stability of the antimonene/MXene composite electrode and remarkably enhance the energy storage capability in both protic and neutral electrolytes. Notably, an ultrahigh specific volumetric capacitance of 4255 F cm^?3 is achieved by the electrode tested in a1 m H₂SO₄ electrolyte, which represents the state‐of‐the‐art value reported to date for supercapacitor electrodes based on MXenes. The flexible supercapacitors constructed by the composite electrode, also demonstrate highly competitive energy and power densities: 459.75 mWh cm^?3 and 3.12 W cm^?3 for the asymmetrical one with a much widened potential window of 2 V in neutral electrolyte; 112.52 mWh cm^?3 and 1 W cm^?3 for the symmetrical configuration with an outstanding capacitance of 1265 F cm^?3 in acidic media. This work sheds new light on the fabrication of high‐performance supercapacitor electrodes with functionalities in different electrolyte media and various device configurations.     

Highly Flexible,Freestanding Supercapacitor Electrode with Enhanced Performance Obtained by Hybridizing Polypyrrole Chains with MXene

Though polypyrrole (PPy) is widely used in flexible supercapacitors owing to its high electrochemical activity and intrinsic flexibility, limited capacitance and cycling stability of freestanding PPy films greatly reduce their practicality in real‐world applications. Herein, we report a new approach to enhance PPy's capacitance and cycling stability by forming a freestanding and conductive hybrid film through intercalating PPy into layered Ti₃C₂ (l‐Ti₃C₂, a MXene material). The capacitance increases from 150 (300) to 203 mF cm^?2 (406 F cm^?3). Moreover, almost 100% capacitance retention is achieved, even after 20 000 charging/discharging cycles. The analyses reveal that l‐Ti₃C₂ effectively prevents dense PPy stacking, benefiting the electrolyte infiltration. Furthermore, strong bonds, formed between the PPy backbones and surfaces of l‐Ti₃C₂, not only ensure good conductivity and provide precise pathways for charge‐carrier transport but also improve the structural stability of PPy backbones. The freestanding PPy/l‐Ti₃C₂ film is further used to fabricate an ultra‐thin all‐solid‐state supercapacitor, which shows an excellent capacitance (35 mF cm^?2), stable performance at any bending state and during 10 000 charging/discharging cycles. This novel strategy provides a new way to design conductive polymer‐based freestanding flexible electrodes with greatly improved electrochemical performances.     

Structure‐Controlled,Vertical Graphene‐Based,Binder‐Free Electrodes from Plasma‐Reformed Butter Enhance Supercapacitor Performance

Vertical graphene nanosheets (VGNS) hold great promise for high‐performance supercapacitors owing to their excellent electrical transport property, large surface area and in particular, an inherent three‐dimensional, open network structure. However, it remains challenging to materialise the VGNS‐based supercapacitors due to their poor specific capacitance, high temperature processing, poor binding to electrode support materials, uncontrollable microstructure, and non‐cost effective way of fabrication. Here we use a single‐step, fast, scalable, and environmentally‐benign plasma‐enabled method to fabricate VGNS using cheap and spreadable natural fatty precursor butter, and demonstrate the controllability over the degree of graphitization and the density of VGNS edge planes. Our VGNS employed as binder‐free supercapacitor electrodes exhibit high specific capacitance up to 230 F g^?1 at a scan rate of 10 mV s^?1 and >99% capacitance retention after 1,500 charge‐discharge cycles at a high current density, when the optimum combination of graphitic structure and edge plane effects is utilised. The energy storage performance can be further enhanced by forming stable hybrid MnO₂/VGNS nano‐architectures which synergistically combine the advantages from both VGNS and MnO₂. This deterministic and plasma‐unique way of fabricating VGNS may open a new avenue for producing functional nanomaterials for advanced energy storage devices.     

2D Metal Zn Nanostructure Electrodes for High‐Performance Zn Ion Supercapacitors

Recent supercapacitors show a high power density with long‐term cycle life time in energy‐powering applications. A supercapacitor based on a single metal electrode accompanying multivalent cations, multiple charging/discharging kinetics, and high electrical conductivity is a promising energy‐storing system that replaces conventionally used oxide and sulfide materials. Here, a hierarchically nanostructured 2D‐Zn metal electrode‐ion supercapacitor (ZIC) is reported which significantly enhances the ion diffusion ability and overall energy storage performance. Those nanostructures can also be successfully plated on various flat‐type and fiber‐type current collectors by a controlled electroplating method. The ZIC exhibits excellent pseudocapacitive performance with a high energy density of 208 W h kg^?1 and a power density from 500 W kg^?1, which are significantly higher than those of previously reported supercapacitors with oxide and sulfide materials. Furthermore, the fiber‐type ZIC also shows high energy‐storing performance, outstanding mechanical flexibility, and waterproof characteristics, without any significant capacitance degradation during bending tests. These results highlight the promising possibility of nanostructured 2D Zn metal electrodes with the controlled electroplating method for future energy storage applications.     

All‐Printed MnHCF‐MnOx‐Based High‐Performance Flexible Supercapacitors

Here, a simple active materials synthesis method is presented that boosts electrode performance and utilizes a facile screen‐printing technique to prepare scalable patterned flexible supercapacitors based on manganese hexacyanoferrate‐manganese oxide and electrochemically reduced graphene oxide electrode materials (MnHCF‐MnO_x/ErGO). A very simple in situ self‐reaction method is developed to introduce MnO_x pseudocapacitor material into the MnHCF system by using NH₄F. This MnHCF‐MnO_x electrode materials can deliver excellent capacitance of 467 F g^?1 at a current density of 1 A g^?1, which is a 2.4 times capacitance increase compared to MnHCF. In addition a printed, patterned, flexible MnHCF‐MnO_x/ErGO supercapacitor is fabricated, showing a remarkable areal capacitance of 16.8 mF cm^?2 and considerable energy and power density of 0.5 mWh cm^?2 and 0.0023 mW cm^?2, respectively. Furthermore, the printed patterned flexible supercapacitors also exhibit exceptional flexibility, and the capacitance remains stable, even while bending to various angles (60°, 90°, and 180°) and for 100 cycles. The flexible supercapacitor arrays integrated by multiple prepared single supercapacitors can power various LEDs even in the bent states. This approach offers promising opportunities for the development of printable energy storage materials and devices with high energy density, large scalability, and excellent flexibility.     

Pore and Heteroatom Engineered Carbon Foams for Supercapacitors

Carbonaceous materials are attractive supercapacitor electrode materials due to their high electronic conductivity, large specific surface area, and low cost. Here, a unique hierarchical porous N,O,S‐enriched carbon foam (KNOSC) with high level of structural complexity for supercapacitors is reported. It is fabricated via a combination of a soft‐template method, freeze‐drying, and chemical etching. The carbon foam is a macroporous structure containing a network of mesoporous channels filled with micropores. It has an extremely large specific surface area of 2685 m² g^?1. The pore engineered carbon structure is also uniformly doped with N, O, and S. The KNOSC electrode achieves an outstanding capacitance of 402.5 F g^?1 at 1 A g^?1 and superior rate capability of 308.5 F g^?1 at 100 A g^?1. The KNOSC exhibits a Bode frequency at the phase angle of ?45° of 18.5 Hz, which corresponds to a time constant of 0.054 s only. A symmetric supercapacitor device using KNOSC as electrodes can be charged/discharged within 1.52 s to deliver a specific energy density of 15.2 W h kg^?1 at a power density of 36 kW kg^?1. These results suggest that the pore and heteroatom engineered structures are promising electrode materials for ultrafast charging.     

Miniaturized Supercapacitors: Focused Ion Beam Reduced Graphene Oxide Supercapacitors with Enhanced Performance Metrics

Miniaturization of energy storage devices with enhanced performance metrics can reduce the footprint of microdevices being used in our daily life. Micro‐­supercapacitor architectures with planar geometry provides several advantages, such as, the ability to control and reduce the distances ions travel between two electrodes, easy integration to microdevices, and offer the potential of being extended into 3D without compromising the interelectrode distances. Here, focused ion beam (FIB) technology is used to directly write miniaturized planar electrode systems of reduced graphene oxide (FIB‐rGO) on films of graphene oxide. Using optimized ion beam irradiation, interdigitated FIB‐rGO electrode designs with 40 μm long and 3.5 μm wide fingers with ultrasmall interelectrode spacing of 1 μm demonstrate a large capacitance (102 mF cm^?2), ultrasmall time response (0.03 ms), low equivalent series resistance (0.35 mΩ cm²), and retain 95% of the capacitance after 1000 cycles at an ultrahigh current density of 45 mA cm^?2. These performance metrics show remarkable improvements on several counts of supercapacitor performance over existing reports due to the miniaturized electrode dimensions and minimal damage to the graphene sheets. It is believed that these results can provide avenues for large‐scale fabrication of arrayed, planar, high‐performance micro‐supercapacitors with a small environmental footprint.     

Large‐Scale Conductive Yarns Based on Twistable Korean Traditional Paper (Hanji) for Supercapacitor Applications: Toward High‐Performance Paper Supercapacitors

A simple and scalable method to fabricate a yarn‐type supercapacitor with a large specific capacitance without the aid of traditional pseudocapacitive electrode materials such as conducting polymers and metal oxides is reported. The yarn‐type supercapacitors are made from twisting reduced graphene oxide (rGO) or/and single‐walled carbon nanotubes (SWNTs)‐coated Korean traditional paper (KTP). The yarn‐type paper supercapacitor displays surprisingly enhanced electrochemical capacitance values, showing synergistic effect between rGO and SWNTs (500 times larger than performance of yarn‐type rGO‐coated paper supercapacitors). Coating rGO or/and SWNTs on KTP gives good morphology to the composite film, in which porosity increases and mean pore diameter decreases. The yarn‐type rGO/SWNT paper supercapacitor shows good mechanical strength, high flexibility, excellent electrochemical performance, and long‐life operation. The yarn‐type supercapacitor has an excellent electrochemical performance with a specific capacitance of 366 F g^?1 at scan rate of 25 mV s^?1 and high stability without any degradation in electrical performance up to 10 000 charge–discharge cycles. The average capacitance of rGO/SWNT@KTP yarn‐type supercapacitors is seven times higher than that of sheet‐type supercapacitors at scan rate of 500 mV s^?1. The lighting of a red light‐emitting diode (LED) is demonstrated by the yarn‐type paper supercapacitor without connecting supercapacitors in series.     

Flexible Nano‐felts of Carbide‐Derived Carbon with Ultra‐high Power Handling Capability

Nano‐fibrous felts (nano‐felts) of carbide‐derived carbon (CDC) have been developed from the precursor of electrospun titanium carbide (TiC) nano‐felts. Conformal transformation of TiC into CDC conserves main features of the precursor including the high interconnectivity and structural integrity; the developed TiC‐CDC nano‐felts are mechanically flexible/resilient, and can be used as electrode material for supercapacitor application without the addition of any binder. After synthesis through chlorination of the precursor at 600 °C, the TiC‐CDC nano‐fibers show an average pore size of ～1nm, a high specific surface area of 1390 m²/g; and the nano‐fibers have graphitic carbon ribbons embedded in a highly disordered carbon matrix. Graphitic carbon is preserved from the precursor nano‐fibers where a few graphene layers surround TiC nanocrystallites. Electrochemical measurements show a high gravimetric capacitance of 110 F/g in aqueous electrolyte (1 M H₂SO₄) and 65 F/g in organic electrolyte (1.5 M TEA‐BF₄ in acetonitrile). Because of the unique microstructure of TiC‐CDC nano‐felts, a fade of the capacitance of merely 50% at a high scan rate of 5 V/s is observed. A fade of just 15% is observed for nano‐felt film electrodes tested in 1 M H₂ SO₄ at 1 V/s, resulting in a high gravimetric capacitance of 94 F/g. Such a high rate performance is only known for graphene or carbon‐onion based supercapacitors, whereas binders have to be used for the fabrication of those supercapacitors.     

Battery‐like Supercapacitors from Vertically Aligned Carbon Nanofiber Coated Diamond: Design and Demonstrator

To fabricate battery‐like supercapacitors with high power and energy densities, big capacitances, as well as long‐term capacitance retention, vertically aligned carbon nanofibers (CNFs) grown on boron doped diamond (BDD) films are employed as the capacitor electrodes. They possess large surface areas, high conductivity, high stability, and importantly are free of binder. The large surface areas result from their porous structures. The containment of graphene layers and copper metal catalysts inside CNFs leads to their high conductivity. Both electrical double layer capacitors (EDLCs) in inert solutions and pseudocapacitors (PCs) using Fe(CN)₆^3?/4? redox‐active electrolytes are constructed with three‐ and two‐electrode systems. The assembled two‐electrode symmetrical supercapacitor devices exhibit capacitances of 30 and 48 mF cm^?2 at 10 mV s^?1 for EDLC and PC devices, respectively. They remain constant even after 10 000 charging/discharging cycles. The power densities are 27.3 and 25.3 kW kg^?1 for EDLC and PC devices, together with their energy densities of 22.9 and 44.1 W h kg^?1, respectively. The performance of these devices is superior to most of the reported supercapacitors and batteries. Vertically aligned CNF/BDD hybrid films are thus useful to construct high‐performance battery‐like and industry‐orientated supercapacitors for future power devices.     

High Performance,Flexible, Solid‐State Supercapacitors Based on a Renewable and Biodegradable Mesoporous Cellulose Membrane

A flexible, transparent, and renewable mesoporous cellulose membrane (mCel‐membrane) featuring uniform mesopores of ≈24.7 nm and high porosity of 71.78% is prepared via a facile and scalable solution‐phase inversion process. KOH‐saturated mCel‐membrane as a polymer electrolyte demonstrates a high electrolyte retention of 451.2 wt%, a high ionic conductivity of 0.325 S cm^?1, and excellent mechanical flexibility and robustness. A solid‐state electric double layer capacitor (EDLC) using activated carbon as electrodes, the KOH‐saturated mCel‐membrane as a polymer electrolyte exhibits a high capacitance of 110 F g^?1 at 1.0 A g^?1, and long cycling life of 10 000 cycles with 84.7% capacitance retention. Moreover, a highly integrated planar‐type micro‐supercapacitor (MSC) can be facilely fabricated by directly depositing the electrode materials on the mCel‐membrane‐based polymer electrolyte without using complicated devices. The resulting MSC exhibits a high areal capacitance of 153.34 mF cm^?2 and volumetric capacitance of 191.66 F cm^?3 at 10 mV s^?1, representing one of the highest values among all carbon‐based MSC devices. These findings suggest that the developed renewable, flexible, mesoporous cellulose membrane holds great promise in the practical applications of flexible, solid‐state, portable energy storage devices that are not limited to supercapacitors.