Reusable Cellulose‐Based Hydrogel Sticker Film Applied as Gate Dielectric in Paper Electrolyte‐Gated Transistors

A new concept for reusable eco‐friendly hydrogel electrolytes based on cellulose is introduced. The reported electrolytes are designed and engineered through a simple, fast, low‐cost, and eco‐friendly dissolution method of microcrystalline cellulose at low temperature using an aqueous LiOH/urea solvent system. The cellulose solution is combined with carboxymethyl cellulose, followed by the regeneration and simultaneous ion incorporation. The produced free standing cellulose‐based electrolyte films exhibit interesting properties for application in flexible electrochemical devices, such as biosensors or electrolyte‐gated transistors (EGTs), because of their high specific capacitances (4–5 µF cm^?2), transparency, and flexibility. Indium–gallium–zinc‐oxide EGTs on glass with laminated cellulose‐based hydrogel electrolytes (CHEs) as the gate dielectric are produced presenting a low working voltage (<2 V), showing an on–off current ratio (I _on/off) of 10⁶, a subthreshold swing lower than 0.2 V dec^?1, and saturation mobility (μ_Sat) reaching 26 cm² V^?1 s^?1. The flexible CHE‐gated transistors on paper are also demonstrated, which operate at switching frequencies up to 100 Hz. Combining the flexibility of the EGTs on paper with the reusability of the developed CHEs is a breakthrough toward biodegradable advanced functional materials allied with disposable/recyclable and low‐cost electronic devices.     

Field-effect transistor based on ZnO nanorods with a variable threshold cutoff voltage

This study is concerned with the fabrication and electrical characteristics of short-channel (2 μm) field-effect transistors (FETs) based on ZnO nanorods. In FET fabrication, single-crystal ZnO nanorods are grown using the catalyst-free chemical vapor deposition (CVD) method. Although the short-channel ZnO-nanorod FETs exhibit good electrical characteristics (a transconductance of 100 nS, electron mobility of 6 cm² V^?1 s^?1, and a large turn-ON/OFF ratio of 10⁴), their characteristics significantly depend on the length of the nanorods. The effect of the drain-source voltage on the threshold gate voltage is studied.     

High‐Speed,Low‐Voltage,and Environmentally Stable Operation of Electrochemically Gated Zinc Oxide Nanowire Field‐Effect Transistors

Single‐crystal, 1D nanostructures are well known for their high mobility electronic transport properties. Oxide‐nanowire field‐effect transistors (FETs) offer both high optical transparency and large mechanical conformability which are essential for flexible and transparent display applications. Whereas the “on‐currents” achieved with nanowire channel transistors are already sufficient to drive active matrix organic light emitting diode (AMOLED) displays; it is shown here that incorporation of electrochemical‐gating (EG) to nanowire electronics reduces the operation voltage to ≤2 V. This opens up new possibilities of realizing flexible, portable, transparent displays that are powered by thin film batteries. A composite solid polymer electrolyte (CSPE) is used to obtain all‐solid‐state FETs with outstanding performance; the field‐effect mobility, on/off current ratio, transconductance, and subthreshold slope of a typical ZnO single‐nanowire transistor are 62 cm²/Vs, 10⁷, 155 μS/μm and 115 mV/dec, respectively. Practical use of such electrochemically‐gated field‐effect transistor (EG FET) devices is supported by their long‐term stability in air. Moreover, due to the good conductivity (≈10^?2 S/cm) of the CSPE, sufficiently high switching speed of such EG FETs is attainable; a cut‐off frequency in excess of 100 kHz is measured for in‐plane FETs with large gate‐channel distance of >10 μm. Consequently, operation speeds above MHz can be envisaged for top‐gate transistor geometries with insulator thicknesses of a few hundreds of nanometers. The solid polymer electrolyte developed in this study has great potential in future device fabrication using all‐solution processed and high throughput techniques.     

All-Printed Green Micro-Supercapacitors Based on a Natural-derived Ionic Liquid for Flexible Transient Electronics

The fabrication and characterization of green, flexible, and ultra-thin supercapacitors that are able to operate above 1.5 V is reported, using an all-printed fabrication process. The devices are produced by aqueous spray casting of a natural-derived electrolyte ionogel composed by 2-hydroxyethyl cellulose and by the ionic liquid choline lactate, while the electrodes are composed of highly porous nanostructured carbon films deposited by supersonic cluster beam deposition (SCBD). The obtained supercapacitors (device thickness < 10 μm) are stable to bending and they possess power values up to 120 kW kg^–1. The combination of aqueous spray casting and SCBD constitutes a versatile, scalable, and eco-friendly fabrication process able to directly print interconnected elements suitable for transient electronic systems.     

Multilayer‐Folded Graphene Ribbon Film with Ultrahigh Areal Capacitance and High Rate Performance for Compressible Supercapacitors

Limited by 2D geometric morphology and low bulk packing density, developing graphene‐based flexible/compressible supercapacitors with high specific capacitances (gravimetric/volumetric/areal), especially at high rates, is an outstanding challenge. Here, a strategy for the synthesis of free‐standing graphene ribbon films (GRFs) for high‐performance flexible and compressible supercapacitors through blade‐coating of interconnected graphene oxide ribbons and a subsequent thermal treatment process is reported. With an ultrahigh mass loading of 21 mg cm^?2, large ion‐accessible surface area, efficient electron and ion transport pathways as well as high packing density, the compressed multilayer‐folded GRF films (F‐GRF) exhibit ultrahigh areal capacitance of 6.7 F cm^?2 at 5 mA cm^?2, high gravimetric/volumetric capacitances (318 F g^?1, 293 F cm^?3), and high rate performance (3.9 F cm^?2 at 105 mA cm^?2), as well as excellent cycling stability (109% of capacitance retention after 40 000 cycles). Furthermore, the assembled F‐GRF symmetric supercapacitor with compressible and flexible characteristics, can deliver an ultrahigh areal energy density of 0.52 mWh cm^?2 in aqueous electrolyte, almost two times higher than the values obtained from symmetric supercapacitors with comparable dimensions.     

Radially Aligned Porous Carbon Nanotube Arrays on Carbon Fibers: A Hierarchical 3D Carbon Nanostructure for High‐Performance Capacitive Energy Storage

A novel and scalable synthesis approach to produce hierarchically aligned porous carbon nanotube arrays (PCNTAs) on flexible carbon fibers (CFs) is developed. The PCNTAs are obtained by catalytic conversion of ethanol on ZnO nanorod arrays and then reduction‐evaporation of ZnO nanorods, resulting in uniform and controllable wall thicknesses of the final PCNTAs. The 3D arrangement, the diameters, and the lengths of the PCNTAs can be tuned by adjusting the synthesis protocols of the ZnO nanorod arrays. The PCNTAs@CFs exhibit a high specific capacitance of 182 F g^?1 at 40 A g^?1 (188 F g^?1 at 20 A g^?1) in 6 m KOH. The symmetric supercapacitor shows an excellent cycling stability with only 0.0016% loss per cycle after 10 000 continuous cycles at the current density of 12 A g^?1. These excellent electrochemical performances are ascribed to the unique structural design of hierarchical PCNTAs, which provide not only appropriate channels for enhanced electronic and ionic transport but also increased surface area for accessing more electrolyte ions. The structural design and the synthesis approach are general and can be extended to synthesizing a broad range of materials systems.     

Micro‐Supercapacitors Based on Interdigital Electrodes of Reduced Graphene Oxide and Carbon Nanotube Composites with Ultrahigh Power Handling Performance

A novel method for fabricating micro‐patterned interdigitated electrodes based on reduced graphene oxide (rGO) and carbon nanotube (CNT) composites for ultra‐high power handling micro‐supercapacitor application is reported. The binder‐free microelectrodes were developed by combining electrostatic spray deposition (ESD) and photolithography lift‐off methods. Without typically used thermal or chemical reduction, GO sheets are readily reduced to rGO during the ESD deposition. Electrochemical measurements show that the in‐plane interdigital design of the microelectrodes is effective in increasing accessibility of electrolyte ions in‐between stacked rGO sheets through an electro‐activation process. Addition of CNTs results in reduced restacking of rGO sheets and improved energy and power density. Cyclic voltammetry (CV) measurements show that the specific capacitance of the micro‐supercapacitor based on rGO–CNT composites is 6.1 mF cm^?2 at 0.01 V s^?1. At a very high scan rate of 50 V s^?1, a specific capacitance of 2.8 mF cm^?2 (stack capacitance of 3.1 F cm^?3) is recorded, which is an unprecedented performance for supercapacitors. The addition of CNT, electrolyte‐accessible and binder‐free microelectrodes, as well as an interdigitated in‐plane design result in a high‐frequency response of the micro‐supercapacitors with resistive‐capacitive time constants as low as 4.8 ms. These characteristics suggest that interdigitated rGO–CNT composite electrodes are promising for on‐chip energy storage application with high power demands.     

Pom Functionalized Ionogels with Tunable Optical,Mechanical, Electrical,and Sensory Properties

Ionogels, with wide applications in tissue engineering, soft robotics, and flexible iontronic devices, require tunable optical, mechanical, and electrical properties for advanced functionality applications. Here, a facile strategy is reported to tune a set of properties of ionogels via tuning the redox states of the added polyoxometalate (POM) clusters. Upon external electrical stimuli, the POM clusters in the ionogels can be reversibly tuned from a transparent, oxidized state to a blue, reduced state. The redox states of the POM anions influence the POM-polymer interactions, which promotes the in situ modulation of the ionogel properties reversibly over a large window: optical transparency from 91% to 7%, dissipated energy from 0.9 to 3.1 MJ m⁻³, elastic modulus from 1.5 to 2 MPa, conductivity from 1.6 × 10⁻⁴ to 2.2 × 10⁻⁴ S cm⁻¹. Meanwhile, the sensory properties of the ionogels can be modulated simultaneously. For strain sensing and pressure sensing, the GF can be tuned from 2.3 to 7.2, and the sensitivity can be tuned from 0.8 to 1.2 kPa⁻¹. Such an ionogel with tunable optical, mechanical, and electrical properties may find a variety of applications meeting specific demands. The POM functionalization strategy may also bring new insights into the design of the stimuli-responsive ionogels.     

Shape Persistent,Highly Conductive Ionogels from Ionic Liquids Reinforced with Cellulose Nanocrystal Network

Shape-persistent, conductive ionogels where both mechanical strength and ionic conductivity are enhanced are developed using multiphase materials composed of cellulose nanocrystals and hyperbranched polymeric ionic liquids (PILs) as a mechanically strong supporting network matrix for ionic liquids with an interrupted ion-conducting pathway. The integration of needlelike nanocrystals and PIL promotes the formation of multiple hydrogen bonding and electrostatic ionic interaction capacitance, resulting in the formation of interconnected networks capable of confining a high amount of ionic liquid (≈95 wt%) without losing its self-sustained shape. The resulting nanoporous and robust ionogels possess outstanding mechanical strength with a high compressive elastic modulus (≈5.6 MPa), comparable to that of tough, rubbery materials. Surprisingly, these rigid materials preserve the high ionic conductivity of original ionic liquids (≈7.8 mS cm⁻¹), which are distributed within and supported by the nanocrystal network-like rigid frame. On the one hand, such stable materials possess superior ionic conductivities in comparison to traditional solid electrolytes; on the other hand, the high compression resistance and shape-persistence allow for easy handling in comparison to traditional fluidic electrolytes. The synergistic enhancement in ion transport and solid-like mechanical properties afforded by these ionogel materials make them intriguing candidates for sustainable electrodeless energy storage and harvesting matrices.     

Oxygen‐Deficient Bismuth Oxide/Graphene of Ultrahigh Capacitance as Advanced Flexible Anode for Asymmetric Supercapacitors

Oxygen‐deficient bismuth oxide (r‐Bi₂O₃)/graphene (GN) is designed, fabricated, and demonstrated via a facile solvothermal and subsequent solution reduction method. The ultrafine network bacterial cellulose (BC) as substrate for r‐Bi₂O₃/GN exhibits high flexibility, remarkable tensile strength (55.1 MPa), and large mass loading of 9.8 mg cm^?2. The flexible r‐Bi₂O₃/GN/BC anode delivers appreciable areal capacitance (6675 mF cm^?2 at 1 mA cm^?2) coupled with good rate capability (3750 mF cm^?2 at 50 mA cm^?2). In addition, oxygen vacancies have great influence on the capacitive performance of Bi₂O₃, delivering significantly improved capacitive values than the untreated Bi₂O₃ flexible electrode, and ultrahigh gravimetric capacitance of 1137 F g^?1 (based on the mass of r‐Bi₂O₃) can be obtained, achieving 83% of the theoretical value (1370 F g^?1). Flexible asymmetric supercapacitor is fabricated with r‐Bi₂O₃/GN/BC and Co₃O₄/GN/BC paper as the negative and positive electrodes, respectively. The operation voltage is expanded to 1.6 V, revealing a maximum areal energy density of 0.449 mWh cm^?2 (7.74 mWh cm^?3) and an areal power density of 40 mW cm^?2 (690 mW cm^?3). Therefore, this flexible anode with excellent electrochemical performance and high mechanical properties shows great potential in the field of flexible energy storage devices.     

Capacitively Coupled Hybrid Ion Gel and Carbon Nanotube Thin‐Film Transistors for Low Voltage Flexible Logic Circuits

The lamination of a high‐capacitance ion gel dielectric layer onto semiconducting carbon nanotube (CNT) thin‐film transistors (TFTs) that are bottom‐gated with a low‐capacitance polymer dielectric layer drastically reduces the operating voltage of the devices resulting from the capacitive coupling effect between the two dielectric layers sandwiching the CNT channel. As the CNT channel has a network structure, only a compact area of ion gel is required to make the capacitive coupling effect viable, unlike the planar channels of previously reported transistors that required a substantially larger area of ion gel dielectric layer to induce the coupling effect. The capacitively coupled CNT TFTs possess superlative electrical characteristics such as high carrier mobilities (42.0 cm² (Vs)^?1 for holes and 59.1 cm² (Vs)^?1 for electrons), steep subthreshold swings (160 mV dec^?1 for holes and 100 mV dec^?1 for electrons), and low gate leakage currents (<1 nA). These devices can be further integrated to form complex logic circuits on flexible substrates with high mechanical resilience. The layered geometry of the device coupled with scalable solution‐based fabrication has significant potential for large‐scale flexible electronics.     

On the Relation between Morphology and FET Mobility of Poly(3‐alkylthiophene)s at the Polymer/SiO2 and Polymer/Air Interface

The influence of the interface of the dielectric SiO₂ on the performance of bottom‐contact, bottom‐gate poly(3‐alkylthiophene) (P3AT) field‐effect transistors (FETs) is investigated. In particular, the operation of transistors where the active polythiophene layer is directly spin‐coated from chlorobenzene (CB) onto the bare SiO₂ dielectric is compared to those where the active layer is first spin‐coated then laminated via a wet transfer process such that the film/air interface of this film contacts the SiO₂ surface. While an apparent alkyl side‐chain length dependent mobility is observed for films directly spin‐coated onto the SiO₂ dielectric (with mobilities of ≈10^?3 cm² V^?1 s^?1 or less) for laminated films mobilities of 0.14 ± 0.03 cm² V^?1 s^?1 independent of alkyl chain length are recorded. Surface‐sensitive near edge X‐ray absorption fine structure (NEXAFS) spectroscopy measurements indicate a strong out‐of‐plane orientation of the polymer backbone at the original air/film interface while much lower average tilt angles of the polymer backbone are observed at the SiO₂/film interface. A comparison with NEXAFS on crystalline P3AT nanofibers, as well as molecular mechanics and electronic structure calculations on ideal P3AT crystals suggest a close to crystalline polymer organization at the P3AT/air interface of films from CB. These results emphasize the negative influence of wrongly oriented polymer on charge carrier mobility and highlight the potential of the polymer/air interface in achieving excellent “out‐of‐plane” orientation and high FET mobilities.     

DyeIonogels: Proton‐Responsive Ionogels Based on a Dye‐Ionic Liquid Exhibiting Reversible Color Change

Transparent, ion‐conducting, and flexible ionogels based on the room temperature ionic liquid (IL) 1‐butyl‐3‐methylimidazolium bis(trifluoromethane sulfonyl)imide [Bmim][N(Tf)₂], the dye‐IL (DIL) 1‐butyl‐3‐methylimidazolium methyl orange [Bmim][MO], and poly(methylmethacrylate) (PMMA) are prepared. Upon IL incorporation the thermal stability of the PMMA matrix significantly increases from 220 to 280 °C. The ionogels have a relatively high ionic conductivity of 10^?4 S cm^?1 at 373 K. Most importantly, the ionogels exhibit a strong and reversible color change when exposed to aqueous or organic solutions containing protons or hydroxide ions. The resulting material is thus a prototype of soft multifunctional matter featuring ionic conductivity, easy processability, response to changes in the environment, and a strong readout signal, the color change, that could be used in optical data storage or environmental sensing.     

Knittable and Washable Multifunctional MXene‐Coated Cellulose Yarns

Textile‐based electronics enable the next generation of wearable devices, which have the potential to transform the architecture of consumer electronics. Highly conductive yarns that can be manufactured using industrial‐scale processing and be washed like everyday yarns are needed to fulfill the promise and rapid growth of the smart textile industry. By coating cellulose yarns with Ti₃C₂T_x MXene, highly conductive and electroactive yarns are produced, which can be knitted into textiles using an industrial knitting machine. It is shown that yarns with MXene loading of ≈77 wt% (≈2.2 mg cm^?1) have conductivity of up to 440 S cm^?1. After washing for 45 cycles at temperatures ranging from 30 to 80 °C, MXene‐coated cotton yarns exhibit a minimal increase in resistance while maintaining constant MXene loading. The MXene‐coated cotton yarn electrode offers a specific capacitance of 759.5 mF cm^?1 at 2 mV s^?1. A fully knitted textile‐based capacitive pressure sensor is also prepared, which offers high sensitivity (gauge factor of ≈6.02), wide sensing range of up to ≈20% compression, and excellent cycling stability (2000 cycles at ≈14% compression strain). This work provides new and practical insights toward the development of platform technology that can integrate MXene in cellulose‐based yarns for textile‐based devices.     

Fully Transparent p‐MoTe2 2D Transistors Using Ultrathin MoOx/Pt Contact Media for Indium‐Tin‐Oxide Source/Drain

Since transition metal dichalcogenide (TMD) semiconductors are found as 2D van der Waals materials with a discrete energy bandgap, many 2D‐like thin field effect transistors (FETs) and PN diodes are reported as prototype electrical and optoelectronic devices. As a potential application of display electronics, transparent 2D FET devices are also reported recently. Such transparent 2D FETs are very few in report, yet no p‐type channel 2D‐like FETs are seen. Here, 2D‐like thin transparent p‐channel MoTe₂ FETs with oxygen (O₂) plasma‐induced MoO_x/Pt/indium‐tin‐oxide (ITO) contact are reported for the first time. For source/drain contact, 60 s short O₂ plasma and ultrathin Pt‐deposition processes on MoTe₂ surface are sequentially introduced before ITO thin film deposition and patterning. As a result, almost transparent 2D FETs are obtained with a decent mobility of ≈5 cm² V^?1 s^?1, a high ON/OFF current ratio of ≈10⁵, and 70% transmittance. In particular, for normal MoTe₂ FETs without ITO, O₂ plasma process greatly improves the hole injection efficiency and device mobility (≈60 cm² V^?1 s^?1), introducing ultrathin MoO_x between Pt source/drain and MoTe₂. As a final device application, a photovoltaic current modulator, where the transparent FET stably operates as gated by photovoltaic effects, is integrated.     

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.     

Printed Sub‐2 V Gel‐Electrolyte‐Gated Polymer Transistors and Circuits

The fabrication and characterization of printed ion‐gel‐gated poly(3‐hexylthiophene) (P3HT) transistors and integrated circuits is reported, with emphasis on demonstrating both function and performance at supply voltages below 2 V. The key to achieving fast sub‐2 V operation is an unusual gel electrolyte based on an ionic liquid and a gelating block copolymer. This gel electrolyte serves as the gate dielectric and has both a short polarization response time (<1 ms) and a large specific capacitance (>10 µF cm^?2), which leads simultaneously to high output conductance (>2 mS mm^?1), low threshold voltage (<1 V) and high inverter switching frequencies (1–10 kHz). Aerosol‐jet‐printed inverters, ring oscillators, NAND gates, and flip‐flop circuits are demonstrated. The five‐stage ring oscillator operates at frequencies up to 150 Hz, corresponding to a propagation delay of 0.7 ms per stage. These printed gel electrolyte gated circuits compare favorably with other reported printed circuits that often require much larger operating voltages. Materials factors influencing the performance of the devices are discussed.     

Scalable Production of Graphene Inks via Wet‐Jet Milling Exfoliation for Screen‐Printed Micro‐Supercapacitors

The miniaturization of energy storage units is pivotal for the development of next‐generation portable electronic devices. Micro‐supercapacitors (MSCs) hold great potential to work as on‐chip micro‐power sources and energy storage units complementing batteries and energy harvester systems. Scalable production of supercapacitor materials with cost‐effective and high‐throughput processing methods is crucial for the widespread application of MSCs. Here, wet‐jet milling exfoliation of graphite is reported to scale up the production of graphene as a supercapacitor material. The formulation of aqueous/alcohol‐based graphene inks allows metal‐free, flexible MSCs to be screen‐printed. These MSCs exhibit areal capacitance (C_areal) values up to 1.324 mF cm^?2 (5.296 mF cm^?2 for a single electrode), corresponding to an outstanding volumetric capacitance (C_vol) of 0.490 F cm^?3 (1.961 F cm^?3 for a single electrode). The screen‐printed MSCs can operate up to a power density above 20 mW cm^?2 at an energy density of 0.064 µWh cm^?2. The devices exhibit excellent cycling stability over charge–discharge cycling (10 000 cycles), bending cycling (100 cycles at a bending radius of 1 cm) and folding (up to angles of 180°). Moreover, ethylene vinyl acetate‐encapsulated MSCs retain their electrochemical properties after a home‐laundry cycle, providing waterproof and washable properties for prospective application in wearable electronics.     

Flexible and Wire‐Shaped Micro‐Supercapacitor Based on Ni(OH)2‐Nanowire and Ordered Mesoporous Carbon Electrodes

Portable and multifunctional electronic devices are developing in the trend of being small, flexible, roll‐up, and even wearable, which asks us to develop flexible and micro‐sized energy conversion/storage devices. Here, the high performance of a flexible, wire‐shaped, and solid‐state micro‐supercapacitor, which is prepared by twisting a Ni(OH)2‐nanowire fiber‐electrode and an ordered mesoporous carbon fiber‐electrode together with a polymer electrolyte, is demonstrated. This micro‐supercapacitor displays a high specific capacitance of 6.67 mF cm^–1 (or 35.67 mF cm^–2) and a high specific energy density of 0.01 mWh cm^–2 (or 2.16 mWh cm^–3), which are about 10–100 times higher than previous reports. Furthermore, its capacitance retention is 70% over 10 000 cycles, indicating perfect cyclic ability. Two wire‐shaped micro‐supercapacitors (0.6 mm in diameter, ≈3 cm in length) in series can successfully operate a red light‐emitting‐diode, indicating promising practical application. Furthermore, synchrotron radiation X‐ray computed microtomo­graphy technology is employed to investigate inner structure of the micro‐device, confirming its solid‐state characteristic. This micro‐supercapacitor may bring new design opportunities of device configuration for energy‐storage devices in the future wearable electronic area.     

Engineering 3D Ion Transport Channels for Flexible MXene Films with Superior Capacitive Performance

2D MXene materials are of considerable interest for future energy storage. A MXene film could be used as an effective flexible supercapacitor electrode due to its flexibility and, more importantly, its high specific capacitance. However, although it has excellent electronic conductivity, sluggish ionic kinetics within the MXene film becomes a fundamental limitation to the electrochemical performance. To compensate for the relative deficiency, MXene films are frequently reduced to several micrometer dimensions with low mass loading (<1 mg cm^?2), to the point of detriment of areal performance and commercial value. Herein, for the first time, the design of a 3D porous MXene/bacterial cellulose (BC) self‐supporting film is reported for ultrahigh capacitance performance (416 F g^?1, 2084 mF cm^?2) with outstanding mechanical properties and high flexibility, even when the MXene loading reaches 5 mg cm^?2. The highly interconnected MXene/BC network enables both excellent electron and ion transport channel. Additionally, a maximum energy density of 252 µWh cm^?2 is achieved in an asymmetric supercapacitor, higher than that of all ever‐reported MXene‐based supercapacitors. This work exploits a simple route for assembling 2D MXene materials into 3D porous films as state‐of‐the‐art electrodes for high performance energy storage devices.