Design of Hierarchical NiCo@NiCo Layered Double Hydroxide Core–Shell Structured Nanotube Array for High‐Performance Flexible All‐Solid‐State Battery‐Type Supercapacitors

A novel hierarchical nanotube array (NTA) with a massive layered top and discretely separated nanotubes in a core–shell structure, that is, nickel–cobalt metallic core and nickel–cobalt layered double hydroxide shell (Ni?Co@Ni?Co LDH), is grown on carbon fiber cloth (CFC) by template‐assisted electrodeposition for high‐performance supercapacitor application. The synthesized Ni?Co@Ni?Co LDH NTAs/CFC shows high capacitance of 2200 F g^?1 at a current density of 5 A g^?1, while 98.8% of its initial capacitance is retained after 5000 cycles. When the current density is increased from 1 to 20 A g^?1, the capacitance loss is less than 20%, demonstrating excellent rate capability. A highly flexible all‐solid‐state battery‐type supercapacitor is successfully fabricated with Ni?Co LDH NTAs/CFC as the positive electrode and electrospun carbon fibers/CFC as the negative electrode, showing a maximum specific capacitance of 319 F g^?1, a high energy density of 100 W h kg^?1 at 1.5 kW kg^?1, and good cycling stability (98.6% after 3000 cycles). These fascinating electrochemical properties are resulted from the novel structure of electrode materials and synergistic contributions from the two electrodes, showing great potential for energy storage applications.     

Design of Hierarchical Ni?Co@Ni?Co Layered Double Hydroxide Core–Shell Structured Nanotube Array for High‐Performance Flexible All‐Solid‐State Battery‐Type Supercapacitors

A novel hierarchical nanotube array (NTA) with a massive layered top and discretely separated nanotubes in a core–shell structure, that is, nickel–cobalt metallic core and nickel–cobalt layered double hydroxide shell (Ni? Co@Ni? Co LDH), is grown on carbon fiber cloth (CFC) by template‐assisted electrodeposition for high‐performance supercapacitor application. The synthesized Ni? Co@Ni? Co LDH NTAs/CFC shows high capacitance of 2200 F g^?1 at a current density of 5 A g^?1, while 98.8% of its initial capacitance is retained after 5000 cycles. When the current density is increased from 1 to 20 A g^?1, the capacitance loss is less than 20%, demonstrating excellent rate capability. A highly flexible all‐solid‐state battery‐type supercapacitor is successfully fabricated with Ni? Co LDH NTAs/CFC as the positive electrode and electrospun carbon fibers/CFC as the negative electrode, showing a maximum specific capacitance of 319 F g^?1, a high energy density of 100 W h kg^?1 at 1.5 kW kg^?1, and good cycling stability (98.6% after 3000 cycles). These fascinating electrochemical properties are resulted from the novel structure of electrode materials and synergistic contributions from the two electrodes, showing great potential for energy storage applications.     

3D Hierarchical Co3O4 Twin‐Spheres with an Urchin‐Like Structure: Large‐Scale Synthesis,Multistep‐Splitting Growth,and Electrochemical Pseudocapacitors

Novel, 3D hierarchical Co₃O₄ twin‐spheres with an urchin‐like structure are produced successfully on the large scale for the first time by a solvothermal synthesis of cobalt carbonate hydroxide hydrate, Co(CO₃)_0.5(OH)·0.11H₂O, and its subsequent calcination. The morphology of the precursor, which dominates the structure of the final product, evolves from nanorods to sheaf‐like bundles, to flower‐like structures, to dumbbell‐like particles, and eventually to twin‐spheres, accompanying a prolonged reaction time. A multistep‐splitting growth mechanism is proposed to understand the formation of the 3D hierarchical twin‐spheres of the precursor, based on the time effect on the morphologies of the precursor. The 3D hierarchical Co₃O₄ twin‐spheres are further used as electrode materials to fabricate supercapacitors with high specific capacitances of 781, 754, 700, 670, and 611 F g^?1 at current densities of 0.5, 1, 2, 4, and 8 A g^?1, respectively. The devices also show high charge‐discharge reversibility with an efficiency of 97.8% after cycling 1000 times at a current density of 4 A g^?1.     

Multicomponent Hierarchical Cu‐Doped NiCo‐LDH/CuO Double Arrays for Ultralong‐Life Hybrid Fiber Supercapacitor

Fiber supercapacitors have aroused great interest in the field of portable and wearable electronic devices. However, the restrained surface area of fibers and limited reaction kinetics of active materials are unfavorable for performance enhancement. Herein, an efficient multicomponent hierarchical structure is constructed by integrating the Cu‐doped cobalt copper carbonate hydroxide@nickel cobalt layered double hydroxide (CCCH@NiCo‐LDH) core–shell nanowire arrays (NWAs) on Cu fibers with highly conductive Au‐modified CuO nanosheets (CCCH@NiCo‐LDH NWAs@Au–CuO/Cu) via a novel in situ corrosion growth method. This multicomponent hierarchical structure contributes to a large accessible surface area, which results in sufficient permeation of the electrolyte. The Cu dopant could reduce the work function and facilitate fast charge transfer kinetics. Therefore, the effective ion diffusion and electron conduction will facilitate the electrochemical reaction kinetics of the electrode. Benefiting from this unique structure, the electrode delivers a high specific capacitance (1.97 F cm^?2/1237 F g^?1/193.3 mAh g^?1) and cycling stability (90.8% after 30 000 cycles), exhibiting superb performance compared with most oxide‐based fiber electrodes. Furthermore, the hybrid fiber supercapacitor of CCCH@NiCo‐LDH NWAs@Au–CuO/Cu//VN/carbon fibers is fabricated, providing a remarkable maximal energy density of 34.97 Wh kg^?1 and a power density of 13.86 kW kg^?1, exhibiting a great potential in high‐performance fiber‐shape energy‐related systems.     

Novel Core–Shell FeOF/Ni(OH)2 Hierarchical Nanostructure for All‐Solid‐State Flexible Supercapacitors with Enhanced Performance

Well‐controlled core–shell hierarchical nanostructures based on oxyfluoride and hydroxide are for the first time rationally designed and synthesized via a simple solvothermal and chemical precipitation route, in which FeOF nanorod acts as core and porous Ni(OH)₂ nanosheets as shell. When evaluated as electrodes for supercapacitors, a high specific capacitance of 1452 F g^?1 can be obtained at a current density of 1 A g^?1. Even as the current density increases to 10 A g^?1, the core–shell hybrid still reserves a noticeable capacitance of 1060 F g^?1, showing an excellent rate capacity. Furthermore, all‐solid‐state flexible asymmetric supercapacitor based on the FeOF/Ni(OH)₂ hybrid as a positive electrode and activated carbon as a negative electrode shows high power density, high energy density, and long cycling lifespan. The excellent electrochemical performance of the FeOF/Ni(OH)₂ core–shell hybrid is ascribed to the unique microstructure and synergistic effects. FeOF nanorod from FeF₃ by partial substitution of fluorine with oxygen behaves as a low intrinsic resistance, thus facilitating charge transfer processes. While the hierarchical Ni(OH)₂ nanosheets with large surface area provide enough active sites for redox chemical reactions, leading to greatly enhanced electrochemical activity. The well‐controllable oxyfluoride/hydroxide hybrid is inspiring, opening up a new way to design new electrodes for next‐generation all‐solid‐state supercapacitors.     

Nickel–Cobalt Layered Double Hydroxide Nanosheets for High‐performance Supercapacitor Electrode Materials

A facile and novel one‐step method of growing nickel‐cobalt layered double hydroxide (Ni‐Co LDH) hybrid films with ultrathin nanosheets and porous nanostructures on nickel foam is presented using cetyltrimethylammonium bromide as nanostructure growth assisting agent but without any adscititious alkali sources and oxidants. As pseudocapacitors, the as‐obtained Ni‐Co LDH hybrid film‐based electrodes display a significantly enhanced specific capacitance (2682 F g^?1 at 3 A g^?1, based on active materials) and energy density (77.3 Wh kg^?1 at 623 W kg^?1), compared to most previously reported electrodes based on nickel‐cobalt oxides/hydroxides. Moreover, the asymmetric supercapacitor, with the Ni‐Co LDH hybrid film as the positive electrode material and porous freeze‐dried reduced graphene oxide (RGO) as the negative electrode material, exhibits an ultrahigh energy density (188 Wh kg^?1) at an average power density of 1499 W kg^?1 based on the mass of active material, which greatly exceeds the energy densities of most previously reported nickel or cobalt oxide/hydroxide‐based asymmetric supercapacitors.     

3D Micro‐Extrusion of Graphene‐based Active Electrodes: Towards High‐Rate AC Line Filtering Performance Electrochemical Capacitors

A facile one‐step printing process by 3D micro‐extrusion affording binder‐free thermally reduced graphene oxide (TRGO) based electrochemical capacitors (ECs) that display high‐rate performance is presented. Key intermediates are binder‐free TRGO dispersion printing inks with concentrations up to 15 g L^?1. This versatile printing technique enables easy fabrication of EC electrodes, useful in both aqueous and non‐aqueous electrolyte systems. The as‐prepared TRGO material with high specific surface area (SSA) of 593 m² g^?1 and good electrical conductivity of ≈16 S cm^?1 exhibits impressive charge storage performances. At 100 and 120 Hz, ECs fabricated with TRGO show time constants of 2.5 ms and 2.3 ms respectively. Very high capacitance values are derived at both frequencies ranging from 3.55 mF cm^?2 to 1.76 mF cm^?2. Additionally, these TRGO electrodes can be charged and discharged at very high voltage scan rates up to 15 V s^?1 yielding 4 F cm^?3 with 50% capacitance retention. Electrochemical performance of TRGO electrodes in electrolyte containing tetraethyl ammonium tetrafluoroborate and acetonitrile (TEABF4‐ACN) yields high energy density of 4.43 mWh cm^?3 and power density up to 42.74 kW cm^?3, which is very promising for AC line filtering application and could potentially substitute state of the art electrolytic capacitor technology.     

Hierarchical Composite Electrodes of Nickel Oxide Nanoflake 3D Graphene for High‐Performance Pseudocapacitors

NiO nanoflakes are created with a simple hydrothermal method on 3D (three‐dimensional) graphene scaffolds grown on Ni foams by microwave plasma enhanced chemical vapor deposition (MPCVD). Such as‐grown NiO‐3D graphene hierarchical composites are then applied as monolithic electrodes for a pseudo‐supercapacitor application without needing binders or metal‐based current collectors. Electrochemical measurements impart that the hierarchical NiO‐3D graphene composite delivers a high specific capacitance of ≈1829 F g^?1 at a current density of 3 A g^?1 (the theoretical capacitance of NiO is 2584 F g^?1). Furthermore, a full‐cell is realized with an energy density of 138 Wh kg^?1 at a power density of 5.25 kW kg^?1, which is much superior to commercial ones as well as reported devices in asymmetric capacitors of NiO. More attractively, this asymmetric supercapacitor exhibits capacitance retention of 85% after 5000 cycles relative to the initial value of the 1^st cycle.     

Oxygen‐Deficient Homo‐Interface toward Exciting Boost of Pseudocapacitance

Pseudocapacitors hold great promise as charge storage systems that combine battery‐level energy density and capacitor‐level power density. The utilization of pseudocapacitive material, however, is usually restricted to the surface due to poor electrode kinetics, leading to less accessible charge storage sites and limited capacitance. Here, tin oxide is successfully endowed with outstanding pseudocapacitance and fast electrode kinetics in a negative potential window by engineering oxygen‐deficient homo‐interfaces. The as‐prepared SnO_2?x@SnO_2?x electrode yields a specific capacitance of 376.6 F g^?1 at the current density of 2.5 A g^?1 and retains 327 F g^?1 at a high current density of 80 A g^?1. The theoretical calculation reveals that the oxygen defects are more favorable at homo‐interfaces than at the surface due to the lower defect formation energy. Meanwhile, as compared with the surface, the homo‐interface possesses more stable Li⁺ storage sites that are readily accessed by Li⁺ due to the occurrence of oxygen vacancies, enabling outstanding pseudocapacitance as well as high rate capability. This oxygen‐deficient homo‐interface design opens up new opportunities to develop high‐energy and power pseudocapacitors.     

Ultrathin Nickel–Cobalt Phosphate 2D Nanosheets for Electrochemical Energy Storage under Aqueous/Solid‐State Electrolyte

2D materials are ideal for constructing flexible electrochemical energy storage devices due to their great advantages of flexibility, thinness, and transparency. Here, a simple one‐step hydrothermal process is proposed for the synthesis of nickel–cobalt phosphate 2D nanosheets, and the structural influence on the pseudocapacitive performance of the obtained nickel–cobalt phosphate is investigated via electrochemical measurement. It is found that the ultrathin nickel–cobalt phosphate 2D nanosheets with an Ni/Co ratio of 4:5 show the best electrochemical performance for energy storage, and the maximum specific capacitance up to 1132.5 F g^?1. More importantly, an aqueous and solid‐state flexible electrochemical energy storage device has been assembled. The aqueous device shows a high energy density of 32.5 Wh kg^?1 at a power density of 0.6 kW kg^?1, and the solid‐state device shows a high energy density of 35.8 Wh kg^?1 at a power density of 0.7 kW kg^?1. These excellent performances confirm that the nickel–cobalt phosphate 2D nanosheets are promising materials for applications in electrochemical energy storage devices.     

A Low‐Cost,Self‐Standing NiCo2O4@CNT/CNT Multilayer Electrode for Flexible Asymmetric Solid‐State Supercapacitors

The demand for a new generation of flexible, portable, and high‐capacity power sources increases rapidly with the development of advanced wearable electronic devices. Here we report a simple process for large‐scale fabrication of self‐standing composite film electrodes composed of NiCo₂O₄@carbon nanotube (CNT) for supercapacitors. Among all composite electrodes prepared, the one fired in air displays the best electrochemical behavior, achieving a specific capacitance of 1,590 F g^?1 at 0.5 A g^?1 while maintaining excellent stability. The NiCo₂O₄@CNT/CNT film electrodes are fabricated via stacking NiCo₂O₄@CNT and CNT alternately through vacuum filtration. Lightweight, flexible, and self‐standing film electrodes (≈24.3 µm thick) exhibit high volumetric capacitance of 873 F cm^?3 (with an areal mass of 2.5 mg cm^?2) at 0.5 A g^?1. An all‐solid‐state asymmetric supercapacitor consists of a composite film electrode and a treated carbon cloth electrode has not only high energy density (≈27.6 Wh kg^?1) at 0.55 kW kg^?1 (including the weight of the two electrodes) but also excellent cycling stability (retaining ≈95% of the initial capacitance after 5000 cycles), demonstrating the potential for practical application in wearable devices.     

Flexible Solid‐State Supercapacitors with Enhanced Performance from Hierarchically Graphene Nanocomposite Electrodes and Ionic Liquid Incorporated Gel Polymer Electrolyte

High energy density, durability, and flexibility of supercapacitors are required urgently for the next generation of wearable and portable electronic devices. Herein, a novel strategy is introduced to boost the energy density of flexible soild‐state supercapacitors via rational design of hierarchically graphene nanocomposite (GNC) electrode material and employing an ionic liquid gel polymer electrolyte. The hierarchical graphene nanocomposite consisting of graphene and polyaniline‐derived carbon is synthesized as an electrode material via a scalable process. The meso/microporous graphene nanocomposites exhibit a high specific capacitance of 176 F g^?1 at 0.5 A g^?1 in the ionic liquid 1‐ethyl‐3‐methylimidazolium tetrafluoroborate (EMIBF₄) with a wide voltage window of 3.5 V, good rate capability of 80.7% in the range of 0.5–10 A g^?1 and excellent stability over 10 000 cycles, which is attributed to the superior conductivity (7246 S m^?1), and quite large specific surface area (2416 m² g^?1) as well as hierarchical meso/micropores distribution of the electrode materials. Furthermore, flexible solid‐state supercapacitor devices based on the GNC electrodes and gel polymer electrolyte film are assembled, which offer high specific capacitance of 180 F g^?1 at 1 A g^?1, large energy density of 75 Wh Kg^?1, and remarkable flexible performance under consecutive bending conditions.     

Flexible Stable Solid‐State Al‐Ion Batteries

Rechargeable aluminum‐ion batteries (AIBs) are regarded as promising candidates for post‐lithium energy storage systems (ESSs). For addressing the critical issues in the current liquid AIB systems, here a flexible solid‐state AIB is established using a gel‐polymer electrolyte for achieving robust electrode–electrolyte interfaces. Different from utilization of solid‐state systems for alleviating the safety issues and enhancing energy density in lithium‐ion batteries, employment of polymeric electrolytes mainly focuses on addressing the essential problems in the liquid AIBs, including unstable internal interfaces induced by mechanical deformation and production of gases as well as unfavorable separators. Particularly, such gel electrolyte enables the solid‐state AIBs to present an ultra‐fast charge capability within 10 s at current density of 600 mA g^?1. Meanwhile, an impressive specific capacity ≈120 mA h g^?1 is obtained at current density of 60 mA g^?1, approaching the theoretical limit of graphite‐based AIBs. In addition to the well‐retained electrochemical performance below the ice point, the solid‐state AIBs also hold great stability and safety under various critical conditions. The results suggest that such new prototype of solid‐state AIBs with robust electrode–electrolyte interfaces promises a novel strategy for fabricating stable and safe flexible ESSs.     

Dual Electrostatic Assembly of Graphene Encapsulated Nanosheet‐Assembled ZnO‐Mn‐C Hollow Microspheres as a Lithium Ion Battery Anode

Graphene encapsulated nanosheet‐assembled ZnO‐Mn‐C hierarchical hollow microspheres are produced through a simple yet effective dual electrostatic assembly strategy, followed by a heating treatment in inert atmosphere. The modification of graphene sheets, metal Mn, and in situ carbon leads to form 3D interconnected conductive framework as electron highways. The hollow structure and the open configuration of hierarchical microspheres guarantee good structural stability and rapid ionic transport. More importantly, according to the density functional theory calculations, the oxygen vacancies in the hierarchical microspheres would cause an imbalanced charge distribution and thus the formation of local in‐plane electric fields around oxygen vacancy sites, which is beneficial for the ionic/electronic transport during cycling. Due to this multiscale coordinated design, the as‐fabricated graphene encapsulated nanosheet‐assembled ZnO‐Mn‐C hierarchical hollow microspheres demonstrate good lithium storage properties in terms of high reversible capacity (1094 mA h g^?1 at 100 mA g^?1), outstanding high‐rate long‐term cycling stability (843 mA h g^?1 after 1000 cycles at 2000 mA g^?1), and remarkable rate capability (422 mA h g^?1 after total 1600 cycles at 5000 mA g^?1).     

Hierarchical Ni–Co Hydroxide Petals on Mechanically Robust Graphene Petal Foam for High‐Energy Asymmetric Supercapacitors

A hierarchical structure consisting of Ni–Co hydroxide nanopetals (NCHPs) grown on a thin free‐standing graphene petal foam (GPF) has been designed and fabricated by a two‐step process for pseudocapacitive electrode applications. The mechanical behavior of GPFs has been, for the first time to our knowledge, quantitatively measured from in situ scanning electron microscope characterization of the petal foams during in‐plane compression and bending processes. The Young's modulus of a typical GPF is 3.42 GPa, indicating its outstanding mechanical robustness as a nanotemplate. The GPF/NCHP electrodes exhibit volumetric capacitances as high as 765 F cm^?3, equivalent to an areal capacitance of 15.3 F cm^?2 and high rate capability. To assess practical functionality, two‐terminal asymmetric solid‐state supercapacitors with 3D GPF/NCHPs as positive electrodes are fabricated and shown to exhibit outstanding energy and power densities, with maximum average energy density of ≈10 mWh cm^?3 and maximum power density of ≈3 W cm^?3, high rate capability (a capacitance retention of ≈60% at 100 mA cm^?2), and excellent long‐term cyclic stability (full capacitance retention over 15 000 cycles).     

Ultrahigh‐Performance Pseudocapacitor Electrodes Based on Transition Metal Phosphide Nanosheets Array via Phosphorization: A General and Effective Approach

In this study, a general and effective phosphorization strategy is successfully demonstrated to enhance supercapacitor performance of various transition metals oxide or hydroxide, such as Ni(OH)₂, Co(OH)₂, MnO₂, and Fe₂O₃. For example, a 3D networked Ni₂P nanosheets array via a facile phosphorization reaction of Ni(OH)₂ nanosheets is grown on the surface of a Ni foam. The Ni foam‐supported Ni₂P nanosheet (Ni₂P NS/NF) electrode shows a remarkable specific capacitance of 2141 F g^?1 at a scan rate of 50 mV s^?1 and remains as high as 1109 F g^?1 even at the current density of 83.3 A g^?1. The specific capacitance is much larger than those of Ni(OH)₂ NS/NF (747 F g^?1 at 50 mV s^?1). Furthermore, the electrode retains a high specific capacitance of 1437 F g^?1 even after 5000 cycles at a current density of 10 A g^?1, in sharp contrast with only 403 F g^?1 of Ni(OH)₂ NS/NF at the same current density. The similar enhanced performance is observed for Ni₂P powder, which eliminates the influence of nickel foam. The enhanced supercapacitor performances are attributed to the 3D porous nanosheets network, enhanced conductivity, and two active components of Ni²⁺ and P^δ? with rich valences of Ni₂P.     

3D Carbon Nanotube Network Bridged Hetero‐Structured Ni‐Fe‐S Nanocubes toward High‐Performance Lithium,Sodium, and Potassium Storage

Lithium‐ion, sodium‐ion, and potassium‐ion batteries have captured tremendous attention in power supplies for various electric vehicles and portable electronic devices. However, their practical applications are severely limited by factors such as poor rate capability, fast capacity decay, sluggish charge storage dynamics, and low reversibility. Herein, hetero‐structured bimetallic sulfide (NiS/FeS) encapsulated in N‐doped porous carbon cubes interconnected with CNTs (Ni‐Fe‐S‐CNT) are prepared through a convenient co‐precipitation and post‐heat treatment sulfurization technique of the corresponding Prussian‐blue analogue nanocage precursor. This special 3D hierarchical structure can offer a stable interconnect and conductive network and shorten the diffusion path of ions, thereby greatly enhancing the mobility efficiency of alkali (Li, Na, K) ions in electrode materials. The Ni‐Fe‐S‐CNT nanocomposite maintains a charge capacity of 1535 mAh g^?1 at 0.2 A g^?1 for lithium ion batteries, 431 mAh g^?1 at 0.1 A g^?1 for sodium ion batteries, and 181 mAh g^?1 at 0.1 A g^?1 for potassium‐ion batteries, respectively. The high performance is mainly attributed to the 3D hierarchically high‐conductivity network architecture, in which the hetero‐structured FeS/NiS nanocubes provide fast Li⁺/Na⁺/K⁺ insertion/extraction and reduced ion diffusion paths, and the distinctive 3D networks maintain the electrical contact and guarantee the structural integrity.     

Homologous CoP/NiCoP Heterostructure on N‐Doped Carbon for Highly Efficient and pH‐Universal Hydrogen Evolution Electrocatalysis

Hydrogen evolution electrocatalysts can achieve sustainable hydrogen production via electrocatalytic water splitting; however, designing highly active and stable noble‐metal‐free hydrogen evolution electrocatalysts that perform as efficiently as Pt catalysts over a wide pH range is a challenging task. Herein, a new 2D cobalt phosphide/nickelcobalt phosphide (CoP/NiCoP) hybrid nanosheet network is proposed, supported on an N‐doped carbon (NC) matrix as a highly efficient and durable pH‐universal hydrogen evolution reaction (HER) electrocatalyst. It is derived from topological transformation of corresponding layer double hydroxides and graphitic carbon nitride. This 2D CoP/NiCoP/NC catalyst exhibits versatile HER electroactivity with very low overpotentials of 75, 60, and 123 mV in 1 m KOH, 0.5 m H₂SO₄, and 1 m PBS electrolytes, respectively, delivering a current density of 10 mA cm^?2 for HER. Such impressive HER performance of the hybrid electrocatalyst is mainly attributed to the collective effects of electronic structure engineering, strong interfacial coupling between CoP and NiCoP in heterojunction, an enlarged surface area/exposed catalytic active sites due to the 2D morphology, and conductive NC support. This method is believed to provide a basis for the development of efficient 2D electrode materials with various electrochemical applications.     

All‐Cellulose‐Based Quasi‐Solid‐State Sodium‐Ion Hybrid Capacitors Enabled by Structural Hierarchy

Na‐ion hybrid capacitors consisting of battery‐type anodes and capacitor‐style cathodes are attracting increasing attention on account of the abundance of sodium‐based resources as well as the potential to bridge the gap between batteries (high energy) and supercapacitors (high power). Herein, hierarchically structured carbon materials inspired by multiscale building units of cellulose from nature are assembled with cellulose‐based gel electrolytes into Na‐ion capacitors. Nonporous hard carbon anodes are obtained through the direct thermal pyrolysis of cellulose nanocrystals. Nitrogen‐doped carbon cathodes with a coral‐like hierarchically porous architecture are prepared via hydrothermal carbonization and activation of cellulose microfibrils. The reversible charge capacity of the anode is 256.9 mAh g^?1 when operating at 0.1 A g^?1 from 0 to 1.5 V versus Na⁺/Na, and the discharge capacitance of cathodes tested within 1.5 to 4.2 V versus Na⁺/Na is 212.4 F g^?1 at 0.1 A g^?1. Utilizing Na⁺ and ClO₄^? as charge carriers, the energy density of the full Na‐ion capacitor with two asymmetric carbon electrodes can reach 181 Wh kg^?1 at 250 W kg^?1, which is one of the highest energy devices reported until now. Combined with macrocellulose‐based gel electrolytes, all‐cellulose‐based quasi‐solid‐state devices are demonstrated possessing additional advantages in terms of overall sustainability.     

3D Structural Strengthening Urchin‐Like Cu(OH)2‐Based Symmetric Supercapacitors with Adjustable Capacitance

Developing advanced three‐dimensional (3D) structural supercapacitors with both high capacity and good mechanical strength remains challenging. Herein, a novel road is reported for fabricating 3D structural strengthening supercapacitors with adjustable capacitance based on urchin‐like Cu(OH)₂ lattice electrodes by bridging 3D printing technology with a facile electroless plating and electro‐oxidation method. As revealed by the results, the 3D‐printed octet‐truss lattice electrode features a high volumetric capacitance of 8.46 F cm^?3 at 5 mA cm^?3 and superior retention capacity of 68% at 1 A cm^?3. The assembled symmetric supercapacitor with a 70.2% capacitance retention after 5000 cycles possesses a 12.8 Wh kg^?1 energy density at a power density of 2110.2 W kg^?1. Additionally, the resulting 3D structural strengthening electrodes can achieve both high compressive strength and toughness of 30 MPa and 264.7 kJ m^?3, respectively, demonstrating high mechanical strength and excellent antideformation capacity. With the proposed strategy, the electrochemical and mechanical properties of these novel 3D structural strengthened supercapacitors can be easily tuned by a simple spatial framework design, fulfilling the increasing demand of highly customized power sources in the space‐constrained microelectronics and astronautic electronics industries.