Surface Pseudocapacitive Mechanism of Molybdenum Phosphide for High‐Energy and High‐Power Sodium‐Ion Capacitors

Sodium‐based energy storage technologies are potential candidates for large‐scale grid applications owing to the earth abundance and low cost of sodium resources. Transition metal phosphides, e.g. MoP, are promising anode materials for sodium‐ion storage, while their detailed reaction mechanisms remain largely unexplored. Herein, the sodium‐ion storage mechanism of hexagonal MoP is systematically investigated through experimental characterizations, density functional theory calculations, and kinetics analysis. Briefly, it is found that the naturally covered surface amorphous molybdenum oxides layers on the MoP grains undergo a faradaic redox reaction during sodiation and desodiation, while the inner crystalline MoP remains unchanged. Remarkably, the MoP anode exhibits a pseudocapacitive‐dominated behavior, enabling the high‐rate sodium storage performance. By coupling the pseudocapacitive anode with a high‐rate‐battery‐type Na₃V₂O₂(PO₄)₂F@rGO cathode, a novel sodium‐ion full cell delivers a high energy density of 157 Wh kg^?1 at 97 W kg^?1 and even 52 Wh kg^?1 at 9316 W kg^?1. These findings present the deep understanding of the sodium‐ion storage mechanism in hexagonal MoP and offer a potential route for the design of high‐rate sodium‐ion storage materials and devices.     

High‐Energy Density Li‐Ion Capacitor with Layered SnS2/Reduced Graphene Oxide Anode and BCN Nanosheet Cathode

Lithium‐ion capacitors (LICs) with capacitor‐type cathodes and battery‐type anodes are considered a promising next‐generation advanced energy storages system that meet the requirements of high energy density and power density. However, the mismatch of charge‐storage capacity and electrode kinetics between positive and negative electrodes remains a challenge. Herein, layered SnS₂/reduced graphene oxide (RGO) nanocomposites are developed for negative electrodes and a 2D B/N codoped carbon (BCN) nanosheet is designed for the positive electrode. The SnS₂/RGO derived from SnS₂‐bonded RGO of high conductivity exhibits a capacity of 1198 mA h g^?1 at 100 mA g^?1. Boron and nitrogen atoms in BCN are found to promote adsorption of anions, which enhance the pseudocapacitive contribution as well as expanding the voltage of LICs. A quantitative kinetics analysis indicates that the SnS₂/RGO electrodes with a dominating capacitive mechanism and a diminished intercalation process, benefit the kinetic balance between the two electrodes. With this particular structure, the LIC is able to operate at the highest operating voltage for these devices recorded to date (4.5 V), exhibiting an energy density of 149.5 W h kg^?1, a power density of 35 kW kg^?1, and a capacity retention ratio of 90% after 10 000 cycles.     

Mesoporous MoS2 as a Transition Metal Dichalcogenide Exhibiting Pseudocapacitive Li and Na‐Ion Charge Storage

The ion insertion properties of MoS₂ continue to be of widespread interest for energy storage. While much of the current work on MoS₂ has been focused on the high capacity four‐electron reduction reaction, this process is prone to poor reversibility. Traditional ion intercalation reactions are highlighted and it is demonstrated that ordered mesoporous thin films of MoS₂ can be utilized as a pseudocapacitive energy storage material with a specific capacity of 173 mAh g^?1 for Li‐ions and 118 mAh g^?1 for Na‐ions at 1 mV s^?1. Utilizing synchrotron grazing incidence X‐ray diffraction techniques, fast electrochemical kinetics are correlated with the ordered porous structure and with an iso‐oriented crystal structure. When Li‐ions are utilized, the material can be charged and discharged in 20 seconds while still achieving a specific capacity of 140 mAh g^?1. Moreover, the nanoscale architecture of mesoporous MoS₂ retains this level of lithium capacity for 10 000 cycles. A detailed electrochemical kinetic analysis indicates that energy storage for both ions in MoS₂ is due to a pseudocapacitive mechanism.     

Dial the Mechanism Switch of VN from Conversion to Intercalation toward Long Cycling Sodium‐Ion Battery

Transition metal nitrides are promising energy storage materials in regard to good metallic conductivity and high theoretical specific capacity, but their cycling stability is impeded by the huge volume change caused by the conversion reaction mechanism. Here, a simple strategy to produce an intercalation pseudocapacitive‐type vanadium nitride (VN) by one‐step ammonification of V₂C MXene for sodium‐ion batteries is reported. Profiting from a distinctive layered structure pillared by Al atoms in the layer spacing, it delivers a high capacity of 372 mA h g^?1 at 50 mA g^?1 and a desirable rate performance. More importantly, it shows remarkably long cycling stability over 7500 cycles without capacity attenuation at 500 mA g^?1. As expected, it is found that the intercalation pseudocapacitance plays an important role in the excellent performance, by using in situ X‐ray diffraction and ex situ X‐ray absorption structure characterization. Even more remarkable, are the high energy and power density of the sodium‐ion capacitor after coupling with a carbon‐based cathode. The hybrid device possesses an energy density of 78.43 Wh kg^?1 at power density of 260 W kg^?1. The results clearly show that such a unique‐layered VN with outstanding Na storage capability is an excellent new material for energy storage systems.     

Toward a High‐Performance All‐Plastic Full Battery with a'Single Organic Polymer as Both Cathode and Anode

The design and fabrication of high‐performance all‐plastic batteries is essentially important to achieve future flexible electronics. A major challenge in this field is the lack of stable and reliable soft organic electrodes with satisfactory performance. Here, a novel all‐plastic‐electrode based Li‐ion battery with a single flexible bi‐functional ladderized heterocyclic poly(quinone), (C₆O₂S₂)_n, as both cathode and anode is demonstrated. Benefiting from its unique ladder‐like quinone and dithioether structure, the as‐prepared polymer cathode shows a high energy density of 624 Wh kg^?1 (vs lithium anode) and a stable battery life of 1000 cycles. Moreover, the as‐fabricated symmetric full‐battery delivers a large capacity of 249 mAh g^?1 (at 20 mA g^?1), a good capacity retention of 119 mAh g^?1 after 250 cycles (at 1.0 A g^?1) and a noteworthy energy density up to 276 Wh kg^?1. The superior performance of poly(2,3‐dithiino‐1,4‐benzoquinone)‐based electrode rivals most of the state‐of‐the‐art demonstrations on organic‐based metal‐ion shuttling batteries. The study provides an effective strategy to develop stable bi‐functional electrode materials toward the next‐generation of high performance all‐plastic batteries.     

Paper‐Based Energy‐Storage Devices Comprising Carbon Fiber‐Reinforced Polypyrrole‐Cladophora Nanocellulose Composite Electrodes

Composites of polypyrrole (PPy) and Cladophora nanocellulose, reinforced with 8 μm‐thick chopped carbon filaments, can be used as electrode materials to obtain paper‐based energy‐storage devices with unprecedented performance at high charge and discharge rates. Charge capacities of more than 200 C g^?1 (PPy) are obtained for paper‐based electrodes at potential scan rates as high as 500 mV s^?1, whereas cell capacitances of ～60–70 F g^?1 (PPy) are reached for symmetric supercapacitor cells with capacitances up to 3.0 F (i.e.,0.48 F cm^?2) when charged to 0.6 V using current densities as high as 31 A g^?1 based on the PPy weight (i.e., 99 mA cm^?2). Energy and power densities of 1.75 Wh kg^?1 and 2.7 kW kg^?1, respectively, are obtained when normalized with respect to twice the PPy weight of the smaller electrode. No loss in cell capacitance is seen during charging/discharging at 7.7 A g^?1 (PPy) over 1500 cycles. It is proposed that the nonelectroactive carbon filaments decrease the contact resistances and the resistance of the reduced PPy composite. The present straightforward approach represents significant progress in the development of low‐cost and environmentally friendly paper‐based energy‐storage devices for high‐power applications.     

Black Phosphorus Quantum Dot/Ti3C2 MXene Nanosheet Composites for Efficient Electrochemical Lithium/Sodium‐Ion Storage

The exploration of new and efficient energy storage mechanisms through nanostructured electrode design is crucial for the development of high‐performance rechargeable batteries. Herein, black phosphorus quantum dots (BPQDs) and Ti₃C₂ nanosheets (TNSs) are employed as battery and pseudocapacitive components, respectively, to construct BPQD/TNS composite anodes with a novel battery‐capacitive dual‐model energy storage (DMES) mechanism for lithium‐ion and sodium‐ion batteries. Specifically, as a battery‐type component, BPQDs anchored on the TNSs are endowed with improved conductivity and relieved stress upon cycling, enabling a high‐capacity and stable energy storage. Meanwhile, the pseudocapacitive TNS component with further atomic charge polarization induced by P? O? Ti interfacial bonds between the two components allows enhanced charge adsorption and efficient interfacial electron transfer, contributing a higher pseudocapacitive value and fast energy storage. The DMES mechanism is evidenced by substantial characterizations of X‐ray photoelectron spectroscopy and X‐ray absorption fine structure spectroscopy, density functional theory calculations, and kinetics analyses. Consequently, the composite electrode exhibits superior battery performance, especially for lithium storage, such as high capacity (910 mAh g^?1 at 100 mA g^?1), long cycling stability (2400 cycles with a capacity retention over 100%), and high rate capability, representing the best comprehensive battery performance in BP‐based anodes to date.     

Graphitic Petal Electrodes for All‐Solid‐State Flexible Supercapacitors

The charge storage characteristics of a composite nanoarchitecture with a highly functional 3D morphology are reported. The electrodes are formed by the electropolymerization of aniline monomers into a nanometer‐thick polyaniline (PANI) film that conformally coats graphitic petals (GPs) grown by microwave plasma chemical vapor deposition (MPCVD) on conductive carbon cloth (CC). The hybrid CC/GPs/PANI electrodes yield results near the theoretical maximum capacitance for PANI of 2000 F g^?1 (based on PANI mass) and a large area‐normalized specific capacitance of ≈2.6 F cm^?2 (equivalent to a volumetric capacitance of ≈230 F cm^?3) at a low current density of 1 A g^?1 (based on PANI mass). The specific capacitances remain above 1200 F g^?1 (based on PANI mass) for currents up to 100 A g^?1 with correspondingly high area‐normalized values. The hybrid electrodes also exhibit a high rate capability with an energy density of 110 Wh kg^?1 and a maximum power density of 265 kW kg^?1 at a current density of 100 A g^?1. Long‐term cyclic stability is good (≈7% loss of initial capacitance after 2000 cycles), with coulombic efficiencies >99%. Moreover, prototype all‐solid‐state flexible supercapacitors fabricated from these hybrid electrodes exhibit excellent energy storage performance.     

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).     

Designing the Charge Storage Properties of Li‐Exchanged Sodium Vanadium Fluorophosphate for Powering Implantable Biomedical Devices

The growing demand for bioelectronics has generated widespread interest in implantable energy storage. These implantable bioelectronic devices, powered by a complementary battery/capacitor system, have faced difficulty in miniaturization without compromising their functionality. This paper reports on the development of a promising high‐rate cathode material for implantable power sources based on Li‐exchanged Na_1.5VOPO₄F_0.5 anchored on reduced graphene oxide (LNVOPF‐rGO). LNVOPF is unique in that it offers dual charge storage mechanisms, which enable it to exhibit mixed battery/capacitor electrochemical behavior. In this work, electrochemical Li‐ion exchange of the LNVOPF structure is characterized by operando X‐ray diffraction. Through designed nanostructuring, the charge storage kinetics of LNVOPF are improved, as reflected in the stored capacity of 107 mAh g^?1 at 20C. A practical full cell device composed of LNVOPF and T‐Nb₂O₅, which serves as a pseudocapacitive anode, is fabricated to demonstrate not only high energy/power density storage (100 Wh kg^?1 at 4000 W kg^?1) but also reliable pulse capability and biocompatibility, a desirable combination for applications in biostimulating devices. This work underscores the potential of miniaturizing biomedical devices by replacing a conventional battery/capacitor couple with a single power source.     

Mulberry Paper‐Based Supercapacitor Exhibiting High Mechanical and Chemical Toughness for Large‐Scale Energy Storage Applications

In response to the demand for flexible and sustainable energy storage devices that exhibit high electrochemical performance, a supercapacitor system is fabricated using mulberry tree‐derived paper as a substrate and Poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) and carbon black as the active material. The mulberry paper‐based supercapacitor system demonstrates high energy density of 29.8–39.8 Wh kg^?1 and power density of 2.8–13.9 kW kg^?1 with 90.7% retention of its initial capacity over 15 000 charge–discharge cycles. In addition, the mulberry tree fibers are known to have superior mechanical strength and toughness and the mulberry paper‐based supercapacitor; as a result, exhibit high mechanical and chemical toughness; 99% of its initial capacity is retained after 100 repeated applications of bending strains, and twisting. 94% capacity retention is observed even after exposure to HCl and H₂SO₄ acid solutions. The fabrication methodology of the mulberry‐based supercapacitor is highly scalable and could be stacked to increase the energy storage capacity, where operation of light‐emitting diode lights with a drive voltage of 12 V integrated in a wearable device is demonstrated.     

Fast Redox Kinetics in Bi‐Heteroatom Doped 3D Porous Carbon Nanosheets for High‐Performance Hybrid Potassium‐Ion Battery Capacitors

Potassium‐ion hybrid capacitors (PIHCs) hold the advantages of high‐energy density of batteries and high‐power output of supercapacitors and thus present great promise for the next generation of electrochemical energy storage devices. One of the most crucial tasks for developing a high‐performance PIHCs is to explore a favorable anode material with capability to balance the kinetics mismatch between battery‐type anodes and capacitor‐type cathode. Herein, a reliable route for fabricating sulfur and nitrogen codoped 3D porous carbon nanosheets (S‐N‐PCNs) is reported. Systematic characterizations coupled with kinetics analysis indicate that the doped heteroatoms of sulfur and nitrogen and the amplified graphite interlayer can provide ample structural defects and redox active sites that are beneficial for improving pseudocapacitive activity, enabling fast kinetics toward efficient potassium‐ion storage. The S‐N‐PCNs are demonstrated to exhibit superior potassium storage capability with a high capacity of 107 mAh g^?1 at 20 A g^?1 and long cycle stability. The as‐developed PIHCs present impressive electrochemical performance with an operating voltage as high as 4.0 V, an energy density of 187 Wh kg^?1, a power density of 5136 W kg^?1, and a capacity retention of 86.4% after 3000 cycles.     

Amorphous Tin‐Based Composite Oxide: A High‐Rate and Ultralong‐Life Sodium‐Ion‐Storage Material

Energy‐storage technology is moving beyond lithium batteries to sodium as a result of its high abundance and low cost. However, this sensible transition requires the discovery of high‐rate and long‐lifespan anode materials, which remains a significant challenge. Here, the facile synthesis of an amorphous Sn₂P₂O₇/reduced graphene oxide nanocomposite and its sodium storage performance between 0.01 and 3.0 V are reported for the first time. This hybrid electrode delivers a high specific capacity of 480 mA h g^?1 at a current density of 50 mA g^?1 and superior rate performance of 250 and 165 mA h g^?1 at 2 and 10 A g^?1, respectively. Strikingly, this anode can sustain 15 000 cycles while retaining over 70% of the initial capacity. Quantitative kinetic analysis reveals that the sodium storage is governed by pseudocapacitance, particularly at high current rates. A full cell with sodium super ionic conductor (NASICON)‐structured Na₃V₂(PO₄)₂F₃ and Na₃V₂(PO₄)₃ as cathodes exhibits a high energy density of over 140 W h kg^?1 and a power density of nearly 9000 W kg^?1 as well as stability over 1000 cycles. This exceptional performance suggests that the present system is a promising power source for promoting the substantial use of low‐cost energy storage systems.     

All Pseudocapacitive MXene‐RuO2 Asymmetric Supercapacitors

2D transition metal carbides and nitrides, known as MXenes, are an emerging class of 2D materials with a wide spectrum of potential applications, in particular in electrochemical energy storage. The hydrophilicity of MXenes combined with their metallic conductivity and surface redox reactions is the key for high‐rate pseudocapacitive energy storage in MXene electrodes. However, symmetric MXene supercapacitors have a limited voltage window of around 0.6 V due to possible oxidation at high anodic potentials. In this study, the fact that titanium carbide MXene (Ti₃C₂T_x) can operate at negative potentials in acidic electrolyte is exploited, to design an all‐pseudocapacitive asymmetric device by combining it with a ruthenium oxide (RuO₂) positive electrode. This asymmetric device operates at a voltage window of 1.5 V, which is about two times wider than the operating voltage window of symmetric MXene supercapacitors, and is the widest voltage window reported to date for MXene‐based supercapacitors. The complementary working potential windows of MXene and RuO₂, along with proton‐induced pseudocapacitance, significantly enhance the device performance. As a result, the asymmetric devices can deliver an energy density of 37 µW h cm^?2 at a power density of 40 mW cm^?2, with 86% capacitance retention after 20 000 charge–discharge cycles. These results show that pseudocapacitive negative MXene electrodes can potentially replace carbon‐based materials in asymmetric electrochemical capacitors, leading to an increased energy density.     

Revealing Pseudocapacitive Mechanisms of Metal Dichalcogenide SnS2/Graphene‐CNT Aerogels for High‐Energy Na Hybrid Capacitors

SnS₂ nanoplatelet electrodes can offer an exceptionally high pseudocapacitance in an organic Na⁺ ion electrolyte system, but their underlying mechanisms are still largely unexplored, hindering the practical applications of pseudocapacitive SnS₂ anodes in Na‐ion batteries (SIBs) and Na hybrid capacitors (SHCs). Herein, SnS₂ nanoplatelets are grown directly on SnO₂/C composites to synthesize SnS₂/graphene‐carbon nanotube aerogel (SnS₂/GCA) by pressurized sulfidation where the original morphology of carbon framework is preserved. The composite electrode possessing a large surface area delivers a remarkable specific capacity of 600.3 mA h g^?1 at 0.2 A g^?1 and 304.8 mA h g^?1 at an ultrahigh current density of 10 A g^?1 in SIBs. SHCs comprising a SnS₂/GCA composite anode and an activated carbon cathode present exceptional energy densities of 108.3 and 26.9 W h kg^?1 at power densities of 130 and 6053 W kg^?1, respectively. The in situ transmission electron microscopy and the density functional theory calculations reveal that the excellent pseudocapacitance originates from the combination of Na adsorption on the surface/Sn edge of SnS₂ nanoplatelets and ultrafast Na⁺ ion intercalation into the SnS₂ layers.     

Flexible Asymmetric Micro‐Supercapacitors Based on Bi2O3 and MnO2 Nanoflowers: Larger Areal Mass Promises Higher Energy Density

A flexible asymmetric supercapacitor (ASC) with high energy density is designed and fabricated using flower‐like Bi₂O₃ and MnO₂ grown on carbon nanofiber (CNF) paper as the negative and positive electrodes, respectively. The lightweight (1.6 mg cm^?2), porous, conductive, and flexible features make the CNF paper an ideal support for guest active materials, which permit a large areal mass of 9 mg cm^?2 for Bi₂O₃ (≈85 wt% of the entire electrode). Thus, the optimal device with an operation voltage of 1.8 V can deliver a high energy density of 43.4 μWh cm^?2 (11.3 W h kg^?1, based on the total electrodes) and a maximum power density of 12.9 mW cm^?2 (3370 W kg^?1). This work provides an example of large areal mass and flexible electrode for ASCs with high areal capacitance and high energy density, holding great promise for future flexible electronic devices.     

Tailored Plum Pudding‐Like Co2P/Sn Encapsulated with Carbon Nanobox Shell as Superior Anode Materials for High‐Performance Sodium‐Ion Capacitors

Sodium‐ion capacitors (SICs) are emerging energy storage devices with high energy, high power, and durable life. Sn is a promising anode material for lithium storage, but the poor conductivity of the a‐NaSn phase upon sodaition hinders its implementation in SICs. Herein, a superior Sn‐based anode material consisting of plum pudding‐like Co₂P/Sn yolk encapsulated with nitrogen‐doped carbon nanobox (Co₂P/Sn@NC) for high‐performance SICs is reported. The 8–10 nm metallic nanoparticles produced in situ are uniformly dispersed in the amorphous Sn matrix serving as conductive fillers to facilitate electron transfer in spite of the formation of electrically resistive a‐NaSn phase during cycling. Meanwhile, the carbon shell buffers the large expansion of active Sn and provides a stable electrode–electrolyte interface. Owing to these merits, the yolk–shell Co₂P/Sn@NC demonstrates a large capacity of 394 mA h g^?1 at 100 mA g^?1, high rate capability of 168 mA h g^?1 at 5000 mA g^?1, and excellent cyclability with 87% capacity retention after 10 000 cycles. By integrating the Co₂P/Sn@NC anode with a peanut shell‐derived carbon cathode in the SIC, high energy densities of 112.3 and 43.7 Wh kg^?1 at power densities of 100 and 10 000 W kg^?1 are achieved.     

NiCo2S4 Nanosheets Grown on Nitrogen‐Doped Carbon Foams as an Advanced Electrode for Supercapacitors

To push the energy density limit of supercapacitors, a new class of electrode materials with favorable architectures is strongly needed. Binary metal sulfides hold great promise as an electrode material for high‐performance energy storage devices because they offer higher electrochemical activity and higher capacity than mono‐metal sulfides. Here, the rational design and fabrication of NiCo₂S₄ nanosheets supported on nitrogen‐doped carbon foams (NCF) is presented as a novel flexible electrode for supercapacitors. A facile two‐step method is developed for growth of NiCo₂S₄ nanosheets on NCF with robust adhesion, involving the growth of Ni‐Co precursor and subsequent conversion into NiCo₂S₄ nanosheets through sulfidation process. Benefiting from the compositional features and 3D electrode architectures, the NiCo₂S₄/NCF electrode exhibits greatly improved electrochemical performance with ultrahigh capacitance (877 F g^?1 at 20 A g^?1) and excellent cycling stability. Moreover, a binder‐free asymmetric supercapacitor device is also fabricated by using NiCo₂S₄/NCF as the positive electrode and ordered mesoporous carbon (OMC)/NCF as the negative electrode; this demonstrates high energy density (≈45.5 Wh kg^?1 at 512 W kg^?1).     

A Pair of NiCo2O4 and V2O5 Nanowires Directly Grown on Carbon Fabric for Highly Bendable Lithium‐Ion Batteries

Mechanically bendable and flexible functionalities are urgently required for next‐generation battery systems that will be included in soft and wearable electronics, active sportswear, and origami‐based deployable space structures. However, it is very difficult to synthesize anode and cathode electrodes that have high energy density and structural reliability under large bending deformation. Here, vanadium oxide (V₂O₅) and nickel cobalt oxide (NiCo₂O₄) nanowire‐carbon fabric electrodes for highly flexible and bendable lithium ion batteries are reported. The vanadium oxide and nickel cobalt oxide nanowires were directly grown on plasma‐treated carbon fabric and were used as cathode and anode electrodes in a full cell lithium ion battery. Most importantly, a pre‐lithiation process was added to the nickel cobalt oxide nanowire anode to facilitate the construction of a full cell using symmetrically‐architectured nanowire‐carbon fabric electrodes. The highly bendable full cell based on poly(ethylene oxide) polymer electrolyte and room temperature ionic liquid shows high energy density of 364.2 Wh kg^?1 at power density of 240 W kg^?1, without significant performance degradation even under large bending deformations. These results show that vanadium oxide and lithiated nickel cobalt oxide nanowire‐carbon fabrics are a good combination for binder‐free electrodes in highly flexible lithium‐ion batteries.     

Achieving Ultrahigh Energy Densities of Supercapacitors with Porous Titanium Carbide/Boron‐Doped Diamond Composite Electrodes

The energy densities of most supercapacitors (SCs) are low, hindering their practical applications. To construct SCs with ultrahigh energy densities, a porous titanium carbide (TiC)/boron‐doped diamond (BDD) composite electrode is synthesized on a titanium plate that is pretreated using a plasma electrolytic oxidation (PEO) technique. The porous and nanometer‐thick TiO₂ layer formed during PEO process prevents the formation of brittle titanium hydride and enhances the BDD growth during chemical vapor deposition processes. Meanwhile, the in situ conversion of TiO₂ into TiC is achieved. Combination of this capacitor electrode with soluble redox electrolytes leads to the fabrication of high‐performance SCs in both aqueous and organic solutions. In 0.05 m Fe(CN)₆^3?/4? + 1 m Na₂SO₄ aqueous solution, the capacitance is as high as 46.3 mF cm^?2 at a current density of 1 mA cm^?2; this capacitance remains 92% of its initial value even after 10 000 charge/discharge cycles; the energy density is up to 47.4 Wh kg^?1 at a power density of 2236 W kg^?1. The performance of constructed SCs is superior to most available SCs and some electrochemical energy storage devices like batteries. Such a porous capacitor electrode is thus promising for the construction of high‐performance SCs for practical applications.