Robust Single-Walled Carbon Nanotube-Infiltrated Carbon Fiber Electrodes for Structural Supercapacitors: from Reductive Dissolution to High Performance Devices

Multifunctional electrodes for structural supercapacitors are prepared by vacuum infiltration of single-walled carbon nanotubes (SWCNTs) into woven carbon fibers (CFs); the use of reductive charging chemistry to form nanotubide solutions ensured a high degree of individualization. The route is highly versatile, as shown by comparing four different commercial nanotube feedstocks. In film form, the pure nanotubide networks (“buckypapers”) are highly conductive (up to 2000 S cm⁻¹) with high surface area (>1000 m² g⁻¹) and great electrochemical performance (capacitance of 101 F g⁻¹, energy density of 27.5 Wh kg⁻¹ and power density of 135 kW kg⁻¹). Uniformly integrating these SWCNT networks throughout the CF fabrics significantly increased electrical conductivity (up to 318 S cm⁻¹), surface area (up to 196 m² g⁻¹), and in-plane shear properties, all simultaneously. The CNT-infiltrated CFs electrodes exhibited intrinsically high specific energy (2.6–4.2 Wh kg⁻¹) and power (6.0–8.7 kW kg⁻¹) densities in pure 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIM TFSI) electrolyte. Multifunctional structural supercapacitors based on CNT-coated CFs offer a substantial increase in capacitive performance while maintaining the tensile mechanical properties of the as-received CF-based composite. This non-damaging approach to modify CFs with highly graphitic, high surface area nanocarbons provides a new route to structural energy storage systems.     

Flexible Carbon Dots-Intercalated MXene Film Electrode with Outstanding Volumetric Performance for Supercapacitors

2D MXenes have emerged as promising supercapacitor electrode materials due to their metallic conductivity, pseudo-capacitive mechanism, and high density. However, layer-restacking is a bottleneck that restrains their ionic kinetics and active site exposure. Herein, a carbon dots-intercalated strategy is proposed to fabricate flexible MXene film electrodes with both large ion-accessible active surfaces and high density through gelation of calcium alginate (CA) within the MXene nanosheets followed by carbonization. The formation of CA hydrogel within the MXene nanosheets accompanied by evaporative drying endow the MXene/CA film with high density. In the carbonization process, the CA-derived carbon dots can intercalate into the MXene nanosheets, increasing the interlayer spacing and promoting the electrolytic diffusion inside the MXene film. Consequently, the carbon dots-intercalated MXene films exhibit high volumetric capacitance (1244.6 F cm⁻³ at 1 A g⁻¹), superior rate capability (662.5 F cm⁻³ at 1000 A g⁻¹), and excellent cycling stability (93.5% capacitance retention after 30 000 cycles) in 3 m H₂SO₄. Additionally, an all-solid-state symmetric supercapacitor based on the carbon dots-intercalated MXene film achieves a high volumetric energy density of 27.2 Wh L⁻¹. This study provides a simple yet efficient strategy to construct high-volumetric performance MXene film electrodes for advanced supercapacitors.     

Achieving of Flexible,Free‐Standing,Ultracompact Delaminated Titanium Carbide Films for High Volumetric Performance and Heat‐Resistant Symmetric Supercapacitors

The volumetric performance of supercapacitors (SCs), besides the gravimetric performance, is attracting an increasing attention due to the fast development of electric vehicles and smart devices. Here, a unique design of symmetric supercapacitor material is reported with a tight face‐to‐face architecture by applying a high pressure to the delaminated Ti₃C₂ (d‐Ti₃C₂) films. The high pressure makes the d‐Ti₃C₂ films achieve an increased density, high electron conductivity, good wettability, and abundant interconnected mesopore channels to promote ion transport efficiently, that is, more cations can intercalate/deintercalate in the charging–discharging process. As a result, with the increase of the applying pressure, the d‐Ti₃C₂ film pressured at 40 MPa in 1 m Li₂SO₄ exhibits an ultrahigh capacitance of over 633 F cm^?3, outstanding energy density, and cyclic stability. Especially, the corresponding SC in 1 m 1‐ethyl‐3‐methylimidazolium tetrafluoroborate/acetonitrile organic electrolyte shows a high volumetric energy density of 41 Wh L^?1, which is the highest value reported for the SCs based on MXene materials in organic electrolytes. The outstanding volumetric electrochemical performance and thermal stability of the SCs based on the ultracompact d‐Ti₃C₂ film demonstrate their promising potential as forceful power sources for small electronic devices.     

Interlayer Injection of Low-Valence Zn Atoms to Activate MXene-Based Micro-Redox Capacitors With Battery-Type Voltage Plateaus

Insufficient and unstable energy output is the bottleneck issue radically restricting the application of micro-supercapacitors (MSCs). Herein, an interlayer atom injection strategy that can anchor low-valence Zn atoms (Zn^δ+, 0 < δ <2) on O-terminals of Ti₃C₂T_x (MXene) flakes within the MXene/silver-nanowires hybrid cathode of symmetric MSCs is first presented. Combining the polyacrylamide/ZnCl₂ hydrogel electrolyte rich in Cl⁻ and Zn²⁺ ions, the matched Zn^δ+/Zn²⁺ (−0.76 V vs SHE) and Ag/AgCl (0.23 V vs SHE), redox couples between the symmetrical electrodes are activated to offer faradaic charge storage beside ions-intercalation involved pseudocapacitance. Thus, a battery-type voltage plateau (≈0.9 V) appears in the discharge curve of a fabricated pseudo-symmetric micro-redox capacitor, simultaneously achieving energy density enhancement (117 µWh cm⁻² at 0.5 mA cm⁻²) and substantially improved power output stability (46% of the energy from the plateau region) relative to that before activation (98 µWh cm⁻² without voltage platform). The work provides a fire-new strategy to overcome the performance bottlenecks confronting conventional MSCs.     

Full-Temperature All-Solid-State Ti3C2Tx/Aramid Fiber Supercapacitor with Optimal Balance of Capacitive Performance and Flexibility

Full-temperature all-solid-state flexible symmetrical fiber supercapacitors (FSCs) are assembled by using montmorillonite flake/polyvinyl alcohol organic hydrogel (F-MMT/PVA OHGE) as the electrolyte and separator and Ti₃C₂T_x/ANF-5% (T/A-5) fiber as the electrode, in which T/A-5 fiber is prepared by using delaminated Ti₃C₂T_x nanosheets as assembled units and 5% of aramid nanofiber (ANF) as the functional additive using a wet spinning method in a coagulated bath with 0.5 m FeCl₂ solution. The T/A-5 hybrid fiber exhibits a specific capacity of 807 F cm⁻³ in 3 m H₂SO₄ electrolyte, a superior mechanical strength of 104 MPa, and a high conductivity of 1025 S cm⁻¹. The assembled F-MMT/PVA OHGE T/A-5 FSC not only shows a specific capacitance of 295 F cm⁻³ and a capacitance retention of 91% at a current density of 5 A cm⁻³ after 10 000 charging/discharging cycles, but also a maximum volumetric energy density of 26.2 mWh cm⁻³. Meanwhile, the assembled device displays good flexibility and excellent capacitance in a wide temperature range of −40 to 80 °C, the electrochemical performance of the FSC is maintained under varying degrees of bending. This study provides an effective strategy for designing and assembling of full-temperature all-solid-state symmetrical flexible FSCs with the optimal balance of capacitive performance and flexibility.     

Modifying Electronic Structure of Cation-Exchanged Bimetallic Sulfide/Metal Oxide Heterostructure through In Situ Inclusion of Silver (Ag) Nanoparticles for Extrinsic Pseudocapacitor

The inferior electrical conductivity of conventional electrodes and their slow charge transport impose limitations on the electrochemical performance of supercapacitors (SCs) using those electrodes, necessitating strategies to overcome the limitations. An in situ Ag ion-incorporated cation-exchanged bimetallic sulfide/metal oxide heterostructure (Ag-Co_9-xFe_xS₈@α-Fe_xO_y) is synthesized using a two-step hydrothermal method. The coordination bond formation and Ag nanoparticle (NP) incorporation improve the electrical conductivity and adhesion of the heterostructure and reduce its interface resistance and volume expansion throughout the charge/discharge cycles. Density functional theory investigations indicate that the remarkable interlayer and interparticle conductivities of the heterostructure resulting from Ag doping have changed its electronic states, leading to an enhanced electrical conductivity. The optimized electrode has an excellent specific capacity (213.6 mA h g⁻¹ at 1 A g⁻¹) and can maintain 93.2% capacity retention with excellent Coulombic efficiency over 20 000 charge/discharge cycles. A flexible solid-state extrinsic pseudocapacitor (EPSC) is fabricated using Ag-Co_9-xFe_xS₈@α-Fe_xO_y and Ti₃C₂T_X electrodes. The EPSC has specific and volumetric capacitances of 259 F g⁻¹ and 2.7 F cm⁻³ at 0.7 A g⁻¹, respectively, an energy density of 80.9 Wh kg⁻¹ at 525 W kg⁻¹, and a capacity retention of 92.8% over 5000 charge/discharge cycles.     

A High‐Power Symmetric Na‐Ion Pseudocapacitor

Batteries and supercapacitors are critical devices for electrical energy storage with wide applications from portable electronics to transportation and grid. However, rechargeable batteries are typically limited in power density, while supercapacitors suffer low energy density. Here, a novel symmetric Na‐ion pseudocapacitor with a power density exceeding 5.4 kW kg^?1 at 11.7 A g^?1, a cycling life retention of 64.5% after 10 000 cycles at 1.17 A g^?1, and an energy density of 26 Wh kg^?1 at 0.585 A g^?1 is reported. Such a device operates on redox reactions occurring on both electrodes with an identical active material, viz., Na₃V₂(PO₄)₃ encapsulated inside nanoporous carbon. This device, in a full‐cell scale utilizing highly reversible and high‐rate Na‐ion intercalational pseudocapacitance, can bridge the performance gap between batteries and supercapacitors. The characteristics of the device and the potentially low‐cost production make it attractive for hybrid electric vehicles and low‐maintenance energy storage systems.     

Tailoring Ultrahigh Energy Density and Stable Dendrite-Free Flexible Anode with Ti3C2Tx MXene Nanosheets and Hydrated Ammonium Vanadate Nanobelts for Aqueous Rocking-Chair Zinc Ion Batteries

Exploiting Zn metal-free anode materials would be an effective strategy to resolve the problems of Zn metal dendrites that severely hinder the development of Zn ion batteries (ZIBs). However, the study of Zn metal-free anode materials is still in their infancy, and more importantly, the low energy density severely limits their practical implementations. Herein, a novel (NH₄)₂V₁₀O₂₅ · 8H₂O@Ti₃C₂T_x (NHVO@Ti₃C₂T_x) film anode is proposed and investigated for constructing “rocking-chair” ZIBs. The NHVO@Ti₃C₂T_x electrode shows a capacity of 514.7 mAh g⁻¹ and presents low potential which is 0.59 V (vs Zn²⁺/Zn) at 0.1 A g⁻¹. The introduction of Ti₃C₂T_x not only affords an interconnected conductive network, but also stabilizes the NHVO nanobelts structure for a long cycle life (84.2% retention at 5.0 A g⁻¹ over 6000 cycles). As a proof-of-concept, a zinc metal-free full battery is successfully demonstrated, which delivers the highest capacity of 131.7 mAh g⁻¹ (mass containing anodic and cathodic) and energy density of 97.1 Wh kg⁻¹ compared to all reported aqueous “rocking-chair” ZIBs. Furthermore, a long cycling span of 6000 cycles is obtained with capacity retention reaching up to 92.1%, which is impressive. This work is expected to provide new moment toward V-based materials for “rocking-chair” ZIBs.     

Ultrahigh Energy Storage Capacitors Based on Freestanding Single-Crystalline Antiferroelectric Membrane/PVDF Composites

Inorganic/organic dielectric composites are very attractive for high energy density electrostatic capacitors. Usually, linear dielectric and ferroelectric materials are chosen as inorganic fillers to improve energy storage performance. Antiferroelectric (AFE) materials, especially single-crystalline AFE oxides, have relatively high efficiency and higher density than linear dielectrics or ferroelectrics. However, adding single-crystalline AFE oxides into polymers to construct composite with improved energy storage performance remains elusive. In this study, high-quality freestanding single-crystalline PbZrO₃ membranes are obtained by a water-soluble sacrificial layer method. They exhibit classic AFE behavior and then 2D–2D type PbZrO₃/PVDF composites with the different film thicknesses of PbZrO₃ (0.1-0.4 µm) is constructed. Their dielectric properties and polarization response improve significantly as compared to pure PVDF and are optimized in the PbZrO₃(0.3 µm)/PVDF composite. Consequently, a record-high energy density of 43.3 J cm⁻³ is achieved at a large breakdown strength of 750 MV m⁻¹. Phase-field simulation indicates that inserting PbZrO₃ membranes effectively reduces the breakdown path. Single-crystalline AFE oxide membranes will be useful fillers for composite-based high-power capacitors.     

Aqueous Ammonium-Ion Supercapacitors with Unprecedented Energy Density and Stability Enabled by Oxygen Vacancy-Enriched MoO3@C

The use of non-metal charge carriers such as ammonium (NH₄⁺) in electrochemical energy storage devices offers advantages in terms of weight, element abundance, and compatibility with aqueous electrolytes. However, the development of suitable electrodes for such carriers lags behind other technologies. Herein, we present a high-performance anode material for ammonium-ion supercapacitors based on a MoO₃/carbon (MoO₃@C) composite. The NH₄⁺ storage performance of such composites and their practical application prospects are evaluated both in a three-electrode configuration and as symmetric supercapacitors. The optimized material reaches an unprecedented specific capacitance of 473 F·g⁻¹ (158 mAh·g⁻¹; 1592 mF·cm⁻²) at a current density of 1 A·g⁻¹, and 92.7% capacitance retention after 5000 cycles in a three-electrode set-up. This outstanding performance is related to the presence of oxygen vacancies that enhance the composites’ ionic/electronic transportation and electrochemical reaction site, while at the same time facilitating the formation of hydrogen bonds between NH₄⁺ and the host material. Using the optimized composite, symmetric supercapacitors based on an (NH₄)₂SO₄ gel electrolyte are fabricated and demonstrated to provide unmatched energy densities above 78 Wh·kg⁻¹ at a power density of 929 W·kg⁻¹. Besides, such devices are characterized by extraordinary capacitance retention of 97.6% after 10,000 cycles.     

High‐Performance Supercapacitor Applications of NiO‐Nanoparticle‐Decorated Millimeter‐Long Vertically Aligned Carbon Nanotube Arrays via an Effective Supercritical CO2‐Assisted Method

Nickel oxide (NiO) nanoparticles are distributed uniformly in the vertically aligned carbon nanotube arrays (VACNTs) with millimeter thickness by an effective supercritical carbon dioxide‐assisted method. The as‐prepared VACNT/NiO hybrid structures are used as electrodes without binders and conducting additives for supercapacitor applications. Due to the synergetic effects of NiO and VACNTs with nanoporous structures and parallel 1D conductive paths for electrons, the supercapacitors exhibit a high capacitance of 1088.44 F g^?1. Furthermore, an asymmetric supercapacitor is assembled using the as‐synthesized VACNTs/NiO hybrids as the positive electrode and the VACNTs as the negative electrode. Remarkably, the energy density of the asymmetric supercapacitor is as high as 90.9 Wh kg^?1 at 3.2 kW kg^?1 and the maximum power density reaches 25.6 kW kg^?1 at 24.9 Wh kg^?1, which are superior to those of the NiO or VACNTs‐based asymmetric supercapacitors. More importantly, the asymmetric supercapacitors exhibit capacitance retention of 87.1% after 2000 cycles at 5 A g^?1. The work provides a novel approach in decorating highly dense and long VACNTs with active materials, which are promising electrodes for supercapacitors with ultrahigh power density and energy density.     

Tetrabutylammonium-Intercalated 1T-MoS2 Nanosheets with Expanded Interlayer Spacing Vertically Coupled on 2D Delaminated MXene for High-Performance Lithium-Ion Capacitors

2D 1T phase MoS₂ (1T-MoS₂) nanosheet with metallic conductivity and expanded interlayer spacing is considered as a highly potential lithium storage electrode material but remains thermodynamic instability in aqueous media, seriously hindering the electrochemical performance. Herein, a versatile strategy is proposed for the preparation of thermodynamically stable 1T-MoS₂/MXene heterostructures with the aid of delaminated Ti₃C₂T_x MXene (d-Ti₃C₂T_x) dispersion containing tetrabutylammonium hydroxide. The 2D d-Ti₃C₂T_x provides more uniform nucleation sites for MoS₂, and the TBA⁺ ions can intercalate into MoS₂ to induce the phase conversion from semiconducting 2H to 1T. Moreover, the electrochemical advantages of 1T-MoS₂ and d-Ti₃C₂T_x can be united by the construction of a well-organized heterostructure. Outstanding rate performance is realized because of extra-large interlayer space of 1T MoS₂ with TBA⁺ intercalation and decreased energy barrier for fast Li⁺ diffusion. Subsequently, a lithium-ion capacitor (LIC) is assembled based on 1T-MoS₂/d-Ti₃C₂T_x as anode and hierarchically porous graphene nanocomposite with micro/mesoporous structure as a cathode. The LIC exhibits a large energy density up to 188 Wh kg⁻¹, an ultra-high power density of 13 kW kg⁻¹, together with remarkable capacity retention of 83% after 5000 cycles. This study demonstrates the great promise of 1T-MoS₂/d-Ti₃C₂T_x heterostructures as anode for high-performance LICs.     

Diamond-Based Supercapacitors with Ultrahigh Cyclic Stability Through Dual-Phase MnO2-Graphitic Transformation Induced by High-Dose Mn-Ion Implantation

While occasionally being able to charge and discharge more quickly than batteries, carbon-based electrochemical supercapacitors (SCs) are nevertheless limited by their simplicity of processing, adjustable porosity, and lack of electrocatalytic active sites for a range of redox reactions. Even SCs based on the most stable form of carbon (sp³ carbon/diamond) have a poor energy density and inadequate capacitance retention during long charge/discharge cycles, limiting their practical applications. To construct a SC with improved cycling stability/energy density Mn-ion implanted (high-dose; 10¹⁵–10¹⁷ ions cm⁻²) boron doped diamond (Mn-BDD) films have been prepared. Mn ion implantation and post-annealing process results in an in situ graphitization (sp² phase) and growth of MnO₂ phase with roundish granular grains on the BDD film, which is favorable for ion transport. The dual advantage of both sp² (graphitic phase) and sp³ (diamond phase) carbons with an additional pseudocapacitor (MnO₂) component provides a unique and critical function in achieving high-energy SC performance. The capacitance of Mn-BDD electrode in a redox active aqueous electrolyte (0.05 M Fe(CN)₆^3-/4− + 1 M Na₂SO₄) is as high as 51 mF cm⁻² at 10 mV s⁻¹ with exceptional cyclic stability (≈100% capacitance even after 10 000 charge/discharge cycles) placing it among the best-performing SCs. Furthermore, the ultrahigh capacitance retention (≈80% retention after 88 000 charge/discharge cycles) in a gel electrolyte containing a two-electrode configuration shows a promising prospect for high-rate electrochemical capacitive energy storage applications.     

Defect Modulation in Cobalt Manganese Oxide Sheets for Stable and High-Energy Aqueous Aluminum-Ion Batteries

Rechargeable aqueous Al-ion batteries (AIBs) are promising low-cost, safe, and high energy density systems for large-scale energy storage. However, the strong electrostatic interaction between the Al³⁺ and the host material, usually leads to sluggish Al³⁺ diffusion kinetics and severe structure collapse of the cathode material. Consequently, aqueous AIBs currently suffer from low energy density as well as inferior rate capability and cycling stability. Here, defective cobalt manganese oxide nanosheets are reported as cathode material for aqueous AIBs to improve both reaction kinetics and stability, delivering a record high energy density of 685 Wh kg⁻¹ (based on the masses of the cathode and anode) and a reversible capacity of 585 mAh g⁻¹ at 100 mA g⁻¹ with a retention of 78% after 300 cycles. The impressive energy density and cycling stability are due to a synergistic effect between the substituted cobalt atoms and the manganese vacancies, which improve the structural stability and promote both electron conductivity and ion diffusion. When applied in aqueous Zn-ion batteries, a high specific energy of 390 Wh kg⁻¹ at 100 mA g⁻¹ is realized while retaining 84% initial capacity over 1000 cycles. The study offers a new pathway to building next-generation high-energy aqueous rechargeable metal batteries.     

Two-Dimensional Siloxene–Graphene Heterostructure-Based High-Performance Supercapacitor for Capturing Regenerative Braking Energy in Electric Vehicles

The development of high-performance electrodes that increase the energy density of supercapacitors (SCs) (without compromising their power density) and have a wide temperature tolerance is crucial for the application of SCs in electric vehicles. Recent research has focused on the preparation of multicomponent materials to form electrodes with enhanced electrochemical properties. Herein, a siloxene–graphene (rGO) heterostructure electrode-based symmetric SC (SSC) is designed that delivers a high energy density (55.79 Wh kg⁻¹) and maximum power density of 15 000 W kg⁻¹. The fabricated siloxene–rGO SSC can operate over a wide temperature range from –15 to 80 °C, which makes them suitable for applications in automobiles. This study shows the practical applicability of siloxene–rGO SSC to drive an electric car as well as to capture the braking energy in a regenerative brake-electric vehicle prototype. This work opens new directions for evaluating the use of siloxene–rGO SSC as suitable energy devices in electric vehicles.     

Engineering the Interlayer Spacing by Pre-Intercalation for High Performance Supercapacitor MXene Electrodes in Room Temperature Ionic Liquid

MXenes exhibit excellent capacitance at high scan rates in sulfuric acid aqueous electrolytes, but the narrow potential window of aqueous electrolytes limits the energy density. Organic electrolytes and room-temperature ionic liquids (RTILs) can provide higher potential windows, leading to higher energy density. The large cation size of RTIL hinders its intercalation in-between the layers of MXene limiting the specific capacitance in comparison to aqueous electrolytes. In this work, different chain lengths alkylammonium (AA) cations are intercalated into Ti₃C₂T_x, producing variation of MXene interlayer spacings (d-spacing). AA-cation-intercalated Ti₃C₂T_x (AA-Ti₃C₂), exhibits higher specific capacitances, and cycling stabilities than pristine Ti₃C₂T_x in 1 m 1-ethly-3-methylimidazolium bis-(trifluoromethylsulfonyl)-imide (EMIMTFSI) in acetonitrile and neat EMIMTFSI RTIL electrolytes. Pre-intercalated MXene with an interlayer spacing of ≈2.2 nm, can deliver a large specific capacitance of 257 F g⁻¹ (1428 mF cm⁻² and 492 F cm⁻³) in neat EMIMTFSI electrolyte leading to high energy density. Quasi elastic neutron scattering and electrochemical impedance spectroscopy are used to study the dynamics of confined RTIL in pre-intercalated MXene. Molecular dynamics simulations suggest significant differences in the structures of RTIL ions and AA cations inside the Ti₃C₂T_x interlayer, providing insights into the differences in the observed electrochemical behavior.     

Ultrahigh Energy Density of Antiferroelectric PbZrO3-Based Films at Low Electric Field

Dielectric capacitors play a vital role in advanced electronics and power systems as a medium of energy storage and conversion. Achieving ultrahigh energy density at low electric field/voltage, however, remains a challenge for insulating dielectric materials. Taking advantage of the phase transition in antiferroelectric (AFE) film PbZrO₃ (PZO), a small amount of isovalent (Sr²⁺) / aliovalent (La³⁺) dopants are introduced to form a hierarchical domain structure to increase the polarization and enhance the backward switching field E_A simultaneously, while maintaining a stable forward switching field E_F. An ultrahigh energy density of 50 J cm⁻³ is achieved for the nominal Pb_0.925La_0.05ZrO₃ (PLZ5) films at low electric fields of 1 MV cm⁻¹, exceeding the current dielectric energy storage films at similar electric field. This study opens a new avenue to enhance energy density of AFE materials at low field/voltage based on a gradient-relaxor AFE strategy, which has significant implications for the development of new dielectric materials that can operate at low field/voltage while still delivering high energy density.     

Overcoming the Challenges of Freestanding Tin Oxide-Based Composite Anodes to Achieve High Capacity and Increased Cycling Stability

Freestanding electrodes are a promising way to increase the energy density of the batteries by decreasing the overall amount of electrochemically inactive materials. Freestanding antimony doped tin oxide (ATO)-based hybrid materials have not been reported so far, although this material has demonstrated excellent performance in conventionally designed electrodes. Two different strategies, namely electrospinning and freeze-casting, are explored for the fabrication of ATO-based hybrid materials. It is shown that the electrospinning of ATO/carbon based electrodes from polyvinyl pyrrolidone polymer (PVP) solutions was not successful, as the resulting electrode material suffers from rapid degradation. However, freestanding reduced graphene oxide (rGO) containing ATO/C/rGO nanocomposites prepared via a freeze-casting route demonstrates an impressive rate and cycling performance reaching 697 mAh g⁻¹ at a high current density of 4 A g⁻¹, which is 40 times higher as compared to SnO₂/rGO and also exceeds the freestanding SnO₂-based composites reported so far. Antimony doping of the nanosized tin oxide phase and carbon coating are thereby shown to be essential factors for appealing electrochemical performance. Finally, the freestanding ATO/C/rGO anodes are combined with freestanding LiFe_0.2Mn_0.8PO₄/rGO cathodes to obtain a full freestanding cell operating without metal current collector foils showing nonetheless an excellent cycling stability.     

High Loading Sulfur Cathodes by Reactive-Type Polymer Tubes for High-Performance Lithium-Sulfur Batteries

Simultaneously attaining high gravimetric energy density (E_g) and volumetric energy density (E_v) in lithium-sulfur (Li–S) batteries is a longstanding challenge that has to be solved for practical application, which demands breakthroughs in electrode materials with optimized functionality and structure. Herein, anthraquinone-containing, reactive-type polymer tubes (PQT) that can be used to regulate the redox chemistry of sulfur species are designed and prepared for practical Li–S batteries. PQT favors a similar redox potential window as sulfur, which effectively facilitates the immobilization and conversion of sulfur species through a reversible lithiation/delithiation process. Its tubular structure and high tap density is vital to the fabrication of intact electrode with high sulfur loading and minimizing electrolyte intake during battery operation. With all these contributions, Li–S battery with PQT/S cathode exhibits a stable cycling capacity (73% at 2.0 C over 1000 cycles), remarkable rate performance (514.2 mAh g⁻¹ at 10 C), and a high areal capacity of 7.20 mAh g⁻¹ with high sulfur loading under lean electrolyte condition. More importantly, the assembled Li–S pouch cell delivers an E_g of 329 Wh kg⁻¹ and an E_v of 401 Wh L⁻¹, which meets the requirement for practical operation.     

Hierarchical Integrated Hybrid Structural Electrodes Based on Co-N/C and Mo-doped NiCo-LDH@Co-N/C Anchored on MX/CF for High Energy Density Fiber-Shaped Supercapacitor

The judicious design of highly electrochemically active materials on 1D fiber substrate to form a hierarchical integrated hybrid structure is an efficient technique to improve the limited cylindrical space and volumetric energy density of fiber-shaped supercapacitors (FSCs). Herein, a 3D negative electrode, consisting of vertically aligned interconnected mesoporous Co-N/C leaf-like structure on 1D MXene-carbon fiber (Co-N/C@MX/CF) is prepared by controlling the composition and morphology. At the same time, a 3D positive electrode is also prepared by introducing Mo in NiCo-LDH anchored on Co-N/C@MX/CF (Mo-NiCo-LDH@Co-N/C@MX/CF) by electrodeposition method. Benefitting from the systematic hierarchical structures with highly accessible surface area, adequate pore size and easy permeation of electrolyte, both positive and negative electrodes demonstrate highly improved electrochemical performance with areal capacity/capacitance of 0.96 mAh cm⁻²/4.55 mF cm⁻² at a current density of 3.86 mA cm⁻², respectively. Furthermore, the fiber-shaped solid-state hybrid supercapacitor (FSHSC) based on Mo_1.5NiCo-LDH@Co-N/C@MX/CF(+)//Co-N/C_0.5@MX/CF(−) is fabricated, exhibiting compelling energy density of 86.72 mWh cm⁻³ at a power density of 480.30 mW cm⁻³ with an outstanding capacitance retention of 80.2% after 20000 galvanostatic-charge-discharge cycles. This study puts forward a new perspective on the development of highly efficient FSCs for practical application.