A High‐Energy Lithium‐Ion Capacitor by Integration of a 3D Interconnected Titanium Carbide Nanoparticle Chain Anode with a Pyridine‐Derived Porous Nitrogen‐Doped Carbon Cathode

Lithium‐ion capacitors (LICs) are hybrid energy storage devices that have the potential to bridge the gap between conventional high‐energy lithium‐ion batteries and high‐power capacitors by combining their complementary features. The challenge for LICs has been to improve the energy storage at high charge?discharge rates by circumventing the discrepancy in kinetics between the intercalation anode and capacitive cathode. In this article, the rational design of new nanostructured LIC electrodes that both exhibit a dominating capacitive mechanism (both double layer and pseudocapacitive) with a diminished intercalation process, is reported. Specifically, the electrodes are a 3D interconnected TiC nanoparticle chain anode, synthesized by carbothermal conversion of graphene/TiO₂ hybrid aerogels, and a pyridine‐derived hierarchical porous nitrogen‐doped carbon (PHPNC) cathode. Electrochemical properties of both electrodes are thoroughly characterized which demonstrate their outstanding high‐rate capabilities. The fully assembled PHPNC//TiC LIC device delivers an energy density of 101.5 Wh kg^?1 and a power density of 67.5 kW kg^?1 (achieved at 23.4 Wh kg^?1), and a reasonably good cycle stability (≈82% retention after 5000 cycles) within the voltage range of 0.0?4.5 V.     

Carbon‐Stabilized High‐Capacity Ferroferric Oxide Nanorod Array for Flexible Solid‐State Alkaline Battery–Supercapacitor Hybrid Device with High Environmental Suitability

Iron oxides are promising to be utilized in rechargeable alkaline battery with high capacity upon complete redox reaction (Fe³⁺ Fe⁰). However, their practical application has been hampered by the poor structural stability during cycling, presenting a challenge that is particularly huge when binder‐free electrode is employed. This paper proposes a “carbon shell‐protection” solution and reports on a ferroferric oxide–carbon (Fe₃O₄–C) binder‐free nanorod array anode exhibiting much improved cyclic stability (from only hundreds of times to >5000 times), excellent rate performance, and a high capacity of ≈7776.36 C cm^?3 (≈0.4278 C cm^?2; 247.5 mAh g^?1, 71.4% of the theoretical value) in alkaline electrolyte. Furthermore, by pairing with a capacitive carbon nanotubes (CNTs) film cathode, a unique flexible solid‐state rechargeable alkaline battery‐supercapacitor hybrid device (≈360 μm thickness) is assembled. It delivers high energy and power densities (1.56 mWh cm^?3; 0.48 W cm^?3/≈4.8 s charging), surpassing many recently reported flexible supercapacitors. The highest energy density value even approaches that of Li thin‐film batteries and is about several times that of the commercial 5.5 V/100 mF supercapacitor. In particular, the hybrid device still maintains good electrochemical attributes in cases of substantially bending, high mechanical pressure, and elevated temperature (up to 80 °C), demonstrating high environmental suitability.     

High‐Performance Sodium‐Ion Hybrid Supercapacitor Based on Nb2O5@Carbon Core–Shell Nanoparticles and Reduced Graphene Oxide Nanocomposites

Sodium‐ion hybrid supercapacitors (Na‐HSCs) have potential for mid‐ to large‐scale energy storage applications because of their high energy/power densities, long cycle life, and the low cost of sodium. However, one of the obstacles to developing Na‐HSCs is the imbalance of kinetics from different charge storage mechanisms between the sluggish faradaic anode and the rapid non‐faradaic capacitive cathode. Thus, to develop high‐power Na‐HSC anode materials, this paper presents the facile synthesis of nanocomposites comprising Nb₂O₅@Carbon core–shell nanoparticles (Nb₂O₅@C NPs) and reduced graphene oxide (rGO), and an analysis of their electrochemical performance with respect to various weight ratios of Nb₂O₅@C NPs to rGO (e.g., Nb₂O₅@C, Nb₂O₅@C/rGO‐70, ‐50, and ‐30). In a Na half‐cell configuration, the Nb₂O₅@C/rGO‐50 shows highly reversible capacity of ≈285 mA h g^?1 at 0.025 A g^?1 in the potential range of 0.01–3.0 V (vs Na/Na⁺). In addition, the Na‐HSC using the Nb₂O₅@C/rGO‐50 anode and activated carbon (MSP‐20) cathode delivers high energy/power densities (≈76 W h kg^?1 and ≈20 800 W kg^?1) with a stable cycle life in the potential range of 1.0–4.3 V. The energy and power densities of the Na‐HSC developed in this study are higher than those of similar Li‐ and Na‐HSCs previously reported.     

Self‐Standing Porous LiCoO2 Nanosheet Arrays as 3D Cathodes for Flexible Li‐Ion Batteries

Self‐standing electrodes are the key to realize flexible Li‐ion batteries. However, fabrication of self‐standing cathodes is still a major challenge. In this work, porous LiCoO₂ nanosheet arrays are grown on Au‐coated stainless steel (Au/SS) substrates via a facile “hydrothermal lithiation” method using Co₃O₄ nanosheet arrays as the template followed by quick annealing in air. The binder‐free and self‐standing LiCoO₂ nanosheet arrays represent the 3D cathode and exhibit superior rate capability and cycling stability. In specific, the LiCoO₂ nanosheet array electrode can deliver a high reversible capacity of 104.6 mA h g^?1 at 10 C rate and achieve a capacity retention of 81.8% at 0.1 C rate after 1000 cycles. By coupling with Li₄Ti₅O₁₂ nanosheet arrays as anode, an all‐nanosheet array based LiCoO₂//Li₄Ti₅O₁₂ flexible Li‐ion battery is constructed. Benefiting from the 3D nanoarchitectures for both cathode and anode, the flexible LiCoO₂//Li₄Ti₅O₁₂ battery can deliver large specific reversible capacities of 130.7 mA h g^?1 at 0.1 C rate and 85.3 mA h g^?1 at 10 C rate (based on the weight of cathode material). The full cell device also exhibits good cycling stability with 80.5% capacity retention after 1000 cycles at 0.1 C rate, making it promising for the application in flexible Li‐ion batteries.     

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.     

Advantageous Functional Integration of Adsorption‐Intercalation‐Conversion Hybrid Mechanisms in 3D Flexible Nb2O5@Hard Carbon@MoS2@Soft Carbon Fiber Paper Anodes for Ultrafast and Super‐Stable Sodium Storage

Using synergetic effects of various sodium storage modes and materials to construct high power, high energy, and long cycling flexible sodium anode materials is significant and still challenging. Here, by advantageous functional integration of adsorption‐intercalation‐conversion sodium storage mechanisms, a 3D flexible fiber paper anode with the composition of Nb₂O₅@hard carbon@MoS₂@soft carbon is designed and prepared. Based on the synergetic effects, it exhibits higher specific capacity than pure Nb₂O₅, with more excellent rate performance (245, 201, 155, 133, and 97 mAh g^?1 at the current density of 0.2, 1, 5, 10, and 20 A g^?1, respectively) than pure MoS₂ as well as admirable long‐term cycling characteristics (≈82% capacity retention after 20 000 cycles at 5 A g^?1). Relevant kinetics mechanisms are expounded in detail. This work can be helpful for preparing other types of hybrid and flexible electrodes for energy storage systems.     

Fast and Large Lithium Storage in 3D Porous VN Nanowires–Graphene Composite as a Superior Anode Toward High‐Performance Hybrid Supercapacitors

Li‐ion hybrid capacitors (LIHCs), consisting of an energy‐type redox anode and a power‐type double‐layer cathode, are attracting significant attention due to the good combination with the advantages of conventional Li‐ion batteries and supercapacitors. However, most anodes are battery‐like materials with the sluggish kinetics of Li‐ion storage, which seriously restrict the energy storage of LIHCs at the high charge/discharge rates. Herein, vanadium nitride (VN) nanowire is demonstated to have obvious pseudocapacitive characteristic of Li‐ion storage and can get further gains in energy storage through a 3D porous architecture with the assistance of conductive reduced graphene oxide (RGO). The as‐prepared 3D VN–RGO composite exhibits the large Li‐ion storage capacity and fast charge/discharge rate within a wide working widow from 0.01–3 V (vs Li/Li⁺), which could potentially boost the operating potential and the energy and power densities of LIHCs. By employing such 3D VN–RGO composite and porous carbon nanorods with a high surface area of 3343 m² g^?1 as the anode and cathode, respectively, a novel LIHCs is fabricated with an ultrahigh energy density of 162 Wh kg^?1 at 200 W kg^?1, which also remains 64 Wh kg^?1 even at a high power density of 10 kW kg^?1.     

Fe2O3 Nanoneedles on Ultrafine Nickel Nanotube Arrays as Efficient Anode for High‐Performance Asymmetric Supercapacitors

High performance of electrochemical energy storage devices depends on the smart structure engineering of electrodes, including the tailored nanoarchitectures of current collectors and subtle hybridization of active materials. To improve the anode supercapacitive performance of Fe₂O₃ for high‐voltage asymmetric supercapacitors, here, a hybrid core‐branch nanoarchitecture is proposed by integrating Fe₂O₃ nanoneedles on ultrafine Ni nanotube arrays (NiNTAs@Fe₂O₃ nanoneedles). The fabrication process employs a bottom‐up strategy via a modified template‐assisted method starting from ultrafine ZnO nanorod arrays, ensuring the formation of ultrafine Ni nanotube arrays with ultrathin tube walls. The novel developed NiNTAs@Fe₂O₃ nanoneedle electrode is demonstrated to be a highly capacitive anode (418.7 F g^?1 at 10 mV s^?1), matching well with the similarly built NiNTAs@MnO₂ nanosheet cathode. Contributed by the efficient electron collection paths and short ion diffusion paths in the uniquely designed anode and cathode, the asymmetric supercapacitors exhibit an excellent maximum energy density of 34.1 Wh kg^?1 at the power density of 3197.7 W kg^?1 in aqueous electrolyte and 32.2 Wh kg^?1 at the power density of 3199.5 W kg^?1 in quasi‐solid‐state gel electrolyte.     

Flexible Sodium‐Ion Pseudocapacitors Based on 3D Na2Ti3O7 Nanosheet Arrays/Carbon Textiles Anodes

Flexible energy storage devices are critical components for emerging flexible and wearable electronics. Improving the electrochemical performance of flexible energy storage devices depends largely on development of novel electrode architectures and new systems. Here, a new class of flexible energy storage device called flexible sodium‐ion pseudocapacitors is developed based on 3D‐flexible Na₂Ti₃O₇ nanosheet arrays/carbon textiles (NTO/CT) as anode and flexible reduced graphene oxide film (GFs) as cathode without metal current collectors or conducting additives. The NTO/CT anode with advanced electrode architectures is fabricated by directly growing Na₂Ti₃O₇ nanosheet arrays on carbon textiles with robust adhesion through a simple hydrothermal process. The flexible GF//NTO/CT configuration achieves a high energy density of 55 Wh kg^?1 and high power density of 3000 W kg^?1. Taking the fully packaged flexible sodium‐ion pseudocapacitors into consideration, the maximum practical volumetric energy density and power density reach up to 1.3 mWh cm^?3 and 70 mW cm^?3, respectively. In addition, the flexible GF//NTO/CT device demonstrates a stable electrochemical performances with almost 100% capacitance retention under harsh mechanical deformation.     

Three‐Dimensional Co3O4@MnO2 Hierarchical Nanoneedle Arrays: Morphology Control and Electrochemical Energy Storage

In this paper, a highly ordered three‐dimensional Co₃O₄@MnO₂ hierarchical porous nanoneedle array on nickel foam is fabricated by a facile, stepwise hydrothermal approach. The morphologies evolution of Co₃O₄ and Co₃O₄@MnO₂ nanostructures upon reaction times and growth temperature are investigated in detail. Moreover, the as‐prepared Co₃O₄@MnO₂ hierarchical structures are investigated as anodes for both supercapacitors and Li‐ion batteries. When used for supercapacitors, excellent electrochemical performances such as high specific capacitances of 932.8 F g^?1 at a scan rate of 10 mV s^?1 and 1693.2 F g^?1 at a current density of 1 A g^?1 as well as long‐term cycling stability and high energy density (66.2 W h kg^?1 at a power density of 0.25 kW kg^?1), which are better than that of the individual component of Co₃O₄ nanoneedles and MnO₂ nanosheets, are obtained. The Co₃O₄@MnO₂ NAs are also tested as anode material for LIBs for the first time, which presents an improved performance with high reversible capacity of 1060 mA h g^?1 at a rate of 120 mA g^?1, good cycling stability, and rate capability.     

Zn(Cu)Si2+xP3 Solid Solution Anodes for High‐Performance Li‐Ion Batteries with Tunable Working Potentials

Si‐based anodes with a stiff diamond structure usually suffer from sluggish lithiation/delithiation reaction due to low Li‐ion and electronic conductivity. Here, a novel ternary compound ZnSi₂P₃ with a cation‐disordered sphalerite structure, prepared by a facile mechanochemical method, is reported, demonstrating faster Li‐ion and electron transport and greater tolerance to volume change during cycling than the existing Si‐based anodes. A composite electrode consisting of ZnSi₂P₃ and carbon achieves a high initial Coulombic efficiency (92%) and excellent rate capability (950 mAh g^?1 at 10 A g^?1) while maintaining superior cycling stability (1955 mAh g^?1 after 500 cycles at 300 mA g^?1), surpassing the performance of most Si‐ and P‐based anodes ever reported. The remarkable electrochemical performance is attributed to the sphalerite structure that allows fast ion and electron transport and the reversible Li‐storage mechanism involving intercalation and conversion reactions. Moreover, the cation‐disordered sphalerite structure is flexible to ionic substitutions, allowing extension to a family of Zn(Cu)Si_2+xP₃ solid solution anodes (x = 0, 2, 5, 10) with large capacity, high initial Coulombic efficiency, and tunable working potentials, representing attractive anode candidates for next‐generation, high‐performance, and low‐cost Li‐ion batteries.     

Approaching the Downsizing Limit of Maricite NaFePO4 toward High‐Performance Cathode for Sodium‐Ion Batteries

Maricite NaFePO₄ nanodots with minimized sizes (≈1.6 nm) uniformly embedded in porous N‐doped carbon nanofibers (designated as NaFePO₄@C) are first prepared by electrospinning for maximized Na‐storage performance. The obtained flexible NaFePO₄@C fiber membrane adherent on aluminum foil is directly used as binder‐free cathode for sodium‐ion batteries, revealing that the ultrasmall nanosize effect as well as a high‐potential desodiation process can transform the generally perceived electrochemically inactive maricite NaFePO₄ into a highly active amorphous phase; meanwhile, remarkable electrochemical performance in terms of high reversible capacity (145 mA h g^?1 at 0.2 C), high rate capability (61 mA h g^?1 at 50 C), and unprecedentedly high cyclic stability (≈89% capacity retention over 6300 cycles) is achieved. Furthermore, the soft package Na‐ion full battery constructed by the NaFePO₄@C nanofibers cathode and the pure carbon nanofibers anode displays a promising energy density of 168.1 Wh kg^?1 and a notable capacity retention of 87% after 200 cycles. The distinctive 3D network structure of very fine NaFePO₄ nanoparticles homogeneously encapsulated in interconnected porous N‐doped carbon nanofibers, can effectively improve the active materials' utilization rate, facilitate the electrons/Na⁺ ions transport, and strengthen the electrode stability upon prolonged cycling, leading to the fascinating Na‐storage performance.     

Metal–Organic Framework (MOF) Derived Electrodes with Robust and Fast Lithium Storage for Li‐Ion Hybrid Capacitors

Hybrid metal–organic frameworks (MOFs) demonstrate great promise as ideal electrode materials for energy‐related applications. Herein, a well‐organized interleaved composite of graphene‐like nanosheets embedded with MnO₂ nanoparticles (MnO₂@C‐NS) using a manganese‐based MOF and employed as a promising anode material for Li‐ion hybrid capacitor (LIHC) is engineered. This unique hybrid architecture shows intriguing electrochemical properties including high reversible specific capacity 1054 mAh g^?1 (close to the theoretical capacity of MnO₂, 1232 mAh g^?1) at 0.1 A g^?1 with remarkable rate capability and cyclic stability (90% over 1000 cycles). Such a remarkable performance may be assigned to the hierarchical porous ultrathin carbon nanosheets and tightly attached MnO₂ nanoparticles, which provide structural stability and low contact resistance during repetitive lithiation/delithiation processes. Moreover, a novel LIHC is assembled using a MnO₂@C‐NS anode and MOF derived ultrathin nanoporous carbon nanosheets (derived from other potassium‐based MOFs) cathode materials. The LIHC full‐cell delivers an ultrahigh specific energy of 166 Wh kg^?1 at 550 W kg^?1 and maintained to 49.2 Wh kg^?1 even at high specific power of 3.5 kW kg^?1 as well as long cycling stability (91% over 5000 cycles). This work opens new opportunities for designing advanced MOF derived electrodes for next‐generation energy storage devices.     

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.     

Lithium Titanate Anode Thin Films for Li‐Ion Solid State Battery Based on Garnets

Solid state electrolytes, such as Li‐Garnets, are fastest Li‐ionic conductor materials that have attracted attention for safe hybrid and full solid state battery architectures. Turning to oxide‐based low voltage anodes gives opportunities to avoid Li‐dendrite formation and also to reach full thin film microbattery architectures based on garnets as high energy density replacement for supercapacitors. Herein, it is demonstrated that Li₄Ti₅O₁₂ thin films deposited by pulsed laser deposition can show stable structures and cycling kinetics reaching almost close to theoretical capacity of 175 mAh g^?1 when combined to Li_6.25Al_0.25La₃Zr₂O₁₂ pellets. Stable operation at room temperature with 90% of theoretical capacity retention at 2.5 mA g^?1 over 22 cycles is achieved on bilayer half cell batteries. Rate capability studies show promising charge and discharge capacities and act as a case study for the well‐known Li₄Ti₅O₁₂ thin film anode, demonstrating its good compatibility with the investigated solid garnet electrolyte. This gives new perspective on the use of oxide‐based low voltage anodes for future strategies avoiding Li‐dendrite formation or safe solid state microbattery thin film assemblies based on Li‐garnets.     

Controlled Design of Well‐Dispersed Ultrathin MoS2 Nanosheets inside Hollow Carbon Skeleton: Toward Fast Potassium Storage by Constructing Spacious “Houses” for K Ions

The large volume expansion induced by K⁺ intercalation is always a big challenge for designing high‐performance electrode materials in potassium‐ion storage system. Based on the idea that large‐sized ions should accommodate big “houses,” a facile‐induced growth strategy is proposed to achieve the self‐loading of MoS₂ clusters inside a hollow tubular carbon skeleton (HTCS). Meantime, a step‐by‐step intercalation technology is employed to tune the interlayer distance and the layer number of MoS₂. Based on the above, the ED‐MoS₂@CT hybrids are achieved by self‐loading and anchoring the well‐dispersed ultrathin MoS₂ nanosheets on the inner surface of HTCSs. This unique compositing model not only alleviates the mechanical strain efficiently, but also provides spacious “roads” (hollow tubular carbon skeleton) and “houses” (interlayer expanded ultrathin MoS₂ sheets) for fast K⁺ transition and storage. As an anode of potassium‐ion batteries, the resultant ED‐MoS₂@CT electrode delivers a high specific capacity of 148.5 mAh g^?1 at 2 A g^?1 after 10 000 cycles with only 0.002% fading per cycle. The assembled ED‐MoS₂@CT//PC potassium‐ion hybrid supercapacitor device shows a high energy density of 148 Wh kg^?1 at a power density of 965 W kg^?1, which is comparable to that of lithium‐ion hybrid supercapacitors.     

A High‐Energy Li‐Ion Battery Using a Silicon‐Based Anode and a Nano‐Structured Layered Composite Cathode

High capacity electrodes based on a Si composite anode and a layered composite oxide cathode, Ni‐rich Li[Ni_0.75Co_0.1Mn_0.15]O₂, are evaluated and combined to fabricate a high energy lithium ion battery. The Si composite anode, Si/C‐IWGS (internally wired with graphene sheets), is prepared by a scalable sol–gel process. The Si/C‐IWGS anode delivers a high capacity of >800 mAh g^?1 with an excellent cycling stability of up to 200 cycles, mainly due to the small amount of graphene (～6 wt%). The cathode (Li[Ni_0.75Co_0.1Mn_0.15]O₂) is structurally optimized (Ni‐rich core and a Ni‐depleted shell with a continuous concentration gradient between the core and shell, i.e., a full concentration gradient, FCG, cathode) so as to deliver a high capacity (>200 mAh g^?1) with excellent stability at high voltage (～4.3 V). A novel lithium ion battery system based on the Si/C‐IWGS anode and FCG cathode successfully demonstrates a high energy density (240 Wh kg^?1 at least) as well as an unprecedented excellent cycling stability of up to 750 cycles between 2.7 and 4.2 V at 1C. As a result, the novel battery system is an attractive candidate for energy storage applications demanding a high energy density and long cycle life.     

All‐Purpose Electrode Design of Flexible Conductive Scaffold toward High‐Performance Li–S Batteries

The main obstacles that hinder the development of efficient lithium sulfur (Li–S) batteries are the polysulfide shuttling effect in sulfur cathode and the uncontrollable growth of dendritic Li in the anode. An all‐purpose flexible electrode that can be used both in sulfur cathode and Li metal anode is reported, and its application in wearable and portable storage electronic devices is demonstrated. The flexible electrode consists of a bimetallic CoNi nanoparticle‐embedded porous conductive scaffold with multiple Co/Ni‐N active sites (CoNi@PNCFs). Both experimental and theoretical analysis show that, when used as the cathode, the CoNi and Co/Ni‐N active sites implanted on the porous CoNi@PNCFs significantly promote chemical immobilization toward soluble lithium polysulfides and their rapid conversion into insoluble Li₂S, and therefore effectively mitigates the polysulfide shuttling effect. Additionally, a 3D matrix constructed with porous carbonous skeleton and multiple active centers successfully induces homogenous Li growth, realizing a dendrite‐free Li metal anode. A Li–S battery assembled with S/CoNi@PNCFs cathode and Li/CoNi@PNCFs anode exhibits a high reversible specific capacity of 785 mAh g^?1 and long cycle performance at 5 C (capacity fading rate of 0.016% over 1500 cycles).     

High‐Performance,Low‐Cost,and Dense‐Structure Electrodes with High Mass Loading for Lithium‐Ion Batteries

Lithium‐ion batteries have undergone a remarkable development in the past 30 years. However, conventional electrodes are insufficient for the ever‐increasing demand of high‐energy batteries. Here, reported is a thick electrode with a dense structure, as an alternative to the commonly recognized porous framework. A low‐temperature sintering technology with the aid of aqueous solvent, high pressure, and an ion‐conductive additive is originally developed for preparing the LiCoO₂ (LCO)/Li₄Ti₅O₁₂ (LTO) dense‐structure electrode as the representative cathode/anode material. The 400 µm thick cathode with 110 mg cm^?2 mass loading achieves a high specific capacity of 131.2 mAh g^?1 with a good capacity retention of 96% over 150 cycles, far exceeding the commercial counterpart (≈40 µm) of 54.1 mAh g^?1 with 39%. The ultrathick electrode of 1300 µm thickness presents a remarkable area capacity of 28.6 mAh cm^?2 that is 16 times that of the commercial electrode. The full cell based on the dense electrodes delivers an extremely high areal capacity of 14.4 mAh cm^?2. The ion‐diffusion coefficients of the densely sintered electrodes increase by nearly three orders of magnitude. This design opens up a new avenue for scalable and sustainable material manufacturing towards various practical applications.     

Sodium Storage Behavior in Natural Graphite using Ether‐based Electrolyte Systems

This work reports that natural graphite is capable of Na insertion and extraction with a remarkable reversibility using ether‐based electrolytes. Natural graphite (the most well‐known anode material for Li–ion batteries) has been barely studied as a suitable anode for Na rechargeable batteries due to the lack of Na intercalation capability. Herein, graphite is not only capable of Na intercalation but also exhibits outstanding performance as an anode for Na ion batteries. The graphite anode delivers a reversible capacity of ≈150 mAh g^?1 with a cycle stability for 2500 cycles, and more than 75 mAh g^?1 at 10 A g^?1 despite its micrometer‐size (≈100 μm). An Na storage mechanism in graphite, where Na⁺‐solvent co‐intercalation occurs combined with partial pseudocapacitive behaviors, is revealed in detail. It is demonstrated that the electrolyte solvent species significantly affect the electrochemical properties, not only rate capability but also redox potential. The feasibility of graphite in a Na full cell is also confirmed in conjunction with the Na_1.5VPO_4.8F_0.7 cathode, delivering an energy of ≈120 Wh kg^?1 while maintaining ≈70% of the initial capacity after 250 cycles. This exceptional behavior of natural graphite promises new avenues for the development of cost‐effective and reliable Na ion batteries.