Fabrication of Hierarchical Potassium Titanium Phosphate Spheroids: A Host Material for Sodium‐Ion and Potassium‐Ion Storage

Identifying suitable electrode materials for sodium‐ion and potassium‐ion storage holds the key to the development of earth‐abundant energy‐storage technologies. This study reports an anode material based on self‐assembled hierarchical spheroid‐like KTi₂(PO₄)₃@C nanocomposites synthesized via an electrospray method. Such an architecture synergistically combines the advantages of the conductive carbon network and allows sufficient space for the infiltration of the electrolyte from the porous structure, leading to an impressive electrochemical performance, as reflected by the high reversible capacity (283.7 mA h g^?1 for Na‐ion batteries; 292.7 mA h g^?1 for K‐ion batteries) and superior rate capability (136.1 mA h g^?1 at 10 A g^?1 for Na‐ion batteries; 133.1 mA h g^?1 at 1 A g^?1 for K‐ion batteries) of the resulting material. Moreover, the different ion diffusion behaviors in the two systems are revealed to account for the difference in rate performance. These findings suggest that KTi₂(PO₄)₃@C is a promising candidate as an anode material for sodium‐ion and potassium‐ion batteries. In particular, the present synthetic approach could be extended to other functional electrode materials for energy‐storage materials.     

A Novel Aluminum‐Ion Battery: Al/AlCl3‐[EMIm]Cl/Ni3S2@Graphene

Due to an ever‐increasing demand for electronic devices, rechargeable batteries are attractive for energy storage systems. A novel rechargeable aluminum‐ion battery based on Al³⁺ intercalation and deintercalation is fabricated with Ni₃S₂/graphene microflakes composite as cathode material and high‐purity Al foil as anode. This kind of aluminum‐ion battery comprises of an electrolyte containing AlCl₃ in an ionic liquid of 1‐ethyl‐3‐methylimidazolium chloride ([EMIm]Cl). Galvanostatic charge/discharge measurements have been performed in a voltage range of 0.1–2.0 V versus Al/AlCl₄ ^?. An initial discharge specific capacity of 350 mA h g^?1 at a current density of 100 mA g^?1 is achieved, and the discharge capacity remains over 60 mA h g^?1 and coulombic efficiency of 99% after 100 cycles. Typically, for the current density at 200 mA g^?1, the initial charge and discharge capacities are 300 and 235 mA h g^?1, respectively. More importantly, it should be emphasized that the battery has a high discharge voltage plateau (≈1.0 V vs Al/AlCl₄ ^?). These meaningful results represent a significant step forward in the development of aluminum‐ion batteries.     

A High‐Energy NASICON‐Type Cathode Material for Na‐Ion Batteries

Over the last decade, Na‐ion batteries have been extensively studied as low‐cost alternatives to Li‐ion batteries for large‐scale grid storage applications; however, the development of high‐energy positive electrodes remains a major challenge. Materials with a polyanionic framework, such as Na superionic conductor (NASICON)‐structured cathodes with formula Na_xM₂(PO₄)₃, have attracted considerable attention because of their stable 3D crystal structure and high operating potential. Herein, a novel NASICON‐type compound, Na₄MnCr(PO₄)₃, is reported as a promising cathode material for Na‐ion batteries that deliver a high specific capacity of 130 mAh g^?1 during discharge utilizing high‐voltage Mn^2+/3+ (3.5 V), Mn^3+/4+ (4.0 V), and Cr^3+/4+ (4.35 V) transition metal redox. In addition, Na₄MnCr(PO₄)₃ exhibits a high rate capability (97 mAh g^?1 at 5 C) and excellent all‐temperature performance. In situ X‐ray diffraction and synchrotron X‐ray diffraction analyses reveal reversible structural evolution for both charge and discharge.     

Excellent Comprehensive Performance of Na‐Based Layered Oxide Benefiting from the Synergetic Contributions of Multimetal Ions

Na‐ion batteries are promising for large‐scale energy storage applications, but few cathode materials can be practically used because of the significant difficulty in synthesizing an electrode material with superior comprehensive performance. Herein, an effective strategy based on synergetic contributions of rationally selected metal ions is applied to design layered oxides with excellent electrochemical performances. The power of this strategy is demonstrated by the superior properties of as‐obtained NaFe_0.45Co_0.5Mg_0.05O₂ with 139.9 mA h g^?1 of reversible capacity, 3.1 V of average voltage, 96.6% of initial Coulombic efficiency, and 73.9 mA h g^?1 of capacity at 10 C rate, which benefit from the synergetic effect of Fe³⁺ (high redox potential), Co³⁺ (good kinetics), and inactive Mg²⁺ with compatible radii (stabilizing structure). Moreover, it is clarified that the superior property is not the simple superposition of performance for layered oxides with single metal ions. With the assistance of density functional theory calculations, it is evidenced that the wide capacity range (>70%) of prismatic Na⁺‐occupied sites during sodiation/desodiation is responsible for its high rate performance. This rational strategy of designing high‐performance cathodes based on the synergetic effect of various metal ions might be a powerful step forward in the development of new Na‐ion‐insertion cathodes.     

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.     

In Situ Synthesis of Hierarchical Core Double‐Shell Ti‐Doped LiMnPO4@NaTi2(PO4)3@C/3D Graphene Cathode with High‐Rate Capability and Long Cycle Life for Lithium‐Ion Batteries

Olivine‐type LiMnPO₄ (LMP) cathodes have gained enormous attraction for Li‐ion batteries (LIBs), thanks to their large theoretical capacity, high discharge platform, and thermal stability. However, it is still hugely challenging to achieve encouraging Li‐storage behaviors owing to their low electronic conductivity and limited lithium diffusion. Herein, the core double‐shell Ti‐doped LMP@NaTi₂(PO₄)₃@C/3D graphene (TLMP@NTP@C/3D‐G) architecture is designed and constructed via an in situ synthetic methodology. A continuous electronic conducting network is formed with the unfolded 3D‐G and conducting carbon nanoshell. The Nasicon‐type NTP nanoshell with exceptional ionic conductivity efficiently inhibits gradual enrichment in by‐products, and renders low surfacial/interfacial electron/ion‐diffusion resistance. Besides, a rapid Li⁺ diffusion in the bulk structure is guaranteed with the reduction of Mn_Li+˙ antisite defects originating from the synchronous Ti‐doping. Benefiting from synergetic contributions from these design rationales, the integrated TLMP@NTP@C/3D‐G cathode yields high initial discharge capacity of ≈164.8 mAh g^?1 at 0.05 C, high‐rate reversible capacity of ≈116.2 mAh g^?1 at 10 C, and long‐term capacity retention of ≈93.3% after 600 cycles at 2 C. More significantly, the electrode design developed here will exert significant impact upon constructing other advanced cathodes for high‐energy/power LIBs.     

A Dual‐Insertion Type Sodium‐Ion Full Cell Based on High‐Quality Ternary‐Metal Prussian Blue Analogs

Prussian blue analogs (PBAs) are especially investigated as superior cathodes for sodium‐ion batteries (SIBs) due to high theoretical capacity (≈170 mA h g^?1) with 2‐Na storage and low cost. However, PBAs suffer poor cyclability due to irreversible phase transition in deep charge/discharge states. PBAs also suffer low crystallinity, with considerable [Fe(CN)₆] vacancies, and coordinated water in crystal frameworks. Presently, a new chelating agent/surfactant coassisted crystallization method is developed to prepare high‐quality (HQ) ternary‐metal Ni_xCo_1?x[Fe(CN)₆] PBAs. By introducing inactive metal Ni to suppress capacity fading caused by excessive lattice distortion, these PBAs have tunable limits on depth of charge/discharge. HQ‐Ni_xCo_1?x[Fe(CN)₆] (x = 0.3) demonstrates the best reversible Na‐storage behavior with a specific capacity of ≈145 mA h g^?1 and a remarkably improved cycle performance, with ≈90% capacity retention over 600 cycles at 5 C. Furthermore, a dual‐insertion full cell on the cathode and NaTi₂(PO₄)₃ anode delivers reversible capacity of ≈110 mA h g^?1 at a current rate of 1.0 C without capacity fading over 300 cycles, showing promise as a high‐performance SIB for large‐scale energy‐storage systems. The ultrastable cyclability achieved in the lab and explained herein is far beyond that of any previously reported PBA‐based full cells.     

High Capacity and High‐Rate NASICON‐Na3.75V1.25Mn0.75(PO4)3 Cathode for Na‐Ion Batteries via Modulating Electronic and Crystal Structures

Sodium superionic conductor (NASICON) cathodes are attractive for Na‐ion battery applications as they exhibit both high structural stability and high sodium ion mobility. Herein, a comprehensive study is presented on the structural and electrochemical properties of the NASICON‐Na_3+yV_2?yMn_y(PO₄)₃ (0 ≤ y ≤ 1) series. A phase miscibility gap is observed at y = 0.5, defining two solid solution domains with low and high Mn contents. Although, members of each of these domains Na_3.25V_1.75Mn_0.25(PO₄)₃ and Na_3.75V_1.25Mn_0.75(PO₄)₃ reversibly exchange sodium ions with high structural integrity, the activity of the Mn³⁺/Mn²⁺ redox couple is found to be absent and present in the former and latter candidate, respectively. Galvanostatic cycling and rate studies reveal higher capacity and rate capability for the Na_3.75V_1.25Mn_0.75(PO₄)₃ cathode (100 and 89 mA h g^?1 at 1C and 5C rate, respectively) in the Na_3+yV_2?yMn_y(PO₄)₃ series. Such a remarkable performance is attributed to optimum bottleneck size (≈5 Ų) and modulated V‐ and Mn‐redox centers as deduced from Rietveld analysis and DFT calculations, respectively. This study shows how important it is to manipulate electronic and crystal structures to achieve high‐performance NASICON cathodes.     

Interpenetrating Triphase Cobalt‐Based Nanocomposites as Efficient Bifunctional Oxygen Electrocatalysts for Long‐Lasting Rechargeable Zn–Air Batteries

Rational construction of atomic‐scale interfaces in multiphase nanocomposites is an intriguing and challenging approach to developing advanced catalysts for both oxygen reduction (ORR) and evolution reactions (OER). Herein, a hybrid of interpenetrating metallic Co and spinel Co₃O₄ “Janus” nanoparticles stitched in porous graphitized shells (Co/Co₃O₄@PGS) is synthesized via ionic exchange and redox between Co²⁺ and 2D metal–organic‐framework nanosheets. This strategy is proven to effectively establish highways for the transfer of electrons and reactants within the hybrid through interfacial engineering. Specifically, the phase interpenetration of mixed Co species and encapsulating porous graphitized shells provides an optimal charge/mass transport environment. Furthermore, the defect‐rich interfaces act as atomic‐traps to achieve exceptional adsorption capability for oxygen reactants. Finally, robust coupling between Co and N through intimate covalent bonds prohibits the detachment of nanoparticles. As a result, Co/Co₃O₄@PGS outperforms state‐of‐the‐art noble‐metal catalysts with a positive half‐wave potential of 0.89 V for ORR and a low potential of 1.58 V at 10 mA cm^?2 for OER. In a practical demonstration, ultrastable cyclability with a record lifetime of over 800 h at 10 mA cm^?2 is achieved by Zn–air batteries with Co/Co₃O₄@PGS within the rechargeable air electrode.     

Lithium‐Pretreated Hard Carbon as High‐Performance Sodium‐Ion Battery Anodes

Hard carbon (HC) is the state‐of‐the‐art anode material for sodium‐ion batteries (SIBs). However, its performance has been plagued by the limited initial Coulombic efficiency (ICE) and mediocre rate performance. Here, experimental and theoretical studies are combined to demonstrate the application of lithium‐pretreated HC (LPHC) as high‐performance anode materials for SIBs by manipulating the solid electrolyte interphase in tetraglyme (TEGDME)‐based electrolyte. The LPHC in TEGDME can 1) deliver > 92% ICE and ≈220 mAh g^?1 specific capacity, twice of the capacity (≈100 mAh g^?1) in carbonate electrolyte; 2) achieve > 85% capacity retention over 1000 cycles at 1000 mA g^?1 current density (4 C rate, 1 C = 250 mA g^?1) with a specific capacity of ≈150 mAh g^?1, ≈15 times of the capacity (10 mAh g^?1) in carbonate. The full cell of Na₃V₂(PO₄)₃‐LPHC in TEGDME demonstrated close to theoretical specific capacity of ≈98 mAh g^?1 based on Na₃V₂(PO₄)₃ cathode, ≈2.5 times of the value (≈40 mAh g^?1) with nontreated HC. This work provides new perception on the anode development for SIBs.     

3D‐Printed Cathodes of LiMn1−xFexPO4 Nanocrystals Achieve Both Ultrahigh Rate and High Capacity for Advanced Lithium‐Ion Battery

A 3D‐printing technology and printed 3D lithium‐ion batteries (3D‐printed LIBs) based on LiMn_0.21Fe_0.79PO₄@C (LMFP) nanocrystal cathodes are developed to achieve both ultrahigh rate and high capacity. Coin cells with 3D‐printed cathodes show impressive electrochemical performance: a capacity of 108.45 mAh g^?1 at 100 C and a reversible capacity of 150.21 mAh g^?1 at 10 C after 1000 cycles. In combination with simulation using a pseudo 2D hidden Markov model and experimental data of 3D‐printed and traditional electrodes, for the first time deep insight into how to achieve the ultrahigh rate performance for a cathode with LMFP nanocrystals is obtained. It is estimated that the Li‐ion diffusion in LMFP nanocrystal is not the rate‐limitation step for the rate to 100 C, however, that the electrolyte diffusion factors, such as solution intrinsic diffusion coefficient, efficiency porosity, and electrode thickness, will dominate ultrahigh rate performance of the cathode. Furthermore, the calculations indicate that the above factors play important roles in the equivalent diffusion coefficient with the electrode beyond a certain thickness, which determines the whole kinetic process in LIBs. This fundamental study should provide helpful guidance for future design of LIBs with superior electrochemical performance.     

Stabilized Co3+/Co4+ Redox Pair in In Situ Produced CoSe2−x‐Derived Cobalt Oxides for Alkaline Zn Batteries with 10 000‐Cycle Lifespan and 1.9‐V Voltage Plateau

In aqueous alkaline Zn batteries (AZBs), the Co³⁺/Co⁴⁺ redox pair offers a higher voltage plateau than its Co²⁺/Co³⁺ counterpart. However, related studies are scarce, due to two challenges: the Co³⁺/Co⁴⁺ redox pair is more difficult to activate than Co²⁺/Co³⁺; once activated, the Co³⁺/Co⁴⁺ redox pair is unstable, owing to the rapid reduction of surplus Co³⁺ to Co²⁺. Herein, CoSe_2?x is employed as a cathode material in AZBs. Electrochemical analysis recognizes the principal contributions of the Co³⁺/Co⁴⁺ redox pair to the capacity and voltage plateau. Mechanistic studies reveal that CoSe_2?x initially undergoes a phase transformation to derived Co_xO_ySe_z, which has not been observed in other Zn//cobalt oxide batteries. The Se doping effect is conducive to sustaining abundant and stable Co³⁺ species in Co_xO_ySe_z. As a result, the battery achieves a 10 000‐cycle ultralong lifespan with 0.02% cycle^?1 capacity decay, a 1.9‐V voltage plateau, and an immense areal specific capacity compared to its low‐valence oxide counterparts. When used in a quasi‐solid‐state electrolyte, as‐assembled AZB delivers 4200 cycles and excellent tailorability, a promising result for wearable applications. The presented effective strategy for obtaining long‐cyclability cathodes via a phase transformation‐induced heteroatom doping effect may promote high‐valence metal species mediation toward highly stable electrodes.     

Realizing Three‐Electron Redox Reactions in NASICON‐Structured Na3MnTi(PO4)3 for Sodium‐Ion Batteries

Developing multielectron reaction electrode materials is essential for achieving high specific capacity and high energy density in secondary batteries; however, it remains a great challenge. Herein, Na₃MnTi(PO₄)₃/C hollow microspheres with an open and stable NASICON framework are synthesized by a spray‐drying‐assisted process. When applied as a cathode material for sodium‐ion batteries, the resultant Na₃MnTi(PO₄)₃/C microspheres demonstrate fully reversible three‐electron redox reactions, corresponding to the Ti^3+/4+ (≈2.1 V), Mn^2+/3+ (≈3.5 V), and Mn^3+/4+ (≈4.0 V vs Na⁺/Na) redox couples. In situ X‐ray diffraction results reveals that both solid‐solution and two‐phase electrochemical reactions are involved in the sodiation/desodiation processes. The high specific capacity (160 mAh g^?1 at 0.2 C), outstanding cyclability (≈92% capacity retention after 500 cycles at 2 C), and the facile synthesis make the Na₃MnTi(PO₄)₃/C a prospective cathode material for sodium‐ion batteries.     

An Open‐Structured Matrix as Oxygen Cathode with High Catalytic Activity and Large Li2O2 Accommodations for Lithium–Oxygen Batteries

The nonaqueous lithium–oxygen (Li–O₂) battery is considered as one of the most promising candidates for next‐generation energy storage systems because of its very high theoretical energy density. However, its development is severely hindered by large overpotential and limited capacity, far less than theory, caused by sluggish oxygen redox kinetics, pore clogging by solid Li₂O₂ deposition, inferior Li₂O₂/cathode contact interface, and difficult oxygen transport. Herein, an open‐structured Co₉S₈ matrix with sisal morphology is reported for the first time as an oxygen cathode for Li–O₂ batteries, in which the catalyzing for oxygen redox, good Li₂O₂/cathode contact interface, favorable oxygen evolution, and a promising Li₂O₂ storage matrix are successfully achieved simultaneously, leading to a significant improvement in the electrochemical performance of Li–O₂ batteries. The intrinsic oxygen‐affinity revealed by density functional theory calculations and superior bifunctional catalytic properties of Co₉S₈ electrode are found to play an important role in the remarkable enhancement in specific capacity and round‐trip efficiency for Li–O₂ batteries. As expected, the Co₉S₈ electrode can deliver a high discharge capacity of ≈6875 mA h g^?1 at 50 mA g^?1 and exhibit a low overpotential of 0.57 V under a cutoff capacity of 1000 mA h g^?1, outperforming most of the current metal‐oxide‐based cathodes.     

Separator Modified by Cobalt‐Embedded Carbon Nanosheets Enabling Chemisorption and Catalytic Effects of Polysulfides for High‐Energy‐Density Lithium‐Sulfur Batteries

Lithium‐sulfur (Li‐S) batteries are considered to be one of the promising next‐generation energy storage systems. Considerable progress has been achieved in sulfur composite cathodes, but high cycling stability and discharging capacity at the expense of volumetric capacity have offset their advantages. Herein, a functional separator is presented by coating cobalt‐embedded nitrogen‐doped porous carbon nanosheets and graphene on one surface of a commercial polypropylene separator. The coating layer not only suppresses the polysulfide shuttle effect through chemical affinity, but also functions as an electrocatalyst to propel catalytic conversion of intercepted polysulfides. The slurry‐bladed carbon nanotubes/sulfur cathode with 90 wt% sulfur deliver high reversible capacity of 1103 mA h g^?1 and volumetric capacity of 1062 mA h cm^?3 at 0.2 C, and the freestanding carbon nanofibers/sulfur cathode provides a high discharging capacity of 1190 mA h g^?1 and volumetric capacity of 1136 mA h cm^?3 at high sulfur content of 78 wt% and sulfur loading of 10.5 mg cm^?2. The electrochemical performance is comparable with or even superior to those in the state‐of‐the‐art carbon‐based sulfur cathodes. The separator reported in this work holds great promise for the development of high‐energy‐density Li‐S batteries.     

Controlled Oxygen Redox for Excellent Power Capability in Layered Sodium‐Based Compounds

A high‐rate of oxygen redox assisted by cobalt in layered sodium‐based compounds is achieved. The rationally designed Na_0.6[Mg_0.2Mn_0.6Co_0.2]O₂ exhibits outstanding electrode performance, delivering a discharge capacity of 214 mAh g^?1 (26 mA g^?1) with capacity retention of 87% after 100 cycles. High rate performance is also achieved at 7C (1.82 A g^?1) with a capacity of 107 mAh g^?1. Surprisingly, the Na_0.6[Mg_0.2Mn_0.6Co_0.2]O₂ compound is able to deliver capacity for 1000 cycles at 5C (at 1.3 A g^?1), retaining 72% of its initial capacity of 108 mAh g^?1. X‐ray absorption spectroscopy analysis of the O K‐edge indicates the oxygen‐redox species (O^2?/1?) is active during cycling. First‐principles calculations show that the addition of Co reduces the bandgap energy from ≈2.65 to ≈0.61 eV and that overlapping of the Co 3d and O 2p orbitals facilitates facile electron transfer, enabling the long‐term reversibility of the oxygen redox, even at high rates. To the best of the authors' knowledge, this is the first report on high‐rate oxygen redox in sodium‐based cathode materials, and it is believed that the findings will open a new pathway for the use of oxygen‐redox‐based materials for sodium‐ion batteries.     

High Voltage Operation of Ni‐Rich NMC Cathodes Enabled by Stable Electrode/Electrolyte Interphases

The lithium (Li) metal battery (LMB) is one of the most promising candidates for next‐generation energy storage systems. However, it is still a significant challenge to operate LMBs with high voltage cathodes under high rate conditions. In this work, an LMB using a nickel‐rich layered cathode of LiNi_0.76Mn_0.14Co_0.10O₂ (NMC76) and an optimized electrolyte [0.6 m lithium bis(trifluoromethanesulfonyl)imide + 0.4 m lithium bis(oxalato)borate + 0.05 m LiPF₆ dissolved in ethylene carbonate and ethyl methyl carbonate (4:6 by weight)] demonstrates excellent stability at a high charge cutoff voltage of 4.5 V. Remarkably, these Li||NMC76 cells can deliver a high discharge capacity of >220 mA h g^?1 (846 W h kg^?1) and retain more than 80% capacity after 1000 cycles at high charge/discharge current rates of 2C/2C (1C = 200 mA g^?1). This excellent electrochemical performance can be attributed to the greatly enhanced structural/interfacial stability of both the Ni‐rich NMC76 cathode material and the Li metal anode using the optimized electrolyte.     

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.     

Chemical Synthesis of 3D Graphene‐Like Cages for Sodium‐Ion Batteries Applications

Sodium (Na) super ion conductor structured Na₃V₂(PO₄)₃ (NVP) is extensively explored as cathode material for sodium‐ion batteries (SIBs) due to its large interstitial channels for Na⁺ migration. The synthesis of 3D graphene‐like structure coated on NVP nanoflakes arrays via a one‐pot, solid‐state reaction in molten hydrocarbon is reported. The NVP nanoflakes are uniformly coated by the in situ generated 3D graphene‐like layers with the thickness of 3 nm. As a cathode material, graphene covered NVP nanoflakes exhibit excellent electrochemical performances, including close to theoretical reversible capacity (115.2 mA h g^?1 at 1 C), superior rate capability (75.9 mA h g^?1 at 200 C), and excellent cyclic stability (62.5% of capacity retention over 30000 cycles at 50 C). Furthermore, the 3D graphene‐like cages after removing NVP also serve as a good anode material and deliver a specific capacity of 242.5 mA h g^?1 at 0.1 A g^?1. The full SIB using these two cathode and anode materials delivers a high specific capacity (109.2 mA h g^?1 at 0.1 A g^?1) and good cycling stability (77.1% capacity retention over 200 cycles at 0.1 A g^?1).     

Densification by Compaction as an Effective Low‐Cost Method to Attain a High Areal Lithium Storage Capacity in a CNT@Co3O4 Sponge

Achieving a high areal capacity is essential for the transfer of outstanding laboratory electrode results to commercial applications and also to ensure there exists a capacity matched cathode and anode for a properly tuned battery. Despite intensive efforts, most electrode materials exhibit areal capacities lower than that of the graphite anodes (4 mA h cm^?2). An effective and low‐cost approach is reported to attain a high areal capacity via an intense densification by compacting a porous carbon nanotube sponge grafted with Co₃O₄ nanoparticles. The hybrid sponge can be compacted to a large degree (up to a tenfold densification) while still keeping its structural integrity and the 3D porous network. This method allows achieving a mass loading of up ?to 14.3 mg cm^?2 and an areal capacity of 12 mA h cm^?2 (at a current density of 200 mA g^?1) together with a gravimetric capacity of >800 mA h g^?1. This densification by compaction approach offers an effective and low‐cost strategy to develop high mass loading and areal capacity electrodes for practical energy storage systems.