Graphene Oxide Gel‐Derived,Free‐Standing,Hierarchically Porous Carbon for High‐Capacity and High‐Rate Rechargeable Li‐O2 Batteries

Lithium‐oxygen (Li‐O₂) batteries are one of the most promising candidates for high‐energy‐density storage systems. However, the low utilization of porous carbon and the inefficient transport of reactants in the cathode limit terribly the practical capacity and, in particular, the rate capability of state‐of‐the‐art Li‐O₂ batteries. Here, free‐standing, hierarchically porous carbon (FHPC) derived from graphene oxide (GO) gel in nickel foam without any additional binder is synthesized by a facile and effective in situ sol‐gel method, wherein the GO not only acts as a special carbon source, but also provides the framework of a 3D gel; more importantly, the proper acidity via its intrinsic COOH groups guarantees the formation of the whole structure. Interestingly, when employed as a cathode for Li‐O₂ batteries, the capacity reaches 11 060 mA h g^?1 at a current density of 0.2 mA cm^?2 (280 mA g^?1); and, unexpectedly, a high capacity of 2020 mA h g^?1 can be obtained even the current density increases ten times, up to 2 mA cm^?2 (2.8 A g^?1), which is the best rate performance for Li‐O₂ batteries reported to date. This excellent performance is attributed to the synergistic effect of the loose packing of the carbon, the hierarchical porous structure, and the high electronic conductivity of the Ni foam.     

Au‐Decorated Cracked Carbon Tube Arrays as Binder‐Free Catalytic Cathode Enabling Guided Li2O2 Inner Growth for High‐Performance Li‐O2 Batteries

Owing to their extremely high energy density, Li‐O₂ batteries have attained increasing attention in recent studies. However, deposition of the discharge product, insulating Li₂O₂, is known to seriously limit the electrochemical performance of Li‐O₂ batteries. While extensive studies have focused on relieving electrode deactivation by controlling Li₂O₂ growth, no permanent or effective mechanism is delivered. Here, a unique design comprising a catalytic cathode constructed by cracked carbon submicron tube (CST) arrays decorated with Au nanoparticles on inner walls is proposed. The introduction of Au nanoparticles not only improves electrode conductivity but also provides catalytic sites, guiding conformal growth of thin‐layered Li₂O₂ inside the cracked CST. Density functional theory calculations support that Au decoration on CST favors the conformal growth of Li₂O₂ on inner tubular walls. This growth behavior of Li₂O₂ renders easy decomposition of Li₂O₂, prevents carbon tube electrode from full, rapid deactivation, and preserves the free space for reactants transport. Li‐O₂ cells with Au@CST exhibit good rate capability (1208 mAh g^–1 at a high current density of 1000 mA g^–1) and long cycle life (112 cycles at a current density of 400 mA g^–1 with a limited capacity of 500 mAh g^–1).     

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.     

A Composite of Carbon‐Wrapped Mo2C Nanoparticle and Carbon Nanotube Formed Directly on Ni Foam as a High‐Performance Binder‐Free Cathode for Li‐O2 Batteries

Cathode design is indispensable for building Li‐O₂ batteries with long cycle life. A composite of carbon‐wrapped Mo₂C nanoparticles and carbon nanotubes is prepared on Ni foam by direct hydrolysis and carbonization of a gel composed of ammonium heptamolybdate tetrahydrate and hydroquinone resin. The Mo₂C nanoparticles with well‐controlled particle size act as a highly active oxygen reduction reactions/oxygen evolution reactions (ORR/OER) catalyst. The carbon coating can prevent the aggregation of the Mo₂C nanoparticles. The even distribution of Mo₂C nanoparticles results in the homogenous formation of discharge products. The skeleton of porous carbon with carbon nanotubes protrudes from the composite, resulting in extra voids when applied as a cathode for Li‐O₂ batteries. The batteries deliver a high discharge capacity of ≈10 400 mAh g^?1 and a low average charge voltage of ≈4.0 V at 200 mA g^?1. With a cutoff capacity of 1000 mAh g^?1, the Li‐O₂ batteries exhibit excellent charge–discharge cycling stability for over 300 cycles. The average potential polarization of discharge/charge gaps is only ≈0.9 V, demonstrating the high ORR and OER activities of these Mo₂C nanoparticles. The excellent cycling stability and low potential polarization provide new insights into the design of highly reversible and efficient cathode materials for Li‐O₂ batteries.     

Enhancing Ultrafast Lithium Ion Storage of Li4Ti5O12 by Tailored TiC/C Core/Shell Skeleton Plus Nitrogen Doping

It is of great importance to reinforce electronic and ionic conductivity of Li₄Ti₅O₁₂ electrodes to achieve fast reaction kinetics and good high‐power capability. Herein, for the first time, a dual strategy of combing N‐doped Li₄Ti₅O₁₂ (N‐LTO) with highly conductive TiC/C skeleton to realize enhanced ultrafast Li ion storage is reported. Interlinked hydrothermal‐synthesized N‐LTO nanosheets are homogeneously decorated on the chemical vapor deposition (CVD) derived TiC/C nanowires forming binder‐free N‐LTO@TiC/C core–branch arrays. Positive advantages including large surface area, strong mechanical stability, and enhanced electronic/ionic conductivity are obtained in the designed integrated arrays and rooted upon synergistic TiC/C matrix and N doping. The above appealing features can effectively boost kinetic properties throughout the N‐LTO@TiC/C electrodes to realize outstanding high‐rate capability at different working temperatures (143 mAh g^?1/10 C at 25 °C and 122 mAh g^?1/50 C at 50 °C) and notable cycling stability with a capacity retention of 99.3% after 10 000 cycles at 10 C. Moreover, superior high‐rate cycling life is also demonstrated for the full cells with N‐LTO@TiC/C anode and LiFePO₄ cathode. The dual strategy may provoke wide interests in fast energy storage areas and motivate the further performance improvement of power‐type lithium ion batteries (LIBs).     

Platinum‐Coated Hollow Graphene Nanocages as Cathode Used in Lithium‐Oxygen Batteries

One of the formidable challenges facing aprotic lithium‐oxygen (Li‐O₂) batteries is the high charge overpotential, which induces the formation of byproducts, loss in efficiency, and poor cycling performance. Herein, the synthesis of the ultrasmall Pt‐coated hollow graphene nanocages as cathode in Li‐O₂ batteries is reported. The charge voltage plateau can reduce to 3.2 V at the current density of 100 mA g^?1, even maintain below 3.5 V when the current density increased to 500 mA g^?1. The unique hollow graphene nanocages matrix can not only provide numerous nanoscale tri‐phase regions as active sites for efficient oxygen reduction, but also offer sufficient amount of mesoscale pores for rapid oxygen diffusion. Furthermore, with strong atomic‐level oxygen absorption into its subsurface, ultrasmall Pt catalytically serves as the nucleation site for Li₂O₂ growth. The Li₂O₂ is subsequently induced into a favorable form with small size and amorphous state, decomposed more easily during recharge. Meanwhile, the conductive hollow graphene substrate can enhance the catalytic activity of noble metal Pt catalysts due to the graphene‐metal interfacial interaction. Benefiting from the above synergistic effects between the hollow graphene nanocages and the nanosized Pt catalysts, the ultrasmall Pt‐decorated graphene nanocage cathode exhibits enhanced electrochemical performances.     

Fluorinated Polyimide as a Novel High‐Voltage Binder for High‐Capacity Cathode of Lithium‐Ion Batteries

An increase in the energy density of lithium‐ion batteries has long been a competitive advantage for advanced wireless devices and long‐driving electric vehicles. Li‐rich layered oxide, xLi₂MnO₃?(1?x)LiMn_1?y?zNi_yCo_zO₂, is a promising high‐capacity cathode material for high‐energy batteries, whose capacity increases by increasing charge voltage to above 4.6 V versus Li. Li‐rich layered oxide cathode however suffers from a rapid capacity fade during the high‐voltage cycling because of instable cathode–electrolyte interface, and the occurrence of metal dissolution, particle cracking, and structural degradation, particularly, at elevated temperatures. Herein, this study reports the development of fluorinated polyimide as a novel high‐voltage binder, which mitigates the cathode degradation problems through superior binding ability to conventional polyvinylidenefluoride binder and the formation of robust surface structure at the cathode. A full‐cell consisting of fluorinated polyimide binder‐assisted Li‐rich layered oxide cathode and conventional electrolyte without any electrolyte additive exhibits significantly improved capacity retention to 89% at the 100th cycle and discharge capacity to 223–198 mA h g^?1 even under the harsh condition of 55 °C and high charge voltage of 4.7 V, in contrast to a rapid performance fade of the cathode coated with polyvinylidenefluoride binder.     

A New Strategy to Build a High‐Performance P′2‐Type Cathode Material through Titanium Doping for Sodium‐Ion Batteries

Herein, Ti⁴⁺ in P′2‐Na_0.67[(Mn_0.78Fe_0.22)_0.9Ti_0.1]O₂ is proposed as a new strategy for optimization of Mn‐based cathode materials for sodium‐ion batteries, which enables a single phase reaction during de‐/sodiation. The approach is to utilize the stronger Ti–O bond in the transition metal layers that can suppress the movements of Mn–O and Fe–O by sharing the oxygen with Ti by the sequence of Mn–O–Ti–O–Fe. It delivers a discharge capacity of ≈180 mAh g^?1 over 200 cycles (86% retention), with S‐shaped smooth charge–discharge curves associated with a small volume change during cycling. The single phase reaction with a small volume change is further confirmed by operando synchrotron X‐ray diffraction. The low activation barrier energy of ≈541 meV for Na⁺ diffusion is predicted using first‐principles calculations. As a result, Na_0.67[(Mn_0.78Fe_0.22)_0.9Ti_0.1]O₂ can deliver a high reversible capacity of ≈153 mAh g^?1 even at 5C (1.3 A g^?1), which corresponds to ≈85% of the capacity at 0.1C (26 mA g^?1). The nature of the sodium storage mechanism governing the ultrahigh electrode performance in a full cell with a hard carbon anode is elucidated, revealing the excellent cyclability and good retention (≈80%) for 500 cycles (111 mAh g^?1) at 5C (1.3 A g^?1).     

A High‐Performance Li–B–H Electrolyte for All‐Solid‐State Li Batteries

Highly Li‐ion conductive Li₄(BH₄)₃I@SBA‐15 is synthesized by confining the LiI doped LiBH₄ into mesoporous silica SBA‐15. Uniform nanoconfinement of P6₃ mc phase Li₄(BH₄)₃I in SBA‐15 mesopores leads to a significantly enhanced conductivity of 2.5 × 10^?4 S cm^?1 with a Li‐ion transference number of 0.97 at 35 °C. The super Li‐ion mobility in the interface layer with a thickness of 1.2 nm between Li₄(BH₄)₃I and SBA‐15 is believed to be responsible for the fast Li‐ion conduction in Li₄(BH₄)₃I@SBA‐15. Additionally, Li₄(BH₄)₃I@SBA‐15 also exhibits a wide apparent electrochemical stability window (0 to 5 V vs Li/Li⁺) and a superior Li dendrite suppression capability (critical current density 2.6 mA cm^?2 at 55 °C) due to the formation of stable interphases. More importantly, Li₄(BH₄)₃I@SBA‐15‐based Li batteries using either high‐capacity sulfur cathode or high‐voltage oxide cathode show excellent electrochemical performances, making Li₄(BH₄)₃I@SBA‐15 a very attractive electrolyte for next‐generation all‐solid‐state Li batteries.     

3D Porous N‐Doped Graphene Frameworks Made of Interconnected Nanocages for Ultrahigh‐Rate and Long‐Life Li–O2 Batteries

The inferior rate capability and poor cycle stability of the present Li–O₂ batteries are still critical obstacles for practice applications. Configuring novel and integrated air electrode materials with unique structure and tunable chemical compositions is one of the efficient strategies to solve these bottleneck problems. Herein, a novel strategy for synthesis of 3D porous N‐doped graphene aerogels (NPGAs) with frameworks constructed by interconnected nanocages with the aid of polystyrene sphere@polydopamine is reported. The interconnected nanocages as the basic building unit of graphene sheets are assembled inside the skeletons of 3D graphene aerogels, leading to the 3D NPGA with well‐developed interconnected channels and the full exposure of electrochemically active sites. Benefiting from such an unique structure, the as‐made NPGA delivers a high specific capacity, an excellent rate capacity of 5978 mA h g^?1 at 3.2 A g^?1, and long cycle stability, especially at a large current density (54 cycles at 1 A g^?1), indicative of boosted rate capability and cycle life as air electrodes for Li–O₂ batteries. More importantly, based on the total mass of C+Li₂O₂, a gravimetric energy density of 2400 W h kg^?1 for the NPGA–O₂//Li cell is delivered at a power density of 1300 W kg^?1.     

Ultrathin MoS2 Nanosheets@Metal Organic Framework‐Derived N‐Doped Carbon Nanowall Arrays as Sodium Ion Battery Anode with Superior Cycling Life and Rate Capability

This study reports the design and fabrication of ultrathin MoS₂ nanosheets@metal organic framework‐derived N‐doped carbon nanowall array hybrids on flexible carbon cloth (CC@CN@MoS₂) as a free‐standing anode for high‐performance sodium ion batteries. When evaluated as an anode for sodium ion battery, the as‐fabricated CC@CN@MoS₂ electrode exhibits a high capacity (653.9 mA h g^?1 of the second cycle and 619.2 mA h g^?1 after 100 cycles at 200 mA g^?1), excellent rate capability, and long cycling life stability (265 mA h g^?1 at 1 A g^?1 after 1000 cycles). The excellent electrochemical performance can be attributed to the unique 2D hybrid structures, in which the ultrathin MoS₂ nanosheets with expanded interlayers can provide shortened ion diffusion paths and favorable Na⁺ insertion/extraction space, and the porous N‐doped carbon nanowall arrays on flexible carbon cloth are able to improve the conductivity and maintain the structural integrity. Moreover, the N‐doping‐induced defects also make them favorable for the effective storage of sodium ions, which enables the enhanced capacity and rate performance of MoS₂.     

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.     

Ti3+ Self‐Doped Dark Rutile TiO2 Ultrafine Nanorods with Durable High‐Rate Capability for Lithium‐Ion Batteries

Dark‐colored rutile TiO₂ nanorods doped by electroconducting Ti³⁺ have been obtained uniformly with an average diameter of ≈7 nm, and have been first utilized as anodes in lithium‐ion batteries. They deliver a high reversible specific capacity of 185.7 mAh g^?1 at 0.2 C (33.6 mA g^?1) and maintain 92.1 mAh g^?1 after 1000 cycles at an extremely high rate 50 C with an outstanding retention of 98.4%. Notably, the coulombic efficiency of Ti³⁺–TiO₂ has been improved by approximately 10% compared with that of pristine rutile TiO₂, which can be mainly attributed to its prompt electron transfer because of the introduction of Ti³⁺. Again the synergetic merits are noticed when the promoted electronic conductivity is combined with a shortened Li⁺ diffusion length resulting from the ultrafine nanorod structure, giving rise to the remarkable rate capabilities and extraordinary cycling stabilities for applications in fast and durable charge/discharge batteries. It is of great significance to incorporate Ti³⁺ into rutile TiO₂ to exhibit particular electrochemical characteristics triggering an effective way to improve the energy storage properties.     

Quasi‐Stable Electroless Ni–P Deposition: A Pivotal Strategy to Create Flexible Li–S Pouch Batteries with Bench Mark Cycle Stability and Specific Capacity

Development of flexible Li–S batteries brings along the flourishing prospective for energy‐hungry wearable devices. However, it is still seriously restricted due to lack of facile methods to solve its inherent problems and flexible device‐related current collection issues. Herein, quasi‐stable electroless deposition method is firstly proposed to solve these problems by fabricating 3D tunable Ni–P networks in the C/S free‐standing electrode. The ultrathin Ni–P layers which are highly conductive and strongly adhesive with electrode substrates improve the electronic conductivity by two orders of magnitude and rise initial specific capacity from 1200 to 1600 mAh g^?1. The harmful shuttle effect of polysulfide is also effectively alleviated due to the chemical adsorption and physical sieving properties of the 3D networks. The flexible pouch Li–S batteries assembled with commercially applicable structure also show high flexibility and as high as 1420 mAh g^?1 output capacity at 0.1C in cycling test. This method can definitely be extended to other flexible devices such as Li‐ion batteries, Li–O₂ batteries, and supercapacitors.     

Flexible Electrocatalytic Nanofiber Membrane Reactor for Lithium/Sulfur Conversion Chemistry

Severe lithium polysulfide (LiPS) shuttle effects and sluggish electrochemical conversion kinetics constitute bottlenecks in developing fast‐rechargeable, high‐energy, and high‐power Li/S batteries. Here, a flexible and conductive TiN–Ti₄O₇ core‐shell nanofiber (TiNOC) membrane reactor is designed to electrocatalytically mediate Li/S conversion chemistry. The Ti, N, and O atoms in the nanofiber function as electrocatalysts and chemical confinement active sites to initiate long‐chain LiPS conversion and phase change, as well as to suppress soluble LiPS shuttling. With a sulfur cathode‐membrane reactor module configuration, Li/S cells possess a high sulfur utilization of 91.20%, good rate capability of 869.10 mA h g^?1, and high capacity retention of 92.49%, with a coulomb efficiency of 99.57% after 200 cycles at 5 C. Density functional theory (DFT) calculations revealed that the optimized chemisorption configurations facilitate the elongation of Li? S and S? S bonds, as well as charge transfer along Ti? S and Li? N bonds, which favors bond breakage, bond formation, and the activation of solid‐state S₈, Li₂S₂, and Li₂S. Layer‐by‐layer module stacking provides Li/S batteries with a high areal sulfur loading of 12.00 mg cm^?2 to deliver a high areal capacity of 14.40 mA h cm^?2 at 2.26 mA. Two batteries in series can power real‐world applications such as light emitting diode (LED) bulbs with a high energy output of 69.00 mW h.     

Mesoporous Carbon Nanocube Architecture for High‐Performance Lithium–Oxygen Batteries

One of the major challenges to develop high‐performance lithium–oxygen (Li–O₂) battery is to find effective cathode catalysts and design porous architecture for the promotion of both oxygen reduction reactions and oxygen evolution reactions. Herein, the synthesis of mesoporous carbon nanocubes as a new cathode nanoarchitecture for Li–O₂ batteries is reported. The oxygen electrodes made of mesoporous carbon nanocubes contain numerously hierarchical mesopores and macropores, which can facilitate oxygen diffusion and electrolyte impregnation throughout the electrode, and provide sufficient spaces to accommodate insoluble discharge products. When they are applied as cathode catalysts, the Li–O₂ cells deliver discharge capacities of 26 100 mA h g^?1 at 200 mA g^?1, which is much higher than that of commercial carbon black catalysts. Furthermore, the mesoporous nanocube architecture can also serve as a conductive host structure for other highly efficient catalysts. For instance, the Ru functionalized mesoporous carbon nanocubes show excellent catalytic activities toward oxygen evolution reactions. Li–O₂ batteries with Ru functionalized mesoporous carbon nanocube catalysts demonstrate a high charge/discharge electrical energy efficiency of 86.2% at 200 mA g^?1 under voltage limitation and a good cycling performance up to 120 cycles at 400 mA g^?1 with the curtaining capacity of 1000 mA h g^?1.     

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.     

Highly Improved Rate Capability for a Lithium‐Ion Battery Nano‐Li4Ti5O12 Negative Electrode via Carbon‐Coated Mesoporous Uniform Pores with a Simple Self‐Assembly Method

A mesostructured spinel Li₄Ti₅O₁₂ (LTO)‐carbon nanocomposite (denoted as Meso‐LTO‐C) with large (>15 nm) and uniform pores is simply synthesized via block copolymer self‐assembly. Exceptionally high rate capability is then demonstrated for Li‐ion battery (LIB) negative electrodes. Polyisoprene‐block‐poly(ethylene oxide) (PI‐b‐PEO) with a sp²‐hybridized carbon‐containing hydrophobic block is employed as a structure‐directing agent. Then the assembled composite material is crystallized at 700 °C enabling conversion to the spinel LTO structure without loss of structural integrity. Part of the PI is converted to a conductive carbon that coats the pores of the Meso‐LTO‐C. The in situ pyrolyzed carbon not only maintains the porous mesostructure as the LTO is crystallized, but also improves the electronic conductivity. A Meso‐LTO‐C/Li cell then cycles stably at 10 C‐rate, corresponding to only 6 min for complete charge and discharge, with a reversible capacity of 115 mA h g^?1 with 90% capacity retention after 500 cycles. In sharp contrast, a Bulk‐LTO/Li cell exhibits only 69 mA h g^?1 at 10 C‐rate. Electrochemical impedance spectroscopy (EIS) with symmetric LTO/LTO cells prepared from Bulk‐LTO and Meso‐LTO‐C cycled in different potential ranges reveals the factors contributing to the vast difference between the rate‐capabilities. The carbon‐coated mesoporous structure enables highly improved electronic conductivity and significantly reduced charge transfer resistance, and a much smaller overall resistance is observed compared to Bulk‐LTO. Also, the solid electrolyte interphase (SEI)‐free surface due to the limited voltage window (>1 V versus Li/Li⁺) contributes to dramatically reduced resistance.     

Novel Cathode Materials for Na‐Ion Batteries Composed of Spoke‐Like Nanorods of Na[Ni0.61Co0.12Mn0.27]O2 Assembled in Spherical Secondary Particles

The development of high‐energy and high‐power density sodium‐ion batteries is a great challenge for modern electrochemistry. The main hurdle to wide acceptance of sodium‐ion batteries lies in identifying and developing suitable new electrode materials. This study presents a composition‐graded cathode with average composition Na[Ni_0.61Co_0.12Mn_0.27]O₂, which exhibits excellent performance and stability. In addition to the concentration gradients of the transition metal ions, the cathode is composed of spoke‐like nanorods assembled into a spherical superstructure. Individual nanorod particles also possess strong crystallographic texture with respect to the center of the spherical particle. Such morphology allows the spoke‐like nanorods to assemble into a compact structure that minimizes its porosity and maximizes its mechanical strength while facilitating Na⁺‐ion transport into the particle interior. Microcompression tests have explicitly verified the mechanical robustness of the composition‐graded cathode and single particle electrochemical measurements have demonstrated the electrochemical stability during Na⁺‐ion insertion and extraction at high rates. These structural and morphological features contribute to the delivery of high discharge capacities of 160 mAh (g oxide)^?1 at 15 mA g^?1 (0.1 C rate) and 130 mAh g^?1 at 1500 mA g^?1 (10 C rate). The work is a pronounced step forward in the development of new Na ion insertion cathodes with a concentration gradient.     

Engineering MoS2 Nanosheets on Spindle‐Like α‐Fe2O3 as High‐Performance Core–Shell Pseudocapacitive Anodes for Fiber‐Shaped Aqueous Lithium‐Ion Capacitors

Fiber‐shaped aqueous lithium‐ion capacitors (FALICs) featured with high energy and power densities together with outstanding safety characteristics are emerging as promising electrochemical energy‐storage devices for future portable and wearable electronics. However, the lack of high‐capacitance fibrous anodes is a major bottleneck to achieve high performance FALICs. Here, hierarchical MoS₂@α‐Fe₂O₃ core–shell heterostructures consisting of spindle‐shaped α‐Fe₂O₃ cores and MoS₂ nanosheet shells on a carbon nanotube fiber (CNTF) are successfully fabricated. Originating from the unique core/shell architecture and prominent synergetic effects for multi‐components, the resulting MoS₂@α‐Fe₂O₃/CNTF anode delivers a remarkable specific capacitance of 2077.5 mF cm^?2 (554.0 F cm^?3) at 2 mA cm^?2, substantially outperforming most of the previously reported fibrous anode materials. Further density functional theory calculations reveal that the MoS₂@α‐Fe₂O₃ nano‐heterostructure possesses better electrical conductivity and stronger adsorption energy of Li⁺ than those of the individual MoS₂ and α‐Fe₂O₃. By paring with the self‐standing LiCoO₂/CNTF battery‐type cathode, a prototype quasi‐solid‐state FALIC with a maximum operating voltage of 2.0 V is constructed, achieving impressive specific capacitance (253.1 mF cm^?2) and admirable energy density (39.6 mWh cm^?3). Additionally, the newly developed FALICs can be woven into the flexible textile to power wearable electronics. This work presents a novel effective strategy to design high‐performance anode materials for next‐generation wearable ALICs.