Self‐Formed Electronic/Ionic Conductive Fe3S4 @ S @ 0.9Na3SbS4⋅0.1NaI Composite for High‐Performance Room‐Temperature All‐Solid‐State Sodium–Sulfur Battery

Fe₃S₄ @ S @ 0.9Na₃SbS₄?0.1NaI composite cathode is prepared through one‐step wet‐mechanochemical milling procedure. During milling process, ionic conduction pathway is self‐formed in the composite due to the formation of 0.9Na₃SbS₄?0.1NaI electrolyte without further annealing treatment. Meanwhile, the introduction of Fe₃S₄ can increase the electronic conductivity of the composite cathode by one order of magnitude and nearly double enhance the ionic conductivities. Besides, the aggregation of sulfur is effectively suppressed in the obtained Fe₃S₄ @ S @ 0.9Na₃SbS₄?0.1NaI composite, which will enhance the contact between sulfur and 0.9Na₃SbS₄?0.1NaI electrolyte, leading to a decreased interfacial resistance and improving the electrochemical kinetics of sulfur. Therefore, the resultant all‐solid‐state sodium–sulfur battery employing Fe₃S₄ @ S @ 0.9Na₃SbS₄?0.1NaI composite cathode shows discharge capacity of 808.7 mAh g^?1 based on Fe₃S₄@S and a normalized discharge capacity of 1040.5 mAh g^?1 for element S at 100 mA g^?1 for 30 cycles at room temperature. Moreover, the battery also exhibits excellent cycling stability with a reversible capacity of 410 mAh g^?1 at 500 mA g^?1 for 50 cycles, and superior rate capability with capacities of 952.4, 796.7, 513.7, and 445.6 mAh g^?1 at 50, 100, 200, and 500 mA g^?1, respectively. This facile strategy for sulfur‐based composite cathode is attractive for achieving room‐temperature sodium–sulfur batteries with superior electrochemical performance.     

SnS2/Co3S4 Hollow Nanocubes Anchored on S‐Doped Graphene for Ultrafast and Stable Na‐Ion Storage

SnS₂ has been widely studied as an anode material for sodium‐ion batteries (SIBs) based on the high theoretical capacity and layered structure. Unfortunately, rapid capacity decay associated with volume variation during cycling limits practical application. Herein, SnS₂/Co₃S₄ hollow nanocubes anchored on S‐doped graphene are synthesized for the first time via coprecipitation and hydrothermal methods. When applied as the anode for SIBs, the sample delivers a distinguished charge specific capacity of 1141.8 mAh g^?1 and there is no significant capacity decay (0.1 A g^?1 for 50 cycles). When the rate is increased to 0.5 A g^?1, it presents 845.7 mAh g^?1 after cycling 100 times. Furthermore, the composite also exhibits an ultrafast sodium storage capability where 392.9 mAh g^?1 can be obtained at 10 A g^?1 and the charging time is less than 3 min. The outstanding electrochemical properties can be ascribed to the enhancement of conductivity for the addition of S‐doped graphene and the existence of p–n junctions in the SnS₂/Co₃S₄ heterostructure. Moreover, the presence of mesopores between nanosheets can alleviate volume expansion during cycling as well as being beneficial for the migration of Na⁺.     

A Highly Conductive MOF of Graphene Analogue Ni3(HITP)2 as a Sulfur Host for High‐Performance Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries have been considered as one of the most promising energy storage systems owing to their high theoretical capacity and energy density. However, their commercial applications are obstructed by sluggish reaction kinetics and rapid capacity degradation mainly caused by polysulfide shuttling. Herein, the first attempt to utilize a highly conductive metal–organic framework (MOF) of Ni₃(HITP)₂ graphene analogue as the sulfur host material to trap and transform polysulfides for high‐performance Li–S batteries is made. Besides, the traditional conductive additive acetylene black is replaced by carbon nanotubes to construct matrix conduction networks for triggering the rate and cycling performance of the active cathode. As a result, the S@Ni₃(HITP)₂ with sulfur content of 65.5 wt% shows excellent sulfur utilization, rate performance, and cyclic durability. It delivers a high initial capacity of 1302.9 mAh g^?1 and good capacity retention of 848.9 mAh g^?1 after 100 cycles at 0.2 C. Highly reversible discharge capacities of 807.4 and 629.6 mAh g^?1 are obtained at 0.5 and 1 C for 150 and 300 cycles, respectively. Such kinds of pristine MOFs with high conductivity and abundant polar sites reveal broad promising prospect for application in the field of high‐performance Li–S batteries.     

Novel 2D Layered Molybdenum Ditelluride Encapsulated in Few‐Layer Graphene as High‐Performance Anode for Lithium‐Ion Batteries

Molybdenum ditelluride nanosheets encapsulated in few‐layer graphene (MoTe₂/FLG) are synthesized by a simple heating method using Te and Mo powder and subsequent ball milling with graphite. The as‐prepared MoTe₂/FLG nanocomposites as anode materials for lithium‐ion batteries exhibit excellent electrochemical performance with a highly reversible capacity of 596.5 mAh g^?1 at 100 mA g^?1, a high rate capability (334.5 mAh g^?1 at 2 A g^?1), and superior cycling stability (capacity retention of 99.5% over 400 cycles at 0.5 A g^?1). Ex situ X‐ray diffraction and transmission electron microscopy are used to explore the lithium storage mechanism of MoTe₂. Moreover, the electrochemical performance of a MoTe₂/FLG//0.35Li₂MnO₃·0.65LiMn_0.5Ni_0.5O₂ full cell is investigated, which displays a reversible capacity of 499 mAh g^?1 (based on the MoTe₂/FLG mass) at 100 mA g^?1 and a capacity retention of 78% over 50 cycles, suggesting the promising application of MoTe₂/FLG for lithium‐ion storage. First‐principles calculations exhibit that the lowest diffusion barrier (0.18 eV) for lithium ions along pathway III in the MoTe₂ layered structure is beneficial for improving the Li intercalation/deintercalation property.     

Glucose‐Induced Synthesis of 1T‐MoS2/C Hybrid for High‐Rate Lithium‐Ion Batteries

1T phase MoS₂ possesses higher conductivity than the 2H phase, which is a key parameter of electrochemical performance for lithium ion batteries (LIBs). Herein, a 1T‐MoS₂/C hybrid is successfully synthesized through facile hydrothermal method with a proper glucose additive. The synthesized hybrid material is composed of smaller and fewer‐layer 1T‐MoS₂ nanosheets covered by thin carbon layers with an enlarged interlayer spacing of 0.94 nm. When it is used as an anode material for LIBs, the enlarged interlayer spacing facilitates rapid intercalating and deintercalating of lithium ions and accommodates volume change during cycling. The high intrinsic conductivity of 1T‐MoS₂ also contributes to a faster transfer of lithium ions and electrons. Moreover, much smaller and fewer‐layer nanosheets can shorten the diffusion path of lithium ions and accelerate reaction kinetics, leading to an improved electrochemical performance. It delivers a high initial capacity of 920.6 mAh g^?1 at 1 A g^?1 and the capacity can maintain 870 mAh g^?1 even after 300 cycles, showing a superior cycling stability. The electrode presents a high rate performance as well with a reversible capacity of 600 mAh g^?1 at 10 A g^?1. These results show that the 1T‐MoS₂/C hybrid shows potential for use in high‐performance lithium‐ion batteries.     

NixMnyCozO Nanowire/CNT Composite Microspheres with 3D Interconnected Conductive Network Structure via Spray‐Drying Method: A High‐Capacity and Long‐Cycle‐Life Anode Material for Lithium‐Ion Batteries

The combination of high‐capacity and long‐term cycling stability is an important factor for practical application of anode materials for lithium‐ion batteries. Herein, Ni_xMn_yCo_zO nanowire (x + y + z = 1)/carbon nanotube (CNT) composite microspheres with a 3D interconnected conductive network structure (3DICN‐NCS) are prepared via a spray‐drying method. The 3D interconnected conductive network structure can facilitate the penetration of electrolyte into the microspheres and provide excellent connectivity for rapid Li⁺ ion/electron transfer in the microspheres, thus greatly reducing the concentration polarization in the electrode. Additionally, the empty spaces among the nanowires in the network accommodate microsphere volume expansion associated with Li⁺ intercalation during the cycling process, which improves the cycling stability of the electrode. The CNTs distribute uniformly in the microspheres, which act as conductive frameworks to greatly improve the electrical conductivity of the microspheres. As expected, the prepared 3DICN‐NCS demonstrates excellent electrochemical performance, showing a high capacity of 1277 mAh g^?1 at 1 A g^?1 after 2000 cycles and 790 mAh g^?1 at 5 A g^?1 after 1000 cycles. This work demonstrates a universal method to construct a 3D interconnected conductive network structure for anode materials     

Ultrafine Co3O4 Nanoparticles within Nitrogen‐Doped Carbon Matrix Derived from Metal–Organic Complex for Boosting Lithium Storage and Oxygen Evolution Reaction

Transition metal oxides have recently received great attention for application in advanced lithium‐ion batteries (LIBs) and oxygen evolution reaction (OER). Herein, the ethylenediaminetetraacetic cobalt complex as a precursor to synthesize ultrafine Co₃O₄ nanoparticles encapsulated into a nitrogen‐doped carbon matrix (NC) composites is presented. The as‐prepared Co₃O₄/NC‐350 obtained by pyrolysis at 350 °C demonstrates superior rate performance (372 mAh g^?1 at 5.0 A g^?1) and high cycling stability (92% capacity retention after 300 cycles at 1.0 A g^?1) as anode for LIBs. When evaluated as an electrocatalyst for OER, the Co₃O₄/NC‐350 achieves an overpotential of 298 mV at a current density of 10 mA cm^?2. The NC‐encapsualted porous hierarchical structure assures fast and continuous electron transportation, high activity sites, and strong structural integrity. This works offers novel complex precursors for synthesizing transition metal–based electrodes for boosting electrochemical energy conversion and storage.     

Strong Surface‐Bound Sulfur in Carbon Nanotube Bridged Hierarchical Mo2C‐Based MXene Nanosheets for Lithium–Sulfur Batteries

In this work, hydroxyl‐functionalized Mo₂C‐based MXene nanosheets are synthesized by facilely removing the Sn layer of Mo₂SnC. The hydroxyl‐functionalized surface of Mo₂C suppresses the shuttle effect of lithium polysulfides (LiPSs) through strong interaction between Mo atoms on the MXenes surface and LiPSs. Carbon nanotubes (CNTs) are further introduced into Mo₂C phase to enlarge the specific surface area of the composite, improve its electronic conductivity, and alleviate the volume change during discharging/charging. The strong surface‐bound sulfur in the hierarchical Mo₂C‐CNTs host can lead to a superior electrochemical performance in lithium–sulfur batteries. A large reversible capacity of ≈925 mAh g ^{? 1} is observed after 250 cycles at a current density of 0.1 C (1 C = 1675 mAh g^?1) with good rate capability. Notably, the electrodes with high loading amounts of sulfur can also deliver good electrochemical performances, i.e., initial reversible capacities of ≈1314 mAh g^?1 (2.4 mAh cm^?2), ≈1068 mAh g^?1 (3.7 mAh cm^?2), and ≈959 mAh g^?1 (5.3 mAh cm^?2) at various areal loading amounts of sulfur (1.8, 3.5, and 5.6 mg cm^?2) are also observed, respectively.     

Solvent‐Free Synthesis of Uniform MOF Shell‐Derived Carbon Confined SnO2/Co Nanocubes for Highly Reversible Lithium Storage

Tin dioxide (SnO₂) has attracted much attention in lithium‐ion batteries (LIBs) due to its abundant source, low cost, and high theoretical capacity. However, the large volume variation, irreversible conversion reaction limit its further practical application in next‐generation LIBs. Here, a novel solvent‐free approach to construct uniform metal–organic framework (MOF) shell‐derived carbon confined SnO₂/Co (SnO₂/Co@C) nanocubes via a two‐step heat treatment is developed. In particular, MOF‐coated CoSnO₃ hollow nanocubes are for the first time synthesized as the intermediate product by an extremely simple thermal solid‐phase reaction, which is further developed as a general strategy to successfully obtain other uniform MOF‐coated metal oxides. The as‐synthesized SnO₂/Co@C nanocubes, when tested as LIB anodes, exhibit a highly reversible discharge capacity of 800 mAh g^?1 after 100 cycles at 200 mA g^?1 and excellent cycling stability with a retained capacity of 400 mAh g^?1 after 1800 cycles at 5 A g^?1. The experimental analyses demonstrate that these excellent performances are mainly ascribed to the delicate structure and a synergistic effect between Co and SnO₂. This facile synthetic approach will greatly contribute to the development of functional metal oxide‐based and MOF‐assisted nanostructures in many frontier applications.     

Multidimensional Integrated Chalcogenides Nanoarchitecture Achieves Highly Stable and Ultrafast Potassium‐Ion Storage

Potassium‐ion batteries (KIBs) have come into the spotlight in large‐scale energy storage systems because of cost‐effective and abundant potassium resources. However, the poor rate performance and problematic cycle life of existing electrode materials are the main bottlenecks to future potential applications. Here, the first example of preparing 3D hierarchical nanoboxes multidimensionally assembled from interlayer‐expanded nano‐2D MoS₂@dot‐like Co₉S₈ embedded into a nitrogen and sulfur codoped porous carbon matrix (Co₉S₈/NSC@MoS₂@NSC) for greatly boosting the electrochemical properties of KIBs in terms of reversible capacity, rate capability, and cycling lifespan, is reported. Benefiting from the synergistic effects, Co₉S₈/NSC@MoS₂@NSC manifest a very high reversible capacity of 403 mAh g^?1 at 100 mA g^?1 after 100 cycles, an unprecedented rate capability of 141 mAh g^?1 at 3000 mA g^?1 over 800 cycles, and a negligible capacity decay of 0.02% cycle^?1, boosting promising applications in high‐performance KIBs. Density functional theory calculations demonstrate that Co₉S₈/NSC@MoS₂@NSC nanoboxes have large adsorption energy and low diffusion barriers during K‐ion storage reactions, implying fast K‐ion diffusion capability. This work may enlighten the design and construction of advanced electrode materials combined with strong chemical bonding and integrated functional advantages for future large‐scale stationary energy storage.     

Construction of 3D Electronic/Ionic Conduction Networks for All‐Solid‐State Lithium Batteries

High and balanced electronic and ionic transportation networks with nanoscale distribution in solid‐state cathodes are crucial to realize high‐performance all‐solid‐state lithium batteries. Using Cu₂SnS₃ as a model active material, such a kind of solid‐state Cu₂SnS₃@graphene‐Li₇P₃S₁₁ nanocomposite cathodes are synthesized, where 5–10 nm Cu₂SnS₃ nanoparticles homogenously anchor on the graphene nanosheets, while the Li₇P₃S₁₁ electrolytes uniformly coat on the surface of Cu₂SnS₃@graphene composite forming nanoscaled electron/ion transportation networks. The large amount of nanoscaled triple‐phase boundary in cathode ensures high power density due to high ionic/electronic conductions and long cycle life due to uniform and reduced volume change of nano‐Cu₂SnS_3. The Cu₂SnS₃@graphene‐Li₇P₃S₁₁ cathode layer with 2.0 mg cm^?2 loading in all‐solid‐state lithium batteries demonstrates a high reversible discharge specific capacity of 813.2 mAh g^?1 at 100 mA g^?1 and retains 732.0 mAh g^?1 after 60 cycles, corresponding to a high energy density of 410.4 Wh kg^?1 based on the total mass of Cu₂SnS₃@graphene‐Li₇P₃S₁₁ composite based cathode. Moreover, it exhibits excellent rate capability and high‐rate cycling stability, showing reversible capacity of 363.5 mAh g^?1 at 500 mA g^?1 after 200 cycles. The study provides a new insight into constructing both electronic and ionic conduction networks for all‐solid‐state lithium batteries.     

Boosting High‐Rate Sodium Storage Performance of N‐Doped Carbon‐Encapsulated Na3V2(PO4)3 Nanoparticles Anchoring on Carbon Cloth

The further development of high‐power sodium‐ion batteries faces the severe challenge of achieving high‐rate cathode materials. Here, an integrated flexible electrode is constructed by smart combination of a conductive carbon cloth fiber skeleton and N‐doped carbon (NC) shell on Na₃V₂(PO₄)₃ (NVP) nanoparticles via a simple impregnation method. In addition to the great electronic conductivity and high flexibility of carbon cloth, the NC shell also promotes ion/electron transport in the electrode. The flexible NVP@NC electrode renders preeminent rate capacities (80.7 mAh g^?1 at 50 C for cathode; 48 mAh g^?1 at 30 C for anode) and superior cycle performance. A flexible symmetric NVP@NC//NVP@NC full cell is endowed with fairly excellent rate performance as well as good cycle stability. The results demonstrate a powerful polybasic strategy design for fabricating electrodes with optimal performance.     

Formation of Septuple‐Shelled (Co2/3Mn1/3)(Co5/6Mn1/6)2O4 Hollow Spheres as Electrode Material for Alkaline Rechargeable Battery

The multishelled (Co_2/3Mn_1/3)(Co_5/6Mn_1/6)2O₄ hollow microspheres with controllable shell numbers up to septuple shells are synthesized using developed sequential templating method. Exhilaratingly, the septuple‐shelled complex metal oxide hollow microsphere is synthesized for the first time by doping Mn into Co₃O₄, leading to the change of crystalline rate of precursor. Used as electrode materials for alkaline rechargeable battery, it shows a remarkable reversible capacity (236.39 mAh g^?1 at a current density of 1 A g^?1 by three‐electrode system and 106.85 mAh g^?1 at 0.5 A g^?1 in alkaline battery) and excellent cycling performance due to its unique structure.     

Pistachio‐Shuck‐Like MoSe2/C Core/Shell Nanostructures for High‐Performance Potassium‐Ion Storage

Potassium‐ion batteries (KIBs) have recently attracted intensive attention because of the abundant potassium resources and their low cost and high safety. However, the major challenge faced by KIBs lies in the lack of stable and high‐capacity materials for the intercalation/deintercalation of large‐size potassium ions. A unique pistachio‐shuck‐like MoSe₂/C core/shell nanostructure (PMC) is synthesized herein as an advanced anode for boosting the performance of KIBs. This PMC is featured with a few layers of molybdenum selenide as the core with an expanded interlayer spacing of ≈0.85 nm, facilitating the intercalation/deintercalation of K ions, and a thin amorphous carbon as the shell, which can confine the active molybdenum selenide nanosheets during cycling for maintaining the high structural stability. Most importantly, as a whole, the PMC has the advantages of reducing the surplus hollow interior space for improving its packing density and buffering the volume expansion during the K‐ion intercalation for further enhancing the stability. As a consequence, the PMC shows a very high capacity of 322 mAh g^?1 at 0.2 A g^?1 over 100 cycles, and can still remain 226 mAh g^?1 at 1.0 A g^?1 for a long period of 1000 cycles, which is among the best‐reported KIBs anodes.     

Preparation of MoS2‐Coated Three‐Dimensional Graphene Networks for High‐Performance Anode Material in Lithium‐Ion Batteries

A novel composite, MoS₂‐coated three‐dimensional graphene network (3DGN), referred to as MoS₂/3DGN, is synthesized by a facile CVD method. The 3DGN, composed of interconnected graphene sheets, not only serves as template for the deposition of MoS₂, but also provides good electrical contact between the current collector and deposited MoS₂. As a proof of concept, the MoS₂/3DGN composite, used as an anode material for lithium‐ion batteries, shows excellent electrochemical performance, which exhibits reversible capacities of 877 and 665 mAh g^?1 during the 50^th cycle at current densities of 100 and 500 mA g^?1, respectively, indicating its good cycling performance. Furthermore, the MoS₂/3DGN composite also shows excellent high‐current‐density performance, e.g., depicts a 10^th‐cycle capacity of 466 mAh g^?1 at a high current density of 4 A g^?1.     

Ultrafast Sodium Full Batteries Derived from X?Fe (X = Co,Ni, Mn) Prussian Blue Analogs

Exploring high‐rate electrode materials with excellent kinetic properties is imperative for advanced sodium‐storage systems. Herein, novel cubic‐like X? Fe (X = Co, Ni, Mn) Prussian blue analogs (PBAs), as cathodes materials, are obtained through as‐tuned ionic bonding, delivering improved crystallinity and homogeneous particles size. As expected, Ni‐Fe PBAs show a capacity of 81 mAh g^?1 at 1.0 A g^?1, mainly resulting from their physical–chemical stability, fast kinetics, and “zero‐strain” insertion characteristics. Considering that the combination of elements incorporated with carbon may increase the rate of ion transfer and improve the lifetime of cycling stability, they are expected to derive binary metal‐selenide/nitrogen‐doped carbon as anodes. Among them, binary Ni_0.67Fe_0.33Se₂ coming from Ni‐Fe PBAs shows obvious core–shell structure in a dual‐carbon matrix, leading to enhanced electron interactions, electrochemical activity, and “metal‐like” conductivity, which could retain an ultralong‐term stability of 375 mAh g^?1 after 10 000 loops even at 10.0 A g^?1. The corresponding full‐cell Ni‐Fe PBAs versus Ni_0.67Fe_0.33Se₂ deliver a remarkable Na‐storage capacity of 302.2 mAh g^?1 at 1.0 A g^?1. The rational strategy is anticipated to offer more possibilities for designing advanced electrode materials used in high‐performance sodium‐ion batteries.     

Interfacial Engineering Coupled Valence Tuning of MoO3 Cathode for High‐Capacity and High‐Rate Fiber‐Shaped Zinc‐Ion Batteries

Aqueous Zn‐ion batteries (ZIBs) have garnered the researchers' spotlight owing to its high safety, cost effectiveness, and high theoretical capacity of Zn anode. However, the availability of cathode materials for Zn ions storage is limited. With unique layered structure along the [010] direction, α‐MoO₃ holds great promise as a cathode material for ZIBs, but its intrinsically poor conductivity severely restricts the capacity and rate capability. To circumvent this issue, an efficient surface engineering strategy is proposed to significantly improve the electric conductivity, Zn ion diffusion rate, and cycling stability of the MoO₃ cathode for ZIBs, thus drastically promoting its electrochemical properties. With the synergetic effect of Al₂O₃ coating and phosphating process, the constructed Zn//P‐MoO_3?x@Al₂O₃ battery delivers impressive capacity of 257.7 mAh g^?1 at 1 A g^?1 and superior rate capability (57% capacity retention at 20 A g^?1), dramatically surpassing the pristine Zn//MoO₃ battery (115.8 mAh g^?1; 19.7%). More importantly, capitalized on polyvinyl alcohol gel electrolyte, an admirable capacity (19.2 mAh cm^?3) as well as favorable energy density (14.4 mWh cm^?3; 240 Wh kg^?1) are both achieved by the fiber‐shaped quasi‐solid‐state ZIB. This work may be a great motivation for further research on molybdenum or other layered structure materials for high‐performance ZIBs.     

Sulfur‐Grafted Hollow Carbon Spheres for Potassium‐Ion Battery Anodes

Sulfur‐rich carbons are minimally explored for potassium‐ion batteries (KIBs). Here, a large amount of S (38 wt%) is chemically incorporated into a carbon host, creating sulfur‐grafted hollow carbon spheres (SHCS) for KIB anodes. The SHCS architecture provides a combination of nanoscale (≈40 nm) diffusion distances and C? S chemical bonding to minimize cycling capacity decay and Coulombic efficiency (CE) loss. The SHCS exhibit a reversible capacity of 581 mAh g^?1 (at 0.025 A g^?1), which is the highest reversible capacity reported for any carbon‐based KIB anode. Electrochemical analysis of S‐free carbon spheres baseline demonstrates that both the carbon matrix and the sulfur species are highly electrochemically active. SHCS also show excellent rate capability, achieving 202, 160, and 110 mAh g^?1 at 1.5, 3, and 5 A g^?1, respectively. The electrode maintains 93% of the capacity from the 5th to 1000th cycle at 3 A g^?1, with steady‐state CE being near 100%. Raman analysis indicates reversible breakage of C? S and S? S bonds upon potassiation to 0.01 V versus K/K⁺. The galvanostatic intermittent titration technique (GITT) analysis provides voltage‐dependent K⁺ diffusion coefficients that range from 10^?10 to 10^?12 cm² s^?1 upon potassiation and depotassiation, with approximately five times higher coefficient for the former.     

A High‐Capacity O2‐Type Li‐Rich Cathode Material with a Single‐Layer Li2MnO3 Superstructure

A high capacity cathode is the key to the realization of high‐energy‐density lithium‐ion batteries. The anionic oxygen redox induced by activation of the Li₂MnO₃ domain has previously afforded an O3‐type layered Li‐rich material used as the cathode for lithium‐ion batteries with a notably high capacity of 250–300 mAh g^?1. However, its practical application in lithium‐ion batteries has been limited due to electrodes made from this material suffering severe voltage fading and capacity decay during cycling. Here, it is shown that an O2‐type Li‐rich material with a single‐layer Li₂MnO₃ superstructure can deliver an extraordinary reversible capacity of 400 mAh g^?1 (energy density: ≈1360 Wh kg^?1). The activation of a single‐layer Li₂MnO₃ enables stable anionic oxygen redox reactions and leads to a highly reversible charge–discharge cycle. Understanding the high performance will further the development of high‐capacity cathode materials that utilize anionic oxygen redox processes.     

Polyethylenimine Expanded Graphite Oxide Enables High Sulfur Loading and Long‐Term Stability of Lithium–Sulfur Batteries

To realize practical lithium–sulfur batteries (LSBs) with long cycling life, designing cathode hosts with a high specific surface area (SSA) is recognized as an efficient way to trap the soluble polysulfides. However, it is also blamed for diminishing the volumetric energy density and being susceptible to side reactions. Herein, polyethylenimine intercalated graphite oxide (PEI‐GO) with a low SSA of 4.6 m² g^?1 and enlarged interlayer spacing of 13 Å is proposed as a superior sulfur host, which enables homogeneous distribution of high sulfur content (73%) and facilitates Li⁺ transfer in thick sulfur electrode. LSBs with a moderate sulfur loading (3.4 mg S cm^?2) achieve an initial capacity of 1157 and 668 mAh g^?1 after 500 cycles at 0.5 C. Even when the sulfur loading is increased to 7.3 mg cm^?2, the electrode still delivers a high areal capacity of 4.7 mAh cm^?2 (641 mAh g^?1) after 200 cycles at 0.2 C. The excellent electrochemical properties of PEI‐GO are mainly attributed to the homogeneous distribution of sulfur in PEI‐GO and the strong chemical interactions between polysulfides and amine groups, which can mitigate the loss of active phases and contribute to the better cycling stability.