Hierarchical Porous Nanosheets Constructed by Graphene‐Coated,Interconnected TiO2 Nanoparticles for Ultrafast Sodium Storage

Sodium‐ion batteries (SIBs) are considered promising next‐generation energy storage devices. However, a lack of appropriate high‐performance anode materials has prevented further improvements. Here, a hierarchical porous hybrid nanosheet composed of interconnected uniform TiO₂ nanoparticles and nitrogen‐doped graphene layer networks (TiO₂@NFG HPHNSs) that are synthesized using dual‐functional C₃N₄ nanosheets as both the self‐sacrificing template and hybrid carbon source is reported. These HPHNSs deliver high reversible capacities of 146 mA h g^?1 at 5 C for 8000 cycles, 129 mA h g^?1 at 10 C for 20 000 cycles, and 116 mA h g^?1 at 20 C for 10 000 cycles, as well as an ultrahigh rate capability up to 60 C with a capacity of 101 mA h g^?1. These results demonstrate the longest cyclabilities and best rate capability ever reported for TiO₂‐based anode materials for SIBs. The unprecedented sodium storage performance of the TiO₂@NFG HPHNSs is due to their unique composition and hierarchical porous 2D structure.     

Mesoporous NiS2 Nanospheres Anode with Pseudocapacitance for High‐Rate and Long‐Life Sodium‐Ion Battery

It is of great importance to exploit electrode materials for sodium‐ion batteries (SIBs) with low cost, long life, and high‐rate capability. However, achieving quick charge and high power density is still a major challenge for most SIBs electrodes because of the sluggish sodiation kinetics. Herein, uniform and mesoporous NiS₂ nanospheres are synthesized via a facile one‐step polyvinylpyrrolidone assisted method. By controlling the voltage window, the mesoporous NiS₂ nanospheres present excellent electrochemical performance in SIBs. It delivers a high reversible specific capacity of 692 mA h g^?1. The NiS₂ anode also exhibits excellent high‐rate capability (253 mA h g^?1 at 5 A g^?1) and long‐term cycling performance (319 mA h g^?1 capacity remained even after 1000 cycles at 0.5 A g^?1). A dominant pseudocapacitance contribution is identified and verified by kinetics analysis. In addition, the amorphization and conversion reactions during the electrochemical process of the mesoporous NiS₂ nanospheres is also investigated by in situ X‐ray diffraction. The impressive electrochemical performance reveals that the NiS₂ offers great potential toward the development of next generation large scale energy storage.     

Nontopotactic Reaction in Highly Reversible Sodium Storage of Ultrathin Co9Se8/rGO Hybrid Nanosheets

Transition metal chalcogenide with tailored nanosheet architectures with reduced graphene oxide (rGO) for high performance electrochemical sodium ion batteries (SIBs) are presented. Via one‐step oriented attachment growth, a facile synthesis of Co₉Se₈ nanosheets anchored on rGO matrix nanocomposites is demonstrated. As effective anode materials of SIBs, Co₉Se₈/rGO nanocomposites can deliver a highly reversible capacity of 406 mA h g^?1 at a current density of 50 mA g^?1 with long cycle stability. It can also deliver a high specific capacity of 295 mA h g^?1 at a high current density of 5 A g^?1 indicating its high rate capability. Furthermore, ex situ transmission electron microscopy observations provide insight into the reaction path of nontopotactic conversion in the hybrid anode, revealing the highly reversible conversion directly between the hybrid Co₉Se₈/rGO and Co nanoparticles/Na₂Se matrix during the sodiation/desodiation process. In addition, it is experimentally demonstrated that rGO plays significant roles in both controllable growth and electrochemical conversion processes, which can not only modulate the morphology of the product but also tune the sodium storage performance. The investigation on hybrid Co₉Se₈/rGO nanosheets as SIBs anode may shed light on designing new metal chalcogenide materials for high energy storage system.     

Porous Carbon Nanofibers Encapsulated with Peapod‐Like Hematite Nanoparticles for High‐Rate and Long‐Life Battery Anodes

Fe₂O₃ is regarded as a promising anode material for lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs) due to its high specific capacity. The large volume change during discharge and charge processes, however, induces significant cracking of the Fe₂O₃ anodes, leading to rapid fading of the capacity. Herein, a novel peapod‐like nanostructured material, consisting of Fe₂O₃ nanoparticles homogeneously encapsulated in the hollow interior of N‐doped porous carbon nanofibers, as a high‐performance anode material is reported. The distinctive structure not only provides enough voids to accommodate the volume expansion of the pea‐like Fe₂O₃ nanoparticles but also offers a continuous conducting framework for electron transport and accessible nanoporous channels for fast diffusion and transport of Li/Na‐ions. As a consequence, this peapod‐like structure exhibits a stable discharge capacity of 1434 mAh g^?1 (at 100 mA g^?1) and 806 mAh g^?1 (at 200 mA g^?1) over 100 cycles as anode materials for LIBs and SIBs, respectively. More importantly, a stable capacity of 958 mAh g^?1 after 1000 cycles and 396 mAh g^?1 after 1500 cycles can be achieved for LIBs and SIBs, respectively, at a large current density of 2000 mA g^?1. This study provides a promising strategy for developing long‐cycle‐life LIBs and SIBs.     

In Situ Carbon‐Doped Mo(Se0.85S0.15)2 Hierarchical Nanotubes as Stable Anodes for High‐Performance Sodium‐Ion Batteries

Sodium‐ion batteries (SIBs) are promising energy storage devices, but suffer from poor cycling stability and low rate capability. In this work, carbon doped Mo(Se_0.85S_0.15)₂ (i.e., Mo(Se_0.85S_0.15)₂:C) hierarchical nanotubes have been synthesized for the first time and serve as a robust and high‐performance anode material. The hierarchical nanotubes with diameters of 300 nm and wall thicknesses of 50 nm consist of numerous 2D layered nanosheets, and can act as a robust host for sodiation/desodiation cycling. The Mo(Se_0.85S_0.15)₂:C hierarchical nanotubes deliver a discharge capacity of 360 mAh g⁻¹ at a high current density of 2000 mA g⁻¹ and keep a 81.8% capacity retention compared to that at a current density of 50 mA g⁻¹, showing superior rate capability. Comparing with the second cycle discharge capacities, the nanotube anode can maintain capacities of 102.2%, 101.9%, and 97.8% after 100 cycles at current densities of 200, 500, and 1000 mA g⁻¹, respectively. This work demonstrates the best cycling performance and high‐rate sodium storage capabilities of MoSe₂ for SIBs to date. The hollow interior, hierarchical organization, layered structure, and carbon doping are beneficial for fast Na⁺‐ion and electron kinetics and are responsible for the stable cycling performance and high rate capabilities.     

Controllable N‐Doped CuCo2O4@C Film as a Self‐Supported Anode for Ultrastable Sodium‐Ion Batteries

Rational synthesis of flexible electrodes is crucial to rapid growth of functional materials for energy‐storage systems. Herein, a controllable fabrication is reported for the self‐supported structure of CuCo₂O₄ nanodots (≈3 nm) delicately inserted into N‐doped carbon nanofibers (named as 3‐CCO@C); this composite is first used as binder‐free anode for sodium‐ion batteries (SIBs). Benefiting from the synergetic effect of ultrasmall CuCo₂O₄ nanoparticles and a tailored N‐doped carbon matrix, the 3‐CCO@C composite exhibits high cycling stability (capacity of 314 mA h g^?1 at 1000 mA g^?1 after 1000 cycles) and high rate capability (296 mA h g^?1, even at 5000 mA g^?1). Significantly, the Na storage mechanism is systematically explored, demonstrating that the irreversible reaction of CuCo₂O₄, which decomposes to Cu and Co, happens in the first discharge process, and then a reversible reaction between metallic Cu/Co and CuO/Co₃O₄ occurrs during the following cycles. This result is conducive to a mechanistic study of highly promising bimetallic‐oxide anodes for rechargeable SIBs.     

Controllable Design of MoS2 Nanosheets Grown on Nitrogen‐Doped Branched TiO2/C Nanofibers: Toward Enhanced Sodium Storage Performance Induced by Pseudocapacitance Behavior

In this work, expanded MoS₂ nanosheets grown on nitrogen‐doped branched TiO₂/C nanofibers (NBT/C@MoS₂ NFs) are prepared through electrospinning and hydrothermal treatment method as anode materials for sodium‐ion batteries (SIBs). The continuous 1D branched TiO₂/C nanofibers provide a large surface area to grow expanded MoS₂ nanosheets and enhance the electronic conductivity and cycling stability of the electrode. The large surface area and doping of nitrogen can facilitate the transfer of both Na⁺ ions and electrons. With the merits of these unique design and extrinsic pseudocapacitance behavior, the NBT/C@MoS₂ NFs can deliver ultralong cycle stability of 448.2 mA h g^?1 at 200 mA g^?1 after 600 cycles. Even at a high rate of 2000 mA g^?1, a reversible capacity of 258.3 mA h g^?1 can still be achieved. The kinetic analysis demonstrates that pseudocapacitive contribution is the major factor to achieve excellent rate performance. The rational design and excellent electrochemical performance endow the NBT/C@MoS₂ NFs with potentials as promising anode materials for SIBs.     

In Situ Encapsulating α‐MnS into N,S‐Codoped Nanotube‐Like Carbon as Advanced Anode Material: α → β Phase Transition Promoted Cycling Stability and Superior Li/Na‐Storage Performance in Half/Full Cells

Incorporation of N,S‐codoped nanotube‐like carbon (N,S‐NTC) can endow electrode materials with superior electrochemical properties owing to the unique nanoarchitecture and improved kinetics. Herein, α‐MnS nanoparticles (NPs) are in situ encapsulated into N,S‐NTC, preparing an advanced anode material (α‐MnS@N,S‐NTC) for lithium‐ion/sodium‐ion batteries (LIBs/SIBs). It is for the first time revealed that electrochemical α → β phase transition of MnS NPs during the 1st cycle effectively promotes Li‐storage properties, which is deduced by the studies of ex situ X‐ray diffraction/high‐resolution transmission electron microscopy and electrode kinetics. As a result, the optimized α‐MnS@N,S‐NTC electrode delivers a high Li‐storage capacity (1415 mA h g^?1 at 50 mA g^?1), excellent rate capability (430 mA h g^?1 at 10 A g^?1), and long‐term cycling stability (no obvious capacity decay over 5000 cycles at 1 A g^?1) with retained morphology. In addition, the N,S‐NTC‐based encapsulation plays the key roles on enhancing the electrochemical properties due to its high conductivity and unique 1D nanoarchitecture with excellent protective effects to active MnS NPs. Furthermore, α‐MnS@N,S‐NTC also delivers high Na‐storage capacity (536 mA h g^?1 at 50 mA g^?1) without the occurrence of such α → β phase transition and excellent full‐cell performances as coupling with commercial LiFePO₄ and LiNi_0.6Co_0.2Mn_0.2O₂ cathodes in LIBs as well as Na₃V₂(PO₄)₂O₂F cathode in SIBs.     

Hierarchically Porous Fe2CoSe4 Binary‐Metal Selenide for Extraordinary Rate Performance and Durable Anode of Sodium‐Ion Batteries

Owing to high energy capacities, transition metal chalcogenides have drawn significant research attention as the promising electrode materials for sodium‐ion batteries (SIBs). However, limited cycle life and inferior rate capabilities still hinder their practical application. Improvement of the intrinsic conductivity by smart choice of elemental combination along with carbon coupling of the nanostructures may result in excellence of rate capability and prolonged cycling stability. Herein, a hierarchically porous binary transition metal selenide (Fe₂CoSe₄, termed as FCSe) nanomaterial with improved intrinsic conductivity was prepared through an exclusive methodology. The hierarchically porous structure, intimate nanoparticle–carbon matrix contact, and better intrinsic conductivity result in extraordinary electrochemical performance through their synergistic effect. The synthesized FCSe exhibits excellent rate capability (816.3 mA h g^?1 at 0.5 A g^?1 and 400.2 mA h g^?1 at 32 A g^?1), extended cycle life (350 mA h g^?1 even after 5000 cycles at 4 A g^?1), and adequately high energy capacity (614.5 mA h g^?1 at 1 A g^?1 after 100 cycles) as anode material for SIBs. When further combined with lab‐made Na₃V₂(PO₄)₃/C cathode in Na‐ion full cells, FCSe presents reasonably high and stable specific capacity.     

S‐Doped Carbon Fibers Uniformly Embedded with Ultrasmall TiO2 for Na+/Li+ Storage with High Capacity and Long‐Time Stability

Building a rechargeable battery with high capacity, high energy density, and long lifetime contributes to the development of novel energy storage devices in the future. Although carbon materials are very attractive anode materials for lithium‐ion batteries (LIBs), they present several deficiencies when used in sodium‐ion batteries (SIBs). The choice of an appropriate structural design and heteroatom doping are critical steps to improve the capacity and stability. Here, carbon‐based nanofibers are produced by sulfur doping and via the introduction of ultrasmall TiO₂ nanoparticles into the carbon fibers (CNF‐S@TiO₂). It is discovered that the introduction of TiO₂ into carbon nanofibers can significantly improve the specific surface area and microporous volume for carbon materials. The TiO₂ content is controlled to obtain CNF‐S@TiO₂‐5 to use as the anode material for SIBs/LIBs with enhanced electrochemical performance in Na⁺/Li⁺ storage. During the charge/discharge process, the S‐doping and the incorporation of TiO₂ nanoparticles into carbon fibers promote the insertion/extraction of the ions and enhance the capacity and cycle life. The capacity of CNF‐S@TiO₂‐5 can be maintained at ≈300 mAh g^?1 over 600 cycles at 2 A g^?1 in SIBs. Moreover, the capacity retention of such devices is 94%, showing high capacity and good stability.     

Synergizing Phase and Cavity in CoMoOxSy Yolk–Shell Anodes to Co‐Enhance Capacity and Rate Capability in Sodium Storage

Sodium‐ion batteries (SIBs) have been recognized as the promising alternatives to lithium‐ion batteries for large‐scale applications owing to their abundant sodium resource. Currently, one significant challenge for SIBs is to explore feasible anodes with high specific capacity and reversible pulverization‐free Na⁺ insertion/extraction. Herein, a facile co‐engineering on polymorph phases and cavity structures is developed based on CoMo‐glycerate by scalable solvothermal sulfidation. The optimized strategy enables the construction of CoMoO_xS_y with synergized partially sulfidized amorphous phase and yolk–shell confined cavity. When developed as anodes for SIBs, such CoMoO_xS_y electrodes deliver a high reversible capacity of 479.4 mA h g^?1 at 200 mA g^?1 after 100 cycles and a high rate capacity of 435.2 mA h g^?1 even at 2000 mA g^?1, demonstrating superior capacity and rate capability. These are attributed to the unique dual merits of the anodes, that is, the elastic bountiful reaction pathways favored by the sulfidation‐induced amorphous phase and the sodiation/desodiation accommodatable space benefits from the yolk–shell cavity. Such yolk–shell nano‐battery materials are merited with co‐tunable phases and structures, facile scalable fabrication, and excellent capacity and rate capability in sodium storage. This provides an opportunity to develop advanced practical electrochemical sodium storage in the future.     

Synthesis of MoS2@C Nanotubes Via the Kirkendall Effect with Enhanced Electrochemical Performance for Lithium Ion and Sodium Ion Batteries

A MoS₂@C nanotube composite is prepared through a facile hydrothermal method, in which the MoS₂ nanotube and amorphous carbon are generated synchronically. When evaluated as an anode material for lithium ion batteries (LIB), the MoS₂@C nanotube manifests an enhanced capacity of 1327 mA h g^?1 at 0.1 C with high initial Coulombic efficiency (ICE) of 92% and with capacity retention of 1058.4 mA h g^?1 (90% initial capacity retention) after 300 cycles at a rate of 0.5 C. A superior rate capacity of 850 mA h g^?1 at 5 C is also obtained. As for sodium ion batteries, a specific capacity of 480 mA h g^?1 at 0.5 C is achieved after 200 cycles. The synchronically formed carbon and stable hollow structure lead to the long cycle stability, high ICE, and superior rate capability. The good electrochemical behavior of MoS₂@C nanotube composite suggests its potential application in high‐energy LIB.     

Ion Reservoir Enabled by Hierarchical Bimetallic Sulfides Nanocages Toward Highly Effective Sodium Storage

Designing and constructing bimetallic hierarchical structures is vital for the conversion‐alloy reaction anode of sodium‐ion batteries (SIBs). Particularly, the rationally designed hetero‐interface engineering can offer fast diffusion kinetics in the interface, leading to the improved high‐power surface pseudocapacitance and cycling stability for SIBs. Herein, the hierarchical zinc–tin sulfide nanocages (ZnS‐NC/SnS₂) are constructed through hydrothermal and sulfuration reactions. The unconventional hierarchical design with internal void space greatly optimizes the structure stability, and bimetallic sulfide brings a bimetallic composite interface and N heteroatom doping, which are devoted to high electrochemical activity and improved interfacial charge transfer rate for Na⁺ storage. Remarkably, the ZnS‐NC/SnS₂ composite anode exhibits a delightful reversible capacity of 595 mAh g^?1 after 100 cycles at 0.2 A g^?1, and long cycling capability for 500 cycles with a low capacity loss of 0.08% per cycle at 1 A g^?1. This study opens up a new route for rationally constructing hierarchical heterogeneous interfaces and sheds new light on efficient anode material for SIBs.     

FeP@C Nanotube Arrays Grown on Carbon Fabric as a Low Potential and Freestanding Anode for High‐Performance Li‐Ion Batteries

An anode of self‐supported FeP@C nanotube arrays on carbon fabric (CF) is successfully fabricated via a facile template‐based deposition and phosphorization route: first, well‐aligned FeOOH nanotube arrays are simply obtained via a solution deposition and in situ etching route with hydrothermally crystallized (Co,Ni)(CO₃)_0.5OH nanowire arrays as the template; subsequently, these uniform FeOOH nanotube arrays are transformed into robust carbon‐coated Fe₃O₄ (Fe₃O₄@C) nanotube arrays via glucose adsorption and annealing treatments; and finally FeP@C nanotube arrays on CF are achieved through the facile phosphorization of the oxide‐based arrays. As an anode for lithium‐ion batteries (LIBs), these FeP@C nanotube arrays exhibit superior rate capability (reversible capacities of 945, 871, 815, 762, 717, and 657 mA h g⁻¹ at 0.1, 0.2, 0.4, 0.8, 1.3, and 2.2 A g⁻¹, respectively, corresponding to area specific capacities of 1.73, 1.59, 1.49, 1.39, 1.31, 1.20 mA h cm⁻² at 0.18, 0.37, 0.732, 1.46, 2.38, and 4.03 mA cm⁻², respectively) and a stable long‐cycling performance (a high specific capacity of 718 mA h g⁻¹ after 670 cycles at 0.5 A g⁻¹, corresponding to an area capacity of 1.31 mA h cm⁻² at 0.92 mA cm⁻²).     

Bismuth Nanoparticle@Carbon Composite Anodes for Ultralong Cycle Life and High‐Rate Sodium‐Ion Batteries

Bismuth has emerged as a promising anode material for sodium‐ion batteries (SIBs), owing to its high capacity and suitable operating potential. However, large volume changes during alloying/dealloying processes lead to poor cycling performance. Herein, bismuth nanoparticle@carbon (Bi@C) composite is prepared via a facile annealing method using a commercial coordination compound precursor of bismuth citrate. The composite has a uniform structure with Bi nanoparticles embedded within a carbon framework. The nanosized structure ensures a fast kinetics and efficient alleviation of stress/strain caused by the volume change, and the resilient and conductive carbon matrix provides an interconnected electron transportation pathway. The Bi@C composite delivers outstanding sodium‐storage performance with an ultralong cycle life of 30 000 cycles at a high current density of 8 A g^?1 and an excellent rate capability of 71% capacity retention at an ultrahigh current rate of 60 A g^?1. Even at a high mass loading of 11.5 mg cm^?2, a stable reversible capacity of 280 mA h g^?1 can be obtained after 200 cycles. More importantly, full SIBs by pairing with a Na₃V₂(PO₄)₃ cathode demonstrates superior performance. Combining the facile synthesis and the commercial precursor, the exceptional performance makes the Bi@C composite very promising for practical large‐scale applications.     

N‐Doped Carbon Nanofibers with Interweaved Nanochannels for High‐Performance Sodium‐Ion Storage

Although graphite materials have been applied as commercial anodes in lithium‐ion batteries (LIBs), there still remain abundant spaces in the development of carbon‐based anode materials for sodium‐ion batteries (SIBs). Herein, an electrospinning route is reported to fabricate nitrogen‐doped carbon nanofibers with interweaved nanochannels (NCNFs‐IWNC) that contain robust interconnected 1D porous channels, produced by removal of a Te nanowire template that is coelectrospun within carbon nanofibers during the electrospinning process. The NCNFs‐IWNC features favorable properties, including a conductive 1D interconnected porous structure, a large specific surface area, expanded interlayer graphite‐like spacing, enriched N‐doped defects and active sites, toward rapid access and transport of electrolyte and electron/sodium ions. Systematic electrochemical studies indicate that the NCNFs‐IWNC exhibits an impressively high rate capability, delivering a capacity of 148 mA h g^?1 at current density of as high as 10 A g^?1, and has an attractively stable performance over 5000 cycles. The practical application of the as‐designed NCNFs‐IWNC for a full SIBs cell is further verified by coupling the NCNFs‐IWNC anode with a FeFe(CN)₆ cathode, which displays a desirable cycle performance, maintaining acapacity of 97 mA h g^?1 over 100 cycles.     

Unique Cobalt Sulfide/Reduced Graphene Oxide Composite as an Anode for Sodium‐Ion Batteries with Superior Rate Capability and Long Cycling Stability

Exploitation of high‐performance anode materials is essential but challenging to the development of sodium‐ion batteries (SIBs). Among all proposed anode materials for SIBs, sulfides have been proved promising candidates due to their unique chemical and physical properties. In this work, a facile solvothermal method to in situ decorate cobalt sulfide (CoS) nanoplates on reduced graphene oxide (rGO) to build CoS@rGO composite is described. When evaluated as anode for SIBs, an impressive high specific capacity (540 mAh g^?1 at 1 A g^?1), excellent rate capability (636 mAh g^?1 at 0.1 A g^?1 and 306 mAh g^?1 at 10 A g^?1), and extraordinarily cycle stability (420 mAh g^?1 at 1 A g^?1 after 1000 cycles) have been demonstrated by CoS@rGO composite for sodium storage. The synergetic effect between the CoS nanoplates and rGO matrix contributes to the enhanced electrochemical performance of the hybrid composite. The results provide a facile approach to fabricate promising anode materials for high‐performance SIBs.     

Designed Formation of Hybrid Nanobox Composed of Carbon Sheathed CoSe2 Anchored on Nitrogen‐Doped Carbon Skeleton as Ultrastable Anode for Sodium‐Ion Batteries

Research on sodium‐ion batteries (SIBs) has recently been revitalized due to the unique features of much lower costs and comparable energy/power density to lithium‐ion batteries (LIBs), which holds great potential for grid‐level energy storage systems. Transition metal dichalcogenides (TMDCs) are considered as promising anode candidates for SIBs with high theoretical capacity, while their intrinsic low electrical conductivity and large volume expansion upon Na⁺ intercalation raise the challenging issues of poor cycle stability and inferior rate performance. Herein, the designed formation of hybrid nanoboxes composed of carbon‐protected CoSe₂ nanoparticles anchored on nitrogen‐doped carbon hollow skeletons (denoted as CoSe₂@C∩NC) via a template‐assisted refluxing process followed by conventional selenization treatment is reported, which exhibits tremendously enhanced electrochemical performance when applied as the anode for SIBs. Specifically, it can deliver a high reversible specific capacity of 324 mAh g^?1 at current density of 0.1 A g^?1 after 200 cycles and exhibit outstanding high rate cycling stability at the rate of 5 A g^?1 over 2000 cycles. This work provides a rational strategy for the design of advanced hybrid nanostructures as anode candidates for SIBs, which could push forward the development of high energy and low cost energy storage devices.     

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⁺.     

High‐Performance Flexible Freestanding Anode with Hierarchical 3D Carbon‐Networks/Fe7S8/Graphene for Applicable Sodium‐Ion Batteries

Sodium‐ion batteries (SIBs) have gained tremendous interest for grid scale energy storage system and power energy batteries. However, the current researches of anode for SIBs still face the critical issues of low areal capacity, limited cycle life, and low initial coulombic efficiency for practical application perspective. To solve this issue, a kind of hierarchical 3D carbon‐networks/Fe₇S₈/graphene (CFG) is designed and synthesized as freestanding anode, which is constructed with Fe₇S₈ microparticles well‐welded on 3D‐crosslinked carbon‐networks and embedded in highly conductive graphene film, via a facile and scalable synthetic method. The as‐prepared freestanding electrode CFG represents high areal capacity (2.12 mAh cm^?2 at 0.25 mA cm^?2) and excellent cycle stability of 5000 cycles (0.0095% capacity decay per cycle). The assembled all‐flexible sodium‐ion battery delivers remarkable performance (high areal capacity of 1.42 mAh cm^?2 at 0.3 mA cm^?2 and superior energy density of 144 Wh kg^?1), which are very close to the requirement of practical application. This work not only enlightens the material design and electrode engineering, but also provides a new kind of freestanding high energy density anode with great potential application prospective for SIBs.