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.     

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.     

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.     

Flexible and Binder‐Free Electrodes of Sb/rGO and Na3V2(PO4)3/rGO Nanocomposites for Sodium‐Ion Batteries

Flexible power sources have shown great promise in next‐generation bendable, implantable, and wearable electronic systems. Here, flexible and binder‐free electrodes of Na₃V₂(PO₄)₃/reduced graphene oxide (NVP/rGO) and Sb/rGO nanocomposites for sodium‐ion batteries are reported. The Sb/rGO and NVP/rGO paper electrodes with high flexibility and tailorability can be easily fabricated. Sb and NVP nanoparticles are embedded homogenously in the interconnected framework of rGO nanosheets, which provides structurally stable hosts for Na‐ion intercalation and deintercalation. The NVP/rGO paper‐like cathode delivers a reversible capacity of 113 mAh g^?1 at 100 mA g^?1 and high capacity retention of ≈96.6% after 120 cycles. The Sb/rGO paper‐like anode gives a highly reversible capacity of 612 mAh g^?1 at 100 mA g^?1, an excellent rate capacity up to 30 C, and a good cycle performance. Moreover, the sodium‐ion full cell of NVP/rGO//Sb/rGO has been fabricated, delivering a highly reversible capacity of ≈400 mAh g^?1 at a current density of 100 mA g^?1 after 100 charge/discharge cycles. This work may provide promising electrode candidates for developing next‐generation energy‐storage devices with high capacity and long cycle life.     

T‐Nb2O5/C Nanofibers Prepared through Electrospinning with Prolonged Cycle Durability for High‐Rate Sodium–Ion Batteries Induced by Pseudocapacitance

Homogeneous ultrasmall T‐Nb₂O₅ nanocrystallites encapsulated in 1D carbon nanofibers (T‐Nb₂O₅/CNFs) are prepared through electrospinning followed by subsequent pyrolysis treatment. In a Na half‐cell configuration, the obtained T‐Nb₂O₅/CNFs with the merits of unique microstructures and inherent pseudocapacitance, deliver a stable capacity of 150 mAh g⁻¹ at 1 A g⁻¹ over 5000 cycles. Even at an ultrahigh charge–discharge rate of 8 A g⁻¹, a high reversible capacity of 97 mAh g⁻¹ is still achieved. By means of kinetic analysis, it is demonstrated that the larger ratio of surface Faradaic reactions of Nb₂O₅ at high rates is the major factor to achieve excellent rate performance. The prolonged cycle durability and excellent rate performance endows T‐Nb₂O₅/CNFs with potentials as anode materials for sodium‐ion batteries.     

Graphitic Carbon Nitride (g‐C3N4)‐Derived N‐Rich Graphene with Tuneable Interlayer Distance as a High‐Rate Anode for Sodium‐Ion Batteries

Heteroatom‐doped carbon materials with expanded interlayer distance have been widely studied as anodes for sodium‐ion batteries (SIBs). However, it remains unexplored to further enlarge the interlayer spacing and reveal the influence of heteroatom doping on carbon nanostructures for developing more efficient SIB anode materials. Here, a series of N‐rich few‐layer graphene (N‐FLG) with tuneable interlayer distance ranging from 0.45 to 0.51 nm is successfully synthesized by annealing graphitic carbon nitride (g‐C₃N₄) under zinc catalysis and selected temperature (T = 700, 800, and 900 °C). More significantly, the correlation between N dopants and interlayer distance of resultant N‐FLG‐T highlights the effect of pyrrolic N on the enlargement of graphene interlayer spacing, due to its stronger electrostatic repulsion. As a consequence, N‐FLG‐800 achieves the optimal properties in terms of interlayer spacing, nitrogen configuration and electronic conductivity. When used as an anode for SIBs, N‐FLG‐800 shows remarkable Na⁺ storage performance with ultrahigh rate capability (56.6 mAh g^?1 at 40 A g^?1) and excellent long‐term stability (211.3 mAh g^?1 at 0.5 A g^?1 after 2000 cycles), demonstrating the effectiveness of material design.     

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.     

Reactive Oxygen‐Doped 3D Interdigital Carbonaceous Materials for Li and Na Ion Batteries

Carbonaceous materials as anodes usually exhibit low capacity for lithium ion batteries (LIBs) and sodium ion batteries (SIBs). Oxygen‐doped carbonaceous materials have the potential of high capacity and super rate performance. However, up to now, the reported oxygen‐doped carbonaceous materials usually exhibit inferior electrochemical performance. To overcome this problem, a high reactive oxygen‐doped 3D interdigital porous carbonaceous material is designed and synthesized through epitaxial growth method and used as anodes for LIBs and SIBs. It delivers high reversible capacity, super rate performance, and long cycling stability (473 mA h g^?1after 500 cycles for LIBs and 223 mA h g^?1 after 1200 cycles for SIBs, respectively, at the current density of 1000 mA g^?1), with a capacity decay of 0.0214% per cycle for LIBs and 0.0155% per cycle for SIBs. The results demonstrate that constructing 3D interdigital porous structure with reactive oxygen functional groups can significantly enhance the electrochemical performance of oxygen‐doped carbonaceous material.     

Confinement Growth of Layered WS2 in Hollow Beaded Carbon Nanofibers with Synergistic Anchoring Effect to Reinforce Li+/Na+ Storage Performance

Novel nitrogen doped (N‐doped) hollow beaded structural composite carbon nanofibers are successfully applied for lithium‐ion batteries (LIBs) and sodium‐ion batteries (SIBs). Tungsten disulfide (WS₂) nanosheets are confined, through synergistic anchoring, on the surface and inside of hollow beaded carbon nanofibers (HB CNFs) via a hydrothermal reaction method to construct the hierarchical structure HB WS₂@CNFs. Benefiting from this unique advantage, HB WS₂@CNFs exhibits remarkable lithium‐storage performance in terms of high rate capability (≈351 mAh g^?1 at 2 A g^?1) and stable long‐term cycle (≈446 mAh g^?1 at 1 A g^?1 after 100 cycles). Moreover, as an anode material for SIBs, HB WS₂@CNFs obtains excellent long cycle life and rate performance. During the charging/discharging process, the evolution of morphology and composition of the composite are analyzed by a set of ex situ methods. This synergistic anchoring effect between WS₂ nanosheets and HB CNFs is capable of effectively restraining volume expansion from the metal ions intercalation/deintercalation process and improving the cycling stability and rate performance in LIBs and SIBs.     

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⁺.     

Multidimensional Synergistic Nanoarchitecture Exhibiting Highly Stable and Ultrafast Sodium‐Ion Storage

Conversion‐type anodes with multielectron reactions are beneficial for achieving a high capacity in sodium‐ion batteries. Enhancing the electron/ion conductivity and structural stability are two key challenges in the development of high‐performance sodium storage. Herein, a novel multidimensionally assembled nanoarchitecture is presented, which consists of V₂O₃ nanoparticles embedded in amorphous carbon nanotubes that are then coassembled within a reduced graphene oxide (rGO) network, this materials is denoted V₂O₃?C‐NTs?rGO. The selective insertion and multiphase conversion mechanism of V₂O₃ in sodium‐ion storage is systematically demonstrated for the first time. Importantly, the naturally integrated advantages of each subunit synergistically provide a robust structure and rapid electron/ion transport, as confirmed by in situ and ex situ transmission electron microscopy experiments and kinetic analysis. Benefiting from the synergistic effects, the V₂O₃?C‐NTs?rGO anode delivers an ultralong cycle life (72.3% at 5 A g^?1 after 15 000 cycles) and an ultrahigh rate capability (165 mAh g^?1 at 20 A g^?1, ≈30 s per charge/discharge). The synergistic design of the multidimensionally assembled nanoarchitecture produces superior advantages in energy storage.     

Flexible Membrane Consisting of MoP Ultrafine Nanoparticles Highly Distributed Inside N and P Codoped Carbon Nanofibers as High‐Performance Anode for Potassium‐Ion Batteries

Rechargeable potassium‐ion batteries (PIBs) have attracted tremendous attention as potential electrical energy storage systems due to the special merit of abundant resources and low cost of potassium. However, one critical barrier to achieve practical application of PIBs has been the lack of suitable electrode materials. Here, a novel flexible membrane consisting of N, P codoped carbon nanofibers decorated with MoP ultrafine nanoparticles (MoP@NPCNFs) is fabricated via a simple electrospinning method combined with the later carbonization and phosphorization process. The 3D porous CNF structure in the as‐synthesized composite can shorten the transport pathways of K‐ions and improve the conductivity of electrons. The ultrafine MoP nanoparticles can guarantee high specific capacity and the N, P co‐doping could improve wettability of electrodes to electrolytes. As expected, the free‐standing MoP@NPCNF electrode demonstrates a high capacity of 320 mAh g^?1 at 100 mA g^?1, a superior rate capability maintaining 220 mAh g^?1 at 2 A g^?1, as well as a capacity retention of more than 90% even after 200 cycles. The excellent rate performance, high reversible capacity, long‐term cycling stability, and facile synthesis routine make this hybrid membrane promising anode for potassium‐ion batteries.     

2D Film of Carbon Nanofibers Elastically Astricted MnO Microparticles: A Flexible Binder‐Free Anode for Highly Reversible Lithium Ion Storage

MnO as anode materials has received particular interest owing to its high specific capacity, abundant resources, and low cost. However, serious problems related to the large volume change (>170%) during the lithiation/delithiation processes still results in poor rate capability and fast capacity decay. With homogenous crystals of MnO grown in the network of carbon nanofibers (CNF), binding effect of CNF can effectively weaken the volume change of MnO during cycles. In this work, a CNF/MnO flexible electrode for lithium‐ion batteries is designed and synthesized. The CNF play the roles of conductive channel and elastically astricting MnO particles during lithiation/delithiation. CNF/MnO as binder‐free anode delivers specific capacity of 983.8 mAh g^?1 after 100th cycle at a current density of 0.2 A g^?1, and 600 mAh g^?1 at 1 A g^?1 which are much better than those of pure MnO and pure CNF. The ex‐situ morphologies clearly show the relative volume change of MnO/CNF as anode under various discharging and charging times. CNF can elastically buffer the volume change of MnO during charging/discharging cycles. A facile and scalable approach for synthesizing a novel flexible binder‐free anode of CNF/MnO for potential application in highly reversible lithium storage devices is presented.     

Ultrahigh Rate Performance of Hollow Antimony Nanoparticles Impregnated in Open Carbon Boxes for Sodium‐Ion Battery under Elevated Temperature

Antimony is a competitive and promising anode material for sodium‐ion batteries (SIBs) due to its high theoretical capacity. However, the poor rate capability and fast capacity fading greatly restrict its practical application. To address the above issues, a facile and eco‐friendly sacrificial template method is developed to synthesize hollow Sb nanoparticles impregnated in open carbon boxes (Sb HPs@OCB). The as‐obtained Sb HPs@OCB composite exhibits excellent sodium storage properties even when operated at an elevated temperature of 50 °C, delivering a robust rate capability of 345 mAh g^?1 at 16 A g^?1 and rendering an outstanding reversible capacity of 187 mAh g^?1 at a high rate of 10 A g^?1 after 300 cycles. Such superior electrochemical performance of the Sb HPs@OCB can be attributed to the comprehensive characteristics of improved kinetics derived from hollow Sb nanoparticles impregnated into 2D carbon nanowalls, the existence of robust Sb? O? C bond, and enhanced pseudocapacitive behavior. All those factors enable Sb HPs@OCB great potential and distinct merit for large‐scale energy storage of SIBs.     

Urchin‐Like Fe3Se4 Hierarchitectures: A Novel Pseudocapacitive Sodium‐Ion Storage Anode with Prominent Rate and Cycling Properties

Transition metal chalcogenides have received great attention as promising anode candidates for sodium‐ion batteries (SIBs). However, the undesirable cyclic life and inferior rate capability still restrict their practical applications. The design of micro–nano hierarchitectures is considered as a possible strategy to facilitate the electrochemical reaction kinetics and strengthen the electrode structure stability upon repeated Na⁺ insertion/extraction. Herein, urchin‐like Fe₃Se₄ hierarchitectures are successfully prepared and developed as a novel anode material for SIBs. Impressively, the as‐prepared urchin‐like Fe₃Se₄ can present an ultrahigh rate capacity of 200.2 mAh g^‐1 at 30 A g^‐1 and a prominent capacity retention of 99.9% over 1000 cycles at 1 A g^‐1, meanwhile, a respectable initial coulombic efficiency of ≈100% is achieved. Through the conjunct study of in situ X‐ray diffraction, ex situ X‐ray absorption near‐edge structure spectroscopy, as well as cyclic voltammetry curves, it is intriguing to reveal that the phase transformation from monoclinic to amorphous structure accompanied by the pseudocapacitive Na⁺ storage behavior accounts for the superior electrochemical performance. When paired with the Na₃V₂(PO₄)₃ cathode materials, the assembled full cell enables high energy density and decent cyclic stability, demonstrating potential practical feasibility of the present urchin‐like Fe₃Se₄ anode.     

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.     

Focus on Spinel Li4Ti5O12 as Insertion Type Anode for High‐Performance Na‐Ion Batteries

Sodium‐ion batteries (SIBs) toward large‐scale energy storage applications has fascinated researchers in recent years owing to the low cost, environmental friendliness, and inestimable abundance. The similar chemical and electrochemical properties of sodium and lithium make sodium an easy substitute for lithium in lithium‐ion batteries. However, the main issues of limited cycle life, low energy density, and poor power density hamper the commercialization process. In the last few years, the development of electrode materials for SIBs has been dedicated to improving sodium storage capacities, high energy density, and long cycle life. The insertion type spinel Li₄Ti₅O₁₂ (LTO) possesses “zero‐strain” behavior that offers the best cycle life performance among all reported oxide‐based anodes, displaying a capacity of 155 mAh g^?1 via a three‐phase separation mechanism, and competing for future topmost high energy anode for SIBs. Recent reports offer improvement of overall electrode performance through carbon coating, doping, composites with metal oxides, and surface modification techniques, etc. Further, LTO anode with its structure and properties for SIBs is described and effective methods to improve the LTO performance are discussed in both half‐cell and practical configuration, i.e., full‐cell, along with future perspectives and solutions to promote its use.     

Superior Sodium Storage in 3D Interconnected Nitrogen and Oxygen Dual‐Doped Carbon Network

Carbonaceous materials have attracted immense interest as anode materials for Na‐ion batteries (NIBs) because of their good chemical, thermal stabilities, as well as high Na‐storage capacity. However, the carbonaceous materials as anodes for NIBs still suffer from the lower rate capability and poor cycle life. An N,O‐dual doped carbon (denoted as NOC) network is designed and synthesized, which is greatly favorable for sodium storage. It exhibits high specific capacity and ultralong cycling stability, delivering a capacity of 545 mAh g^?1 at 100 mA g^?1 after 100 cycles and retaining a capacity of 240 mAh g^?1 at 2 A g^?1 after 2000 cycles. The NOC composite with 3D well‐defined porosity and N,O‐dual doped induces active sites, contributing to the enhanced sodium storage. In addition, the NOC is synthesized through a facile solution process, which can be easily extended to the preparation of many other N,O‐dual doped carbonaceous materials for wide applications in catalysis, energy storage, and solar cells.     

Nitrogen‐Enriched Carbon/CNT Composites Based on Schiff‐Base Networks: Ultrahigh N Content and Enhanced Lithium Storage Properties

To improve the electrochemical performance of carbonaceous anodes for lithium ion batteries (LIBs), the incorporation of both well‐defined heteroatom species and the controllable 3D porous networks are urgently required. In this work, a novel N‐enriched carbon/carbon nanotube composite (NEC/CNT) through a chemically induced precursor‐controlled pyrolysis approach is developed. Instead of conventional N‐containing sources or precursors, Schiff‐base network (SNW‐1) enables the desirable combination of a 3D polymer with intrinsic microporosity and ultrahigh N‐content, which can significantly promote the fast transport of both Li⁺ and electron. Significantly, the strong interaction between carbon skeleton and nitrogen atoms enables the retention of ultrahigh N‐content up to 21 wt% in the resultant NEC/CNT, which exhibits a super‐high capacity (1050 mAh g^?1) for 1000 cycles and excellent rate performance (500 mAh g^?1 at a current density of 5 A g^?1) as the anode material for LIBs. The NEC/CNT composite affords a new model system as well as a totally different insight for deeply understanding the relationship between chemical structures and lithium ion storage properties, in which chemistry may play a more important role than previously expected.     

Nitrogen Doped γ‐Graphyne: A Novel Anode for High‐Capacity Rechargeable Alkali‐Ion Batteries

High energy density is the major demand for next‐generation rechargeable batteries, while the intrinsic low alkali metal adsorption of traditional carbon–based electrode remains the main challenge. Here, the mechanochemical route is proposed to prepare nitrogen doped γ‐graphyne (NGY) and its high capacity is demonstrated in lithium (LIBs)/sodium (SIBs) ion batteries. The sample delivers large reversible Li (1037 mAh g^?1) and Na (570.4 mAh g^?1) storage capacities at 100 mA g^?1 and presents excellent rate capabilities (526 mAh g^?1 for LIBs and 180.2 mAh g^?1 for SIBs) at 5 A g^?1. The superior Li/Na storage mechanisms of NGY are revealed by its 2D morphology evolution, quantitative kinetics, and theoretical calculations. The effects on the diffusion barriers (E_b) and adsorption energies (E_ad) of Li/Na atoms in NGY are also studied and imine‐N is demonstrated to be the ideal doping format to enhance the Li/Na storage performance. Besides, the Li/Na adsorption routes in NGY are optimized according to the experimental and the first‐principles calculation results. This work provides a facile way to fabricate high capacity electrodes in LIBs/SIBs, which is also instructive for the design of other heteroatomic doped electrodes.