Multicore–Shell Bi@N‐doped Carbon Nanospheres for High Power Density and Long Cycle Life Sodium‐ and Potassium‐Ion Anodes

Bismuth (Bi) is an attractive material as anodes for both sodium‐ion batteries (NIBs) and potassium‐ion batteries (KIBs), because it has a high theoretical gravimetric capacity (386 mAh g^?1) and high volumetric capacity (3800 mAh L^?1). The main challenges associated with Bi anodes are structural degradation and instability of the solid electrolyte interphase (SEI) resulting from the huge volume change during charge/discharge. Here, a multicore–shell structured Bi@N‐doped carbon (Bi@N‐C) anode is designed that addresses these issues. The nanosized Bi spheres are encapsulated by a conductive porous N‐doped carbon shell that not only prevents the volume expansion during charge/discharge but also constructs a stable SEI during cycling. The Bi@N‐C exhibits unprecedented rate capability and long cycle life for both NIBs (235 mAh g^?1 after 2000 cycles at 10 A g^?1) and KIBs (152 mAh g^?1 at 100 A g^?1). The kinetic analysis reveals the outstanding electrochemical performance can be attributed to significant pseudocapacitance behavior upon cycling.     

Engineering Hierarchical Hollow Nickel Sulfide Spheres for High‐Performance Sodium Storage

Sodium‐ion batteries (SIBs) are considered as promising alternatives to lithium‐ion batteries (LIBs) for energy storage due to the abundance of sodium, especially for grid distribution systems. The practical implementation of SIBs, however, is severely hindered by their low energy density and poor cycling stability due to the poor electrochemical performance of the existing electrodes. Here, to achieve high‐capacity and durable sodium storage with good rate capability, hierarchical hollow NiS spheres with porous shells composed of nanoparticles are designed and synthesized by tuning the reaction parameters. The formation mechanism of this unique structure is systematically investigated, which is clearly revealed to be Ostwald ripening mechanism on the basis of the time‐dependent morphology evolution. The hierarchical hollow structure provides sufficient electrode/electrolyte contact, shortened Na⁺ diffusion pathways, and high strain‐tolerance capability. The hollow NiS spheres deliver high reversible capacity (683.8 mAh g^?1 at 0.1 A g^?1), excellent rate capability (337.4 mAh g^?1 at 5 A g^?1), and good cycling stability (499.9 mAh g^?1 with 73% retention after 50 cycles at 0.1 A g^?1).     

All‐Cellulose‐Based Quasi‐Solid‐State Sodium‐Ion Hybrid Capacitors Enabled by Structural Hierarchy

Na‐ion hybrid capacitors consisting of battery‐type anodes and capacitor‐style cathodes are attracting increasing attention on account of the abundance of sodium‐based resources as well as the potential to bridge the gap between batteries (high energy) and supercapacitors (high power). Herein, hierarchically structured carbon materials inspired by multiscale building units of cellulose from nature are assembled with cellulose‐based gel electrolytes into Na‐ion capacitors. Nonporous hard carbon anodes are obtained through the direct thermal pyrolysis of cellulose nanocrystals. Nitrogen‐doped carbon cathodes with a coral‐like hierarchically porous architecture are prepared via hydrothermal carbonization and activation of cellulose microfibrils. The reversible charge capacity of the anode is 256.9 mAh g^?1 when operating at 0.1 A g^?1 from 0 to 1.5 V versus Na⁺/Na, and the discharge capacitance of cathodes tested within 1.5 to 4.2 V versus Na⁺/Na is 212.4 F g^?1 at 0.1 A g^?1. Utilizing Na⁺ and ClO₄^? as charge carriers, the energy density of the full Na‐ion capacitor with two asymmetric carbon electrodes can reach 181 Wh kg^?1 at 250 W kg^?1, which is one of the highest energy devices reported until now. Combined with macrocellulose‐based gel electrolytes, all‐cellulose‐based quasi‐solid‐state devices are demonstrated possessing additional advantages in terms of overall sustainability.     

Ever‐Increasing Pseudocapacitance in RGO–MnO–RGO Sandwich Nanostructures for Ultrahigh‐Rate Lithium Storage

Lithium ion batteries have attained great success in commercialization owing to their high energy density. However, the relatively delaying discharge/charge severely hinders their high power applications due to intrinsically diffusion‐controlled lithium storage of the electrode. This study demonstrates an ever‐increasing surface redox capacitive lithium storage originating from an unique microstructure evolution during cycling in a novel RGO–MnO–RGO sandwich nanostructure. Such surface pseudocapacitance is dynamically in equilibrium with diffusion‐controlled lithium storage, thereby achieving an unprecedented rate capability (331.9 mAh g^?1 at 40 A g^?1, 379 mAh g^?1 after 4000 cycles at 15 A g^?1) with outstanding cycle stability. The dynamic combination of surface and diffusion lithium storage of electrodes might open up possibilities for designing high‐power lithium ion batteries.     

Temperature‐Mediated Engineering of Graphdiyne Framework Enabling High‐Performance Potassium Storage

Graphdiyne (GDY), an emerging type of carbon allotropes, possesses fascinating electrical, chemical, and mechanical properties to readily spark energy applications in the realm of Li‐ion and Na‐ion batteries. Nevertheless, rational design of GDY architectures targeting advanced K‐ion storage has rarely been reported to date. Herein, the first example of synthesizing GDY frameworks in a scalable fashion to realize superb potassium storage for high‐performance K‐ion battery (KIB) anodes is showcased. To begin with, first principles calculations provide theoretical guidances for analyzing the intrinsic potassium storage capability of GDY. Meanwhile, the specific capacity is predicted to be as high as 620 mAh g^?1, which is considerably augmented as compared with graphite (278 mAh g^?1). Experimental tests then reveal that prepared GDY framework indeed harvests excellent electrochemical performance as a KIB anode, achieving high specific capacity (≈505 mAh g^?1 at 50 mA g^?1), outstanding rate performance (150 mAh g^?1 at 5000 mA g^?1) and favorable cycling stability (a high capacity retention of over 90% after 2000 cycles at 1000 mA g^?1). Furthermore, kinetic analysis reveals that capacitive effect mainly accounts for the K‐ion storage, with operando Raman spectroscopy/ex situ X‐ray photoelectron spectroscopy identifying good electrochemical reversibility of GDY.     

Hierarchical NiS2 Modified with Bifunctional Carbon for Enhanced Potassium‐Ion Storage

Potassium‐ion batteries (PIBs) are currently drawing increased attention as a promising alternative to lithium‐ion batteries (LIBs) owing to the abundant resource and low cost of potassium. However, due to the large ionic radius size of K⁺, electrode material that can stably maintain K⁺ insertion/deintercalation is still extremely inadequate, especially for anode material with a satisfactory reversible capacity. As an attempt, nitrogen/carbon dual‐doped hierarchical NiS₂ is introduced as the electrode material in PIBs for the first time. Considering that the introduction of the carbon layer effectively alleviates the volume expansion of the material itself, further improves the electronic conductivity, and finally accelerates the charge transfer of K⁺, not surprisingly, NiS₂ decorated with the bifunctional carbon (NiS₂@C@C) material electrode shows excellent potassium storage performances. When utilized as a PIB anode, it delivers a high reversible capacity of 302.7 mAh g^?1 at 50 mA g^?1 after 100 cycles. The first coulombic efficiency is 78.6% and rate performance is 151.2 mAh g^?1 at 1.6 A g^?1 of the NiS₂@C@C, which are also notable. Given such remarkable electrochemical properties, this work is expected to provide more possibilities for the reasonable design of advanced electrode materials for metal sulfide potassium ion batteries.     

Face‐to‐Face Contact and Open‐Void Coinvolved Si/C Nanohybrids Lithium‐Ion Battery Anodes with Extremely Long Cycle Life

To develop high‐performance anode materials of lithium‐ion batteries (LIBs) instead of commercial graphite for practical applications, herein, a layer of silicon has been well‐anchored onto a 3D graphene/carbon nanotube (CNT) aerogels (CAs) framework with face‐to‐face contact and balanced open void by a simple chemical vapor deposition strategy. The engineered contact interface between CAs and Si creates high‐efficiency channels for the rapid electrons and lithium ions transport, and meanwhile, the balanced open‐void allows the free expansion of Si during cycling while maintaining high structural integrity due to the robust mechanical strength of 3D CAs framework. As a consequence, the as‐synthesized Si/CAs nanohybrids are highly stable anode materials for LIBs with a high reversible discharge capacity (1498 mAh g^?1 at 200 mA g^?1) and excellent rate capability (462 mAh g^?1 at 10 000 mA g^?1), which is much better than Si/graphene‐CNTs‐mixture (51 mAh g^?1 at 10 000 mA g^?1). More significantly, it is found that the Si/CAs nanohybrids display no obvious capacity decline even after 2000 cycles at a high current density of 10 000 mA g^?1. The present Si/CAs nanohybrids are one of the most stable Si‐based anode materials ever reported for LIBs to date.     

Few‐Layered SnS2 on Few‐Layered Reduced Graphene Oxide as Na‐Ion Battery Anode with Ultralong Cycle Life and Superior Rate Capability

Na‐ion Batteries have been considered as promising alternatives to Li‐ion batteries due to the natural abundance of sodium resources. Searching for high‐performance anode materials currently becomes a hot topic and also a great challenge for developing Na‐ion batteries. In this work, a novel hybrid anode is synthesized consisting of ultrafine, few‐layered SnS₂ anchored on few‐layered reduced graphene oxide (rGO) by a facile solvothermal route. The SnS₂/rGO hybrid exhibits a high capacity, ultralong cycle life, and superior rate capability. The hybrid can deliver a high charge capacity of 649 mAh g^?1 at 100 mA g^?1. At 800 mA g^?1 (1.8 C), it can yield an initial charge capacity of 469 mAh g^?1, which can be maintained at 89% and 61%, respectively, after 400 and 1000 cycles. The hybrid can also sustain a current density up to 12.8 A g^?1 (≈28 C) where the charge process can be completed in only 1.3 min while still delivering a charge capacity of 337 mAh g^?1. The fast and stable Na‐storage ability of SnS₂/rGO makes it a promising anode for Na‐ion batteries.     

Layered P2‐Type K0.65Fe0.5Mn0.5O2 Microspheres as Superior Cathode for High‐Energy Potassium‐Ion Batteries

Potassium‐ion batteries have been regarded as the potential alternatives to lithium‐ion batteries (LIBs) due to the low cost, earth abundance, and low potential of K (?2.936 vs standard hydrogen electrode (SHE)). However, the lack of low‐cost cathodes with high energy density and long cycle life always limits its application. In this work, high‐energy layered P2‐type hierarchical K_0.65Fe_0.5Mn_0.5O₂ (P2‐KFMO) microspheres, assembled by the primary nanoparticles, are fabricated via a modified solvent‐thermal method. Benefiting from the unique microspheres with primary nanoparticles, the K⁺ intercalation/deintercalation kinetics of P2‐KFMO is greatly enhanced with a stabilized cathodic electrolyte interphase on the cathode. The P2‐KFMO microsphere presents a highly reversible potassium storage capacity of 151 mAh g^?1 at 20 mA g^?1, fast rate capability of 103 mAh g^?1 at 100 mA g^?1, and long cycling stability with 78% capacity retention after 350 cycles. A full cell with P2‐KFMO microspheres as cathode and hard carbon as anode is constructed, which exhibits long‐term cycling stability (>80% of retention after 100 cycles). The present high‐performance P2‐KFMO microsphere cathode synthesized using earth‐abundant elements provides a new cost‐effective alternative to LIBs for large‐scale energy storage.     

Novel Insoluble Organic Cathodes for Advanced Organic K‐Ion Batteries

Organic redox‐active molecules are inborn electrodes to store large‐radius potassium (K) ion. High‐performance organic cathodes are important for practical usage of organic potassium‐ion batteries (OPIBs). However, small‐molecule organic cathodes face serious dissolution problems against liquid electrolytes. A novel insoluble small‐molecule organic cathode [N,N′‐bis(2‐anthraquinone)]‐perylene‐3,4,9,10‐tetracarboxydiimide (PTCDI‐DAQ, 200 mAh g^?1) is initially designed for OPIBs. In half cells (1–3.8 V vs K⁺/K) using 1 m KPF₆ in dimethoxyethane (DME), PTCDI‐DAQ delivers a highly stable specific capacity of 216 mAh g^?1 and still holds the value of 133 mAh g^?1 at an ultrahigh current density of 20 A g^?1 (100 C). Using reduced potassium terephthalate (K₄TP) as the organic anode, the resulting K₄TP||PTCDI‐DAQ OPIBs with the electrolyte 1 m KPF₆ in DME realize a high energy density of maximum 295 Wh kg^?1_cathode (213 mAh g^?1_cathode × 1.38 V) and power density of 13 800 W Kg^?1_cathode (94 mAh g^?1 × 1.38 V @ 10 A g^?1) during the working voltage of 0.2–3.2 V. Meanwhile, K₄TP||PTCDI‐DAQ OPIBs fulfill the superlong lifespan with a stable discharge capacity of 62 mAh g^?1_cathode after 10 000 cycles and 40 mAh g^?1_cathode after 30 000 cycles (3 A g^?1). The integrated performance of PTCDI‐DAQ can currently defeat any cathode reported in K‐ion half/full cells.     

2D Nanospace Confined Synthesis of Pseudocapacitance‐Dominated MoS2‐in‐Ti3C2 Superstructure for Ultrafast and Stable Li/Na‐Ion Batteries

Exploring a universal strategy to implement the precise control of 2D nanomaterials in size and layer number is a big challenge for achieving ultrafast and stable Li/Na‐ion batteries. Herein, the confined synthesis of 1–3 layered MoS₂ nanocrystals into 2D Ti₃C₂ interlayer nanospace with the help of electrostatic attraction and subsequent cetyltrimethyl ammonium bromide (CTAB) directed growth is reported. The MoS₂ nanocrystals are tightly anchored into the interlayer by 2D confinement effect and strong Mo? C covalent bond. Impressively, the disappearance of Li⁺ intercalated into MoS₂ reduction peak is successfully observed for the first time in the experiment, showing in a typical surface‐controlled charge storage behavior. The pseudocapacitance‐dominated contribution guarantees a much faster and more stable Li/Na storage performance. As predicted, this electrode exhibits a very high Li⁺ storage capacity of 340 mAh g^?1 even at 20 A g^?1 and a long cycle life (>1000 times). It also shows an excellent Na⁺ storage capacity of 310 mAh g^?1 at 1 A g^?1 with a 1600 times high‐rate cycling. Such impressive confined synthesis strategy can be extended to the precise control of other 2D nanomaterials.     

Lithium Accommodation in a Redox‐Active Covalent Triazine Framework for High Areal Capacity and Fast‐Charging Lithium‐Ion Batteries

The synthesis of a new type of redox‐active covalent triazine framework (rCTF) material, which is promising as an anode for Li‐ion batteries, is reported. After activation, it has a capacity up to ≈1190 mAh g^?1 at 0.5C with a current density of 300 mA g^?1 and a high cycling stability of over 1000 discharge/charge cycles with a stable Coulombic efficiency in an rCTF/Li half‐cell. This rCTF has a high rate performance, and at a charging rate of 20C with a current density of 12 A g^?1 and it functions well for over 1000 discharge/charge cycles with a reversible capacity of over 500 mAh g^?1. By electrochemical analysis and theoretical calculations, it is found that its lithium‐storage mechanism involves multi‐electron redox‐reactions at anthraquinone, triazine, and benzene rings by the accommodation of Li. The structural features and progressively increased structural disorder of the rCTF increase the kinetics of infiltration and significantly shortens the activation period, yielding fast‐charging Li‐ion half and full cells even at a high capacity loading.     

Potassium Prussian Blue Nanoparticles: A Low‐Cost Cathode Material for Potassium‐Ion Batteries

Potassium‐ion batteries (KIBs) in organic electrolytes hold great promise as an electrochemical energy storage technology owing to the abundance of potassium, close redox potential to lithium, and similar electrochemistry with lithium system. Although carbon materials have been studied as KIB anodes, investigations on KIB cathodes have been scarcely reported. A comprehensive study on potassium Prussian blue K_0.220Fe[Fe(CN)₆]_0.805?4.01H₂O nanoparticles as a potential cathode material is for the first time reported. The cathode exhibits a high discharge voltage of 3.1–3.4 V, a high reversible capacity of 73.2 mAh g^?1, and great cyclability at both low and high rates with a very small capacity decay rate of ≈0.09% per cycle. Electrochemical reaction mechanism analysis identifies the carbon‐coordinated Fe^III/Fe^II couple as redox‐active site and proves structural stability of the cathode during charge/discharge. Furthermore, for the first time, a KIB full‐cell is presented by coupling the nanoparticles with commercial carbon materials. The full‐cell delivers a capacity of 68.5 mAh g^?1 at 100 mA g^?1 and retains 93.4% of the capacity after 50 cycles. Considering the low cost and material sustainability as well as the great electrochemical performances, this work may pave the way toward more studies on KIB cathodes and trigger future attention on rechargeable KIBs.     

A General Metal‐Organic Framework (MOF)‐Derived Selenidation Strategy for In Situ Carbon‐Encapsulated Metal Selenides as High‐Rate Anodes for Na‐Ion Batteries

On account of increasing demand for energy storage devices, sodium‐ion batteries (SIBs) with abundant reserve, low cost, and similar electrochemical properties have the potential to partly replace the commercial lithium‐ion batteries. In this study, a facile metal‐organic framework (MOF)‐derived selenidation strategy to synthesize in situ carbon‐encapsulated selenides as superior anode for SIBs is rationally designed. These selenides with particular micro‐ and nanostructured features deliver ultrastable cycling performance at high charge–discharge rate and demonstrate ultraexcellent rate capability. For example, the uniform peapod‐like Fe₇Se₈@C nanorods represent a high specific capacity of 218 mAh g^?1 after 500 cycles at 3 A g^?1 and the porous NiSe@C spheres display a high specific capacity of 160 mAh g^?1 after 2000 cycles at 3 A g^?1. The current simple MOF‐derived method could be a promising strategy for boosting the development of new functional inorganic materials for energy storage, catalysis, and sensors.     

Walnut‐Like Multicore–Shell MnO Encapsulated Nitrogen‐Rich Carbon Nanocapsules as Anode Material for Long‐Cycling and Soft‐Packed Lithium‐Ion Batteries

Metal oxide‐based nanomaterials are widely studied because of their high‐energy densities as anode materials in lithium‐ion batteries. However, the fast capacity degradation resulting from the large volume expansion upon lithiation hinders their practical application. In this work, the preparation of walnut‐like multicore–shell MnO encapsulated nitrogen‐rich carbon nanocapsules (MnO@NC) is reported via a facile and eco‐friendly process for long‐cycling Li‐ion batteries. In this hybrid structure, MnO nanoparticles are uniformly dispersed inside carbon nanoshells, which can simultaneously act as a conductive framework and also a protective buffer layer to restrain the volume variation. The MnO@NC nanocapsules show remarkable electrochemical performances for lithium‐ion batteries, exhibiting high reversible capability (762 mAh g^?1 at 100 mA g^?1) and stable cycling life (624 mAh g^?1 after 1000 cycles at 1000 mA g^?1). In addition, the soft‐packed full batteries based on MnO@NC nanocapsules anodes and commercial LiFePO₄ cathodes present good flexibility and cycling stability.     

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).     

Rambutan‐Like Hybrid Hollow Spheres of Carbon Confined Co3O4 Nanoparticles as Advanced Anode Materials for Sodium‐Ion Batteries

Transition metal oxides, possessing high theoretical specific capacities, are promising anode materials for sodium‐ion batteries. However, the sluggish sodiation/desodiation kinetics and poor structural stability restrict their electrochemical performance. To achieve high and fast Na storage capability, in this work, rambutan‐like hybrid hollow spheres of carbon confined Co₃O₄ nanoparticles are synthesized by a facile one‐pot hydrothermal treatment with postannealing. The hierarchy hollow structure with ultrafine Co₃O₄ nanoparticles embedded in the continuous carbon matrix enables greatly enhanced structural stability and fast electrode kinetics. When tested in sodium‐ion batteries, the hollow structured composite electrode exhibits an outstandingly high reversible specific capacity of 712 mAh g^?1 at a current density of 0.1 A g^?1, and retains a capacity of 223 mAh g^?1 even at a large current density of 5 A g^?1. Besides the superior Na storage capability, good cycle performance is demonstrated for the composite electrode with 74.5% capacity retention after 500 cycles, suggesting promising application in advanced sodium‐ion batteries.     

Optimization of Von Mises Stress Distribution in Mesoporous α‐Fe2O3/C Hollow Bowls Synergistically Boosts Gravimetric/Volumetric Capacity and High‐Rate Stability in Alkali‐Ion Batteries

Hollow structures are often used to relieve the intrinsic strain on metal oxide electrodes in alkali‐ion batteries. Nevertheless, one common drawback is that the large interior space leads to low volumetric energy density and inferior electric conductivity. Here, the von Mises stress distribution on a mesoporous hollow bowl (HB) is simulated via the finite element method, and the vital role of the porous HB structure on strain‐relaxation behavior is confirmed. Then, N‐doped‐C coated mesoporous α‐Fe₂O₃ HBs are designed and synthesized using a multistep soft/hard‐templating strategy. The material has several advantages: (i) there is space to accommodate strains without sacrificing volumetric energy density, unlike with hollow spheres; (ii) the mesoporous hollow structure shortens ion diffusion lengths and allows for high‐rate induced lithiation reactivation; and (iii) the N‐doped carbon nanolayer can enhance conductivity. As an anode in lithium‐ion batteries, the material exhibits a very high reversible capacity of 1452 mAh g^?1 at 0.1 A g^?1, excellent cycling stability of 1600 cycles (964 mAh g^?1 at 2 A g^?1), and outstanding rate performance (609 mAh g^?1 at 8 A g^?1). Notably, the volumetric specific capacity of composite electrode is 42% greater than that of hollow spheres. When used in potassium‐ion batteries, the material also shows high capacity and cycle stability.     

Nickel‐Catalyzed Synthesis of 3D Edge‐Curled Graphene for High‐Performance Lithium‐Ion Batteries

Effectively preventing graphene stacking and maintaining ultrathin layers remains a significant research effort for graphene preparation and applications. In this paper, a novel synthetic strategy based on catalyst migration on the surface of a salt template to control the growth of graphene is used to prepare 3D edge‐curled graphene (3D ECG). Under the synergistic effect of the steric hindrance and the migration of the Ni catalyst, 3D ECG forms a special structure in which the intermediate portion is flat and the edge is curled. The resultant unique structure not only effectively prevents the close stacking and aggregation of graphene, but also significantly improves its lithium storage performance. As an anode for lithium ion batteries, the reversible specific capacity can reach 907.5 and 347.8 mAh g^?1 at the current density of 0.05 and 5.0 A g^?1. Even after 1000 cycles, the specific capacity of 3D ECG can still be maintained at 605.2 mAh g^?1 at a current density of 0.5 A g^?1, demonstrating excellent rate performance and cycle performance. This new synthesis strategy and unique edge‐curled structure can be used to guide more design of 3D graphene materials for further functional applications.     

Bamboo‐Like Hollow Tubes with MoS2/N‐Doped‐C Interfaces Boost Potassium‐Ion Storage

Potassium‐ion batteries (KIBs) are new‐concept of low‐cost secondary batteries, but the sluggish kinetics and huge volume expansion during cycling, both rooted in the size of large K ions, lead to poor electrochemical behavior. Here, a bamboo‐like MoS₂/N‐doped‐C hollow tubes are presented with an expanded interlayer distance of 10 Å as a high‐capacity and stable anode material for KIBs. The bamboo‐like structure provides gaps along axial direction in addition to inner cylinder hollow space to mitigate the strains in both radial and vertical directions that ultimately leads to a high structural integrity for stable long‐term cycling. Apart from being a constituent of the interstratified structure the N‐doped‐C layers weave a cage to hold the potassiation products (polysulfide and the Mo nanoparticles) together, thereby effectively hindering the continuing growth of solid electrolyte interphase in the interior of particles. The density functional theory calculations prove that the MoS₂/N‐doped‐C atomic interface can provide an additional attraction toward potassium ion. As a result, it delivers a high capacity at a low current density (330 mAh g^?1 at 50 mA g^?1 after 50 cycles) and a high‐capacity retention at a high current density (151 mAh g^?1 at 500 mA g^?1 after 1000 cycles).