A Flexible 3D Multifunctional MgO‐Decorated Carbon Foam@CNTs Hybrid as Self‐Supported Cathode for High‐Performance Lithium‐Sulfur Batteries

One of the critical challenges to develop advanced lithium‐sulfur (Li‐S) batteries lies in exploring a high efficient stable sulfur cathode with robust conductive framework and high sulfur loading. Herein, a 3D flexible multifunctional hybrid is rationally constructed consisting of nitrogen‐doped carbon foam@CNTs decorated with ultrafine MgO nanoparticles for the use as advanced current collector. The dense carbon nanotubes uniformly wrapped on the carbon foam skeletons enhance the flexibility and build an interconnected conductive network for rapid ionic/electronic transport. In particular, a synergistic action of MgO nanoparticles and in situ N‐doping significantly suppresses the shuttling effect via enhanced chemisorption of lithium polysulfides. Owing to these merits, the as‐built electrode with an ultrahigh sulfur loading of 14.4 mg cm^?2 manifests a high initial areal capacity of 10.4 mAh cm^?2, still retains 8.8 mAh cm^?2 (612 mAh g^?1 in gravimetric capacity) over 50 cycles. The best cycling performance is achieved upon 800 cycles with an extremely low decay rate of 0.06% at 2 C. Furthermore, a flexible soft‐packaged Li‐S battery is readily assembled, which highlights stable electrochemical characteristics under bending and even folding. This cathode structural design may open up a potential avenue for practical application of high‐sulfur‐loading Li‐S batteries toward flexible energy‐storage devices.     

Interfacial Bonding of Metal‐Sulfides with Double Carbon for Improving Reversibility of Advanced Alkali‐Ion Batteries

Engineering interfacial properties of metal‐sulfides toward excellent electrochemical capability is imperative for advanced energy‐storage materials. However, they still suffer from an unclear mechanism of capacity fading, along with ineffective physical–chemical evolution. Herein, a highly‐effective Sb₂S₃ with double carbon is designed with interfacial Sb? C bonds and double carbon, which boosts promoting of ion transferring and alleviates the separation of both active phases (Sb, S). Through “voltage‐cutting” manners, the key elements of capacity improvement about phase transitions are further determined. As expected, even at 5.0 A g^?1, the lithium‐storage capacity remains about 674 mAh g^?1. Utilized as sodium ion battery (SIB) anode, the rate capacity still reaches up to 366 mAh g^?1 at 3.0 A g^?1, much larger than that of Sb₂S₃. Obtaining the full cell of Ni–Fe Prussian blue analog versus M‐Sb₂S₃@DC, the reversible capacity is 330 mAh g^?1 at 0.5 A g^?1. Supported by kinetic analysis, the excellent rate properties are determined by the surface‐controlling behaviors, mainly resulting from the decreased capacitive resistance and improved ion moving. Furthermore, the reassembling evolution of active phases is revealed in detail by ex situ techniques. This work is expected to offer significant insights into interfacial evolutions toward advanced energy‐storage systems.     

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.     

Solid‐State Plastic Crystal Electrolytes: Effective Protection Interlayers for Sulfide‐Based All‐Solid‐State Lithium Metal Batteries

All‐solid‐state lithium metal batteries (ASSLMBs) have attracted significant attention due to their superior safety and high energy density. However, little success has been made in adopting Li metal anodes in sulfide electrolyte (SE)‐based ASSLMBs. The main challenges are the remarkable interfacial reactions and Li dendrite formation between Li metal and SEs. In this work, a solid‐state plastic crystal electrolyte (PCE) is engineered as an interlayer in SE‐based ASSLMBs. It is demonstrated that the PCE interlayer can prevent the interfacial reactions and lithium dendrite formation between SEs and Li metal. As a result, ASSLMBs with LiFePO₄ exhibit a high initial capacity of 148 mAh g^?1 at 0.1 C and 131 mAh g^?1 at 0.5 C (1 C = 170 mA g^?1), which remains at 122 mAh g^?1 after 120 cycles at 0.5 C. All‐solid‐state Li‐S batteries based on the polyacrylonitrile‐sulfur composite are also demonstrated, showing an initial capacity of 1682 mAh g^?1. The second discharge capacity of 890 mAh g^?1 keeps at 775 mAh g^?1 after 100 cycles. This work provides a new avenue to address the interfacial challenges between Li metal and SEs, enabling the successful adoption of Li metal in SE‐based ASSLMBs with high energy density.     

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.     

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.     

3D Carbon Nanotube Network Bridged Hetero‐Structured Ni‐Fe‐S Nanocubes toward High‐Performance Lithium,Sodium, and Potassium Storage

Lithium‐ion, sodium‐ion, and potassium‐ion batteries have captured tremendous attention in power supplies for various electric vehicles and portable electronic devices. However, their practical applications are severely limited by factors such as poor rate capability, fast capacity decay, sluggish charge storage dynamics, and low reversibility. Herein, hetero‐structured bimetallic sulfide (NiS/FeS) encapsulated in N‐doped porous carbon cubes interconnected with CNTs (Ni‐Fe‐S‐CNT) are prepared through a convenient co‐precipitation and post‐heat treatment sulfurization technique of the corresponding Prussian‐blue analogue nanocage precursor. This special 3D hierarchical structure can offer a stable interconnect and conductive network and shorten the diffusion path of ions, thereby greatly enhancing the mobility efficiency of alkali (Li, Na, K) ions in electrode materials. The Ni‐Fe‐S‐CNT nanocomposite maintains a charge capacity of 1535 mAh g^?1 at 0.2 A g^?1 for lithium ion batteries, 431 mAh g^?1 at 0.1 A g^?1 for sodium ion batteries, and 181 mAh g^?1 at 0.1 A g^?1 for potassium‐ion batteries, respectively. The high performance is mainly attributed to the 3D hierarchically high‐conductivity network architecture, in which the hetero‐structured FeS/NiS nanocubes provide fast Li⁺/Na⁺/K⁺ insertion/extraction and reduced ion diffusion paths, and the distinctive 3D networks maintain the electrical contact and guarantee the structural integrity.     

Functional Mesoporous Carbon‐Coated Separator for Long‐Life,High‐Energy Lithium–Sulfur Batteries

The lithium–sulfur (Li–S) battery is regarded as the most promising rechargeable energy storage technology for the increasing applications of clean energy transportation systems due to its remarkable high theoretical energy density of 2.6 kWh kg^?1, considerably outperforming today's lithium‐ion batteries. Additionally, the use of sulfur as active cathode material has the advantages of being inexpensive, environmentally benign, and naturally abundant. However, the insulating nature of sulfur, the fast capacity fading, and the short lifespan of Li–S batteries have been hampered their commercialization. In this paper, a functional mesoporous carbon‐coated separator is presented for improving the overall performance of Li–S batteries. A straightforward coating modification of the commercial polypropylene separator allows the integration of a conductive mesoporous carbon layer which offers a physical place to localize dissolved polysulfide intermediates and retain them as active material within the cathode side. Despite the use of a simple sulfur–carbon black mixture as cathode, the Li–S cell with a mesoporous carbon‐coated separator offers outstanding performance with an initial capacity of 1378 mAh g^?1 at 0.2 C, and high reversible capacity of 723 mAh g^?1, and degradation rate of only 0.081% per cycle, after 500 cycles at 0.5 C.     

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.     

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.     

Bifunctional MOF‐Derived Carbon Photonic Crystal Architectures for Advanced Zn–Air and Li–S Batteries: Highly Exposed Graphitic Nitrogen Matters

Nitrogen‐rich porous carbons (NPCs) are the leading cathode materials for next‐generation Zn–air and Li–S batteries. However, most existing NPC suffers from insufficient exposure and harnessing of nitrogen‐dopants (NDs), constraining the electrochemical performance. Herein, by combining silica templating with in situ texturing of metal–organic frameworks, a new bifunctional 3D nitrogen‐rich carbon photonic crystal architecture of simultaneously record‐high total pore volume (13.42 cm³ g^?1), ultralarge surface area (2546 m² g^?1), and permeable hierarchical macro‐meso‐microporosity is designed, enabling sufficient exposure and accessibility of NDs. Thus, when used as cathode catalysts, the Zn–air battery delivers a fantastic capacity of 770 mAh g_Zn^?1 at an unprecedentedly high rate of 120 mA cm^?2, with an ultrahigh power density of 197 mW cm^?2. When hosting 78 wt% sulfur, the Li–S battery affords a high‐rate capacity of 967 mAh g^?1 at 2 C, with superb stability over 1000 cycles at 0.5 C (0.054% decay rate per cycle), comparable to the best literature value. The results prove the dominant role of highly exposed graphitic‐N in boosting both cathode performances.     

FeP Quantum Dots Confined in Carbon‐Nanotube‐Grafted P‐Doped Carbon Octahedra for High‐Rate Sodium Storage and Full‐Cell Applications

Transition metal phosphides (TMPs) possess high theoretical sodium storage capacities, but suffer from poor rate performance, due to their intrinsic low conductivity and large volume expansion upon sodiation/desodiation. Compositing TMPs with carbon materials or downsizing their feature size are recognized as efficient approaches to address the above issues. Nevertheless the surface‐controlled capacitive behavior is generally dominated, which inevitably compromises the charge/discharge platform, and decreases the operational potential window in full‐cell constructions. In this work, a novel architecture (FeP@OCF) with FeP quantum dots confined in P‐doped 3D octahedral carbon framework/carbon nanotube is rationally designed. Such structure enables a simultaneous enhancement on the diffusion‐controlled capacity in the platform region (2.3 folds), and the surface‐controlled capacity in the slope region (2.9 folds) as compared to that of pure FeP. As a result, an excellent reversible capacity (674 mAh g^?1@ 0.1 A g^?1) and a record high‐rate performance (262 mAh g^?1 @ 20 A g^?1) are achieved. A full‐cell FeP@OCF// Na₃V₂(PO₄)₃ is also constructed showing an outstandingly high energy density of 185 Wh kg^?1 (based on the total mass of active materials in both electrodes), which outperforms the state‐of‐the art TMP‐based sodium‐ion battery full cells.     

A High‐Energy Li‐Ion Battery Using a Silicon‐Based Anode and a Nano‐Structured Layered Composite Cathode

High capacity electrodes based on a Si composite anode and a layered composite oxide cathode, Ni‐rich Li[Ni_0.75Co_0.1Mn_0.15]O₂, are evaluated and combined to fabricate a high energy lithium ion battery. The Si composite anode, Si/C‐IWGS (internally wired with graphene sheets), is prepared by a scalable sol–gel process. The Si/C‐IWGS anode delivers a high capacity of >800 mAh g^?1 with an excellent cycling stability of up to 200 cycles, mainly due to the small amount of graphene (～6 wt%). The cathode (Li[Ni_0.75Co_0.1Mn_0.15]O₂) is structurally optimized (Ni‐rich core and a Ni‐depleted shell with a continuous concentration gradient between the core and shell, i.e., a full concentration gradient, FCG, cathode) so as to deliver a high capacity (>200 mAh g^?1) with excellent stability at high voltage (～4.3 V). A novel lithium ion battery system based on the Si/C‐IWGS anode and FCG cathode successfully demonstrates a high energy density (240 Wh kg^?1 at least) as well as an unprecedented excellent cycling stability of up to 750 cycles between 2.7 and 4.2 V at 1C. As a result, the novel battery system is an attractive candidate for energy storage applications demanding a high energy density and long cycle life.     

Electronic Structure Regulation of Layered Vanadium Oxide via Interlayer Doping Strategy toward Superior High‐Rate and Low‐Temperature Zinc‐Ion Batteries

Currently, development of suitable cathode materials for zinc‐ion batteries (ZIBs) is plagued by the sluggish kinetics of Zn²⁺ with multivalent charge in the host structure. Herein, it is demonstrated that interlayer Mn²⁺‐doped layered vanadium oxide (Mn_0.15V₂O₅·nH₂O) composites with narrowed direct bandgap manifest greatly boosted electrochemical performance as zinc‐ion battery cathodes. Specifically, the Mn_0.15V₂O₅·nH₂O electrode shows a high specific capacity of 367 mAh g^?1 at a current density of 0.1 A g^?1 as well as excellent retentive capacities of 153 and 122 mAh g^?1 after 8000 cycles at high current densities up to 10 and 20 A g^?1, respectively. Even at a low temperature of ?20 °C, a reversible specific capacity of 100 mAh g^?1 can be achieved at a current density of 2.0 A g^?1 after 3000 cycles. The superior electrochemical performance originates from the synergistic effects between the layered nanostructures and interlayer doping of Mn²⁺ ions and water molecules, which can enhance the electrons/ions transport kinetics and structural stability during cycling. With the aid of various ex situ characterization technologies and density functional theory calculations, the zinc‐ion storage mechanism can be revealed, which provides fundamental guidelines for developing high‐performance cathodes for ZIBs.     

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).     

Metal–Organic Framework (MOF) Derived Electrodes with Robust and Fast Lithium Storage for Li‐Ion Hybrid Capacitors

Hybrid metal–organic frameworks (MOFs) demonstrate great promise as ideal electrode materials for energy‐related applications. Herein, a well‐organized interleaved composite of graphene‐like nanosheets embedded with MnO₂ nanoparticles (MnO₂@C‐NS) using a manganese‐based MOF and employed as a promising anode material for Li‐ion hybrid capacitor (LIHC) is engineered. This unique hybrid architecture shows intriguing electrochemical properties including high reversible specific capacity 1054 mAh g^?1 (close to the theoretical capacity of MnO₂, 1232 mAh g^?1) at 0.1 A g^?1 with remarkable rate capability and cyclic stability (90% over 1000 cycles). Such a remarkable performance may be assigned to the hierarchical porous ultrathin carbon nanosheets and tightly attached MnO₂ nanoparticles, which provide structural stability and low contact resistance during repetitive lithiation/delithiation processes. Moreover, a novel LIHC is assembled using a MnO₂@C‐NS anode and MOF derived ultrathin nanoporous carbon nanosheets (derived from other potassium‐based MOFs) cathode materials. The LIHC full‐cell delivers an ultrahigh specific energy of 166 Wh kg^?1 at 550 W kg^?1 and maintained to 49.2 Wh kg^?1 even at high specific power of 3.5 kW kg^?1 as well as long cycling stability (91% over 5000 cycles). This work opens new opportunities for designing advanced MOF derived electrodes for next‐generation energy storage devices.     

Tailoring 2D Heteroatom‐Doped Carbon Nanosheets with Dominated Pseudocapacitive Behaviors Enabling Fast and High‐Performance Sodium Storage

2D carbon nanosheets are considered to be promising candidates for use as sodium ion battery (SIB) anodes due to their large specific surface area and excellent electronic conductivity. However, their applications are hampered by inferior cycling performance, insufficient storage capacity, and high cost. N, B co‐doping carbon nanosheets (NBTs) are synthesized using biomass‐based gelatin as carbon precursor and boric acid as template, and demonstrate their great potential as high‐performance SIB anodes in practical applications. The synergistic effect of heteroatom doping and ultrathin 2D structure provides the NBTs with abundant defects, active sites, and short ion/electron transfer distance, which favors and improves the storage capabilities and rate performances. The optimized NBTs present a remarkable cyclability and superb rate capability (309 mAh g^?1 at 0.2 A g^?1 for 200 cycles; 225 mAh g^?1 at 1 A g^?1 for 2000 cycles). Meanwhile, the Na storage mechanism is proved to be a pseudocapacitive‐controlled process, which accounts for the fast charge/discharge behaviors. This work demonstrates an effective template method to produce 2D heteroatoms co‐doping carbon nanosheets to achieve excellent Na storage performances.     

Zn(Cu)Si2+xP3 Solid Solution Anodes for High‐Performance Li‐Ion Batteries with Tunable Working Potentials

Si‐based anodes with a stiff diamond structure usually suffer from sluggish lithiation/delithiation reaction due to low Li‐ion and electronic conductivity. Here, a novel ternary compound ZnSi₂P₃ with a cation‐disordered sphalerite structure, prepared by a facile mechanochemical method, is reported, demonstrating faster Li‐ion and electron transport and greater tolerance to volume change during cycling than the existing Si‐based anodes. A composite electrode consisting of ZnSi₂P₃ and carbon achieves a high initial Coulombic efficiency (92%) and excellent rate capability (950 mAh g^?1 at 10 A g^?1) while maintaining superior cycling stability (1955 mAh g^?1 after 500 cycles at 300 mA g^?1), surpassing the performance of most Si‐ and P‐based anodes ever reported. The remarkable electrochemical performance is attributed to the sphalerite structure that allows fast ion and electron transport and the reversible Li‐storage mechanism involving intercalation and conversion reactions. Moreover, the cation‐disordered sphalerite structure is flexible to ionic substitutions, allowing extension to a family of Zn(Cu)Si_2+xP₃ solid solution anodes (x = 0, 2, 5, 10) with large capacity, high initial Coulombic efficiency, and tunable working potentials, representing attractive anode candidates for next‐generation, high‐performance, and low‐cost Li‐ion batteries.     

Nanoarchitectured Graphene/CNT@Porous Carbon with Extraordinary Electrical Conductivity and Interconnected Micro/Mesopores for Lithium‐Sulfur Batteries

The sp²‐hybridized nanocarbon (e.g., carbon nanotubes (CNTs) and graphene) exhibits extraordinary mechanical strength and electrical conductivity but limited external accessible surface area and a small amount of pores, while nanostructured porous carbon affords a huge surface area and abundant pore structures but very poor electrical conductance. Herein the rational hybridization of the sp² nanocarbon and nanostructured porous carbon into hierarchical all‐carbon nanoarchitectures is demonstrated, with full inherited advantages of the component materials. The sp² graphene/CNT interlinked networks give the composites good electrical conductivity and a robust framework, while the meso‐/microporous carbon and the interlamellar compartment between the opposite graphene accommodate sulfur and polysulfides. The strong confinement induced by micro‐/mesopores of all‐carbon nanoarchitectures renders the transformation of S₈ crystal into amorphous cyclo‐S₈ molecular clusters, restraining the shuttle phenomenon for high capacity retention of a lithium‐sulfur cell. Therefore, the composite cathode with an ultrahigh specific capacity of 1121 mAh g^?1 at 0.5 C, a favorable high‐rate capability of 809 mAh g^?1 at 10 C, a very low capacity decay of 0.12% per cycle, and an impressive cycling stability of 877 mAh g^?1 after 150 cycles at 1 C. As sulfur loading increases from 50 wt% to 77 wt%, high capacities of 970, 914, and 613 mAh g^?1 are still available at current densities of 0.5, 1, and 5 C, respectively. Based on the total mass of packaged devices, gravimetric energy density of GSH@APC‐S//Li cell is expected to be 400 Wh kg^?1 at a power density of 10 000 W kg^?1, matching the level of engine driven systems.     

Amorphous GaN@Cu Freestanding Electrode for High‐Performance Li‐Ion Batteries

GaN is demonstrated to be an ideal anode for Li‐ion batteries (LIBs) for the first time. Amorphous GaN@Cu nanorods (a‐GaN@Cu) freestanding electrode is designed via a low‐temperature pulsed laser deposition method, which exhibits prominent rate capability and untralong lifespan as an anode for LIBs. With porous interconnected metal nanorods substrate to improve the structure integrity and electronic conductivity, the a‐GaN@Cu electrode delivers a capacity recovery of 980 mAh g^?1 after 150 cycles from 0.25 to 6.25 A g^?1 and a high discharge capacity of 509 mAh g^?1 after 3000 cycles at 10.0 A g^?1. The lithium storage in the a‐GaN is also systematically studied, which suggests a redox reaction mechanism.