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.     

Anionic Se‐Substitution toward High‐Performance CuS1−xSex Nanosheet Cathode for Rechargeable Magnesium Batteries

Rechargeable magnesium batteries (rMBs) are promising as the most ideal further energy storage systems but lack competent cathode materials due to sluggish redox reaction kinetics. Herein, developed is an anionic Se‐substitution strategy to improve the rate capability and the cycling stability of 2D CuS_1?xSe_x nanosheet cathodes through an efficient microwave‐induced heating method. The optimized CuS_1?xSe_x (X = 0.2) nanosheet cathode can exhibit high reversible capacity of 268.5 mAh g^?1 at 20 mA g^?1 and good cycling stability (140.4 mAh g^?1 at 300 mA g^?1 upon 100 cycles). Moreover, the CuS_1?xSe_x (X = 0.2) nanosheet cathode can deliver remarkable rate capability with a reversible capacity of 119.2 mAh g^?1 at 500 mA g^?1, much higher than the 21.7 mAh g^?1 of pristine CuS nanosheets. The superior electrochemical performance can be ascribed to the enhanced reaction kinetics, enriched cation storage active sites, and shortened ion diffusion pathway of the CuS_1?xSe_x nanosheet. Therefore, tuning anionic chemical composition demonstrates an effective strategy to develop novel cathode materials for rMBs.     

Investigation of Binary Metal (Ni,Co) Selenite as Li‐Ion Battery Anode Materials and Their Conversion Reaction Mechanism with Li Ions

Highly efficient anode materials with novel compositions for Li‐ion batteries are actively being researched. Multicomponent metal selenite is a promising candidate, capable of improving their electrochemical performance through the formation of metal oxide and selenide heterostructure nanocrystals during the first cycle. Here, the binary nickel–cobalt selenite derived from Ni–Co Prussian blue analogs (PBA) is chosen as the first target material: the Ni–Co PBA are selenized and partially oxidized in sequence, yielding (NiCo)SeO₃ phase with a small amount of metal selenate. The conversion mechanism of (NiCo)SeO₃ for Li‐ion storage is studied by cyclic voltammetry, in situ X‐ray diffraction, ex situ X‐ray photoelectron spectroscopy, in situ electrochemical impedance spectroscopy, and ex situ transmission electron microscopy. The reversible reaction mechanism of (NiCo)SeO₃ with the Li ions is described by the reaction: NiO + CoO + xSeO₂ + (1 ‐ x)Se + (4x + 6)Li⁺ + (4x + 6)e^? ? Ni + Co + (2x + 2)Li₂O + Li₂Se. To enhance electrochemical properties, polydopamine‐derived carbon is uniformly coated on (NiCo)SeO₃, resulting in excellent cycling and rate performances for Li‐ion storage. The discharge capacity of C‐coated (NiCo)SeO₃ is 680 mAh g^?1 for the 1500th cycle when cycled at a current density of 5 A g^?1.     

Yolk–Shell MnO@ZnMn2O4/N–C Nanorods Derived from α‐MnO2/ZIF‐8 as Anode Materials for Lithium Ion Batteries

Manganese oxides (MnO_x) are promising anode materials for lithium ion batteries, but they generally exhibit mediocre performances due to intrinsic low ionic conductivity, high polarization, and poor stability. Herein, yolk–shell nanorods comprising of nitrogen‐doped carbon (N–C) coating on manganese monoxide (MnO) coupled with zinc manganate (ZnMn₂O₄) nanoparticles are manufactured via one‐step carbonization of α‐MnO₂/ZIF‐8 precursors. When evaluated as anodes for lithium ion batteries, MnO@ZnMn₂O₄/N–C exhibits an reversible capacity of 803 mAh g^?1 at 50 mA g^?1 after 100 cycles, excellent cyclability with a capacity of 595 mAh g^?1 at 1000 mAg^?1 after 200 cycles, as well as better rate capability compared with those non‐N–C shelled manganese oxides (MnO_x). The outstanding electrochemical performance is attributed to the unique yolk–shell nanorod structure, the coating effect of N–C and nanoscale size.     

Birnessite Nanosheet Arrays with High K Content as a High‐Capacity and Ultrastable Cathode for K‐Ion Batteries

Potassium‐ion batteries (PIBs) are one of the emerging energy‐storage technologies due to the low cost of potassium and theoretically high energy density. However, the development of PIBs is hindered by the poor K⁺ transport kinetics and the structural instability of the cathode materials during K⁺ intercalation/deintercalation. In this work, birnessite nanosheet arrays with high K content (K_0.77MnO₂?0.23H₂O) are prepared by “hydrothermal potassiation” as a potential cathode for PIBs, demonstrating ultrahigh reversible specific capacity of about 134 mAh g^?1 at a current density of 100 mA g^?1, as well as great rate capability (77 mAh g^?1 at 1000 mA g^?1) and superior cycling stability (80.5% capacity retention after 1000 cycles at 1000 mA g^?1). With the introduction of adequate K⁺ ions in the interlayer, the K‐birnessite exhibits highly stabilized layered structure with highly reversible structure variation upon K⁺ intercalation/deintercalation. The practical feasibility of the K‐birnessite cathode in PIBs is further demonstrated by constructing full cells with a hard–soft composite carbon anode. This study highlights effective K⁺‐intercalation for birnessite to achieve superior K‐storage performance for PIBs, making it a general strategy for developing high‐performance cathodes in rechargeable batteries beyond lithium‐ion batteries.     

α‐Fe2O3 Nanoparticles Decorated C@MoS2 Nanosheet Arrays with Expanded Spacing of (002) Plane for Ultrafast and High Li/Na‐Ion Storage

MoS₂ nanosheets as a promising 2D nanomaterial have extensive applications in energy storage and conversion, but their electrochemical performance is still unsatisfactory as an anode for efficient Li⁺/Na⁺ storage. In this work, the design and synthesis of vertically grown MoS₂ nanosheet arrays, decorated with graphite carbon and Fe₂O₃ nanoparticles, on flexible carbon fiber cloth (denoted as Fe₂O₃@C@MoS₂/CFC) is reported. When evaluated as an anode for lithium‐ion batteries, the Fe₂O₃@C@MoS₂/CFC electrode manifests an outstanding electrochemical performance with a high discharge capacity of 1541.2 mAh g^?1 at 0.1 A g^?1 and a good capacity retention of 80.1% at 1.0 A g^?1 after 500 cycles. As for sodium‐ion batteries, it retains a high reversible capacity of 889.4 mAh g^?1 at 0.5 A g^?1 over 200 cycles. The superior electrochemical performance mainly results from the unique 3D ordered Fe₂O₃@C@MoS₂ array‐type nanostructures and the synergistic effect between the C@MoS₂ nanosheet arrays and Fe₂O₃ nanoparticles. The Fe₂O₃ nanoparticles act as spacers to steady the structure, and the graphite carbon could be incorporated into MoS₂ nanosheets to improve the conductivity of the whole electrode and strengthen the integration of MoS₂ nanosheets and CFC by the adhesive role, together ensuring high conductivity and mechanical stability.     

Efficient Laser‐Induced Construction of Oxygen‐Vacancy Abundant Nano‐ZnCo2O4/Porous Reduced Graphene Oxide Hybrids toward Exceptional Capacitive Lithium Storage

Recently, binary ZnCo₂O₄ has drawn enormous attention for lithium‐ion batteries (LIBs) as attractive anode owing to its large theoretical capacity and good environmental benignity. However, the modest electrical conductivity and serious volumetric effect/particle agglomeration over cycling hinder its extensive applications. To address the concerns, herein, a rapid laser‐irradiation methodology is firstly devised toward efficient synthesis of oxygen‐vacancy abundant nano‐ZnCo₂O₄/porous reduced graphene oxide (rGO) hybrids as anodes for LIBs. The synergistic contributions from nano‐dimensional ZnCo₂O₄ with rich oxygen vacancies and flexible rGO guarantee abundant active sites, fast electron/ion transport, and robust structural stability, and inhibit the agglomeration of nanoscale ZnCo₂O₄, favoring for superb electrochemical lithium‐storage performance. More encouragingly, the optimal L‐ZCO@rGO‐30 anode exhibits a large reversible capacity of ≈1053 mAh g^?1 at 0.05 A g^?1, excellent cycling stability (≈746 mAh g^?1 at 1.0 A g^?1 after 250 cycles), and preeminent rate capability (≈686 mAh g^?1 at 3.2 A g^?1). Further kinetic analysis corroborates that the capacitive‐controlled process dominates the involved electrochemical reactions of hybrid anodes. More significantly, this rational design holds the promise of being extended for smart fabrication of other oxygen‐vacancy abundant metal oxide/porous rGO hybrids toward advanced LIBs and beyond.     

Multishelled NixCo3–xO4 Hollow Microspheres Derived from Bimetal–Organic Frameworks as Anode Materials for High‐Performance Lithium‐Ion Batteries

Metal–organic frameworks (MOFs) featuring versatile topological architectures are considered to be efficient self‐sacrificial templates to achieve mesoporous nanostructured materials. A facile and cost‐efficient strategy is developed to scalably fabricate binary metal oxides with complex hollow interior structures and tunable compositions. Bimetal–organic frameworks of Ni‐Co‐BTC solid microspheres with diverse Ni/Co ratios are readily prepared by solvothermal method to induce the Ni _x Co_{3? x} O₄ multishelled hollow microspheres through a morphology‐inherited annealing treatment. The obtained mixed metal oxides are demonstrated to be composed of nanometer‐sized subunits in the shells and large void spaces left between adjacent shells. When evaluated as anode materials for lithium‐ion batteries, Ni _x Co_{3? x} O₄‐0.1 multishelled hollow microspheres deliver a high reversible capacity of 1109.8 mAh g^?1 after 100 cycles at a current density of 100 mA g^?1 with an excellent high‐rate capability. Appropriate capacities of 832 and 673 mAh g^?1 could also be retained after 300 cycles at large currents of 1 and 2 A g^?1, respectively. These prominent electrochemical properties raise a concept of synthesizing MOFs‐derived mixed metal oxides with multishelled hollow structures for progressive lithium‐ion batteries.     

MOF‐Derived CuS@Cu‐BTC Composites as High‐Performance Anodes for Lithium‐Ion Batteries

The CuS(x wt%)@Cu‐BTC (BTC = 1,3,5‐benzenetricarboxylate; x = 3, 10, 33, 58, 70, 99.9) materials are synthesized by a facile sulfidation reaction. The composites are composed of octahedral Cu₃(BTC)₂·(H₂O)₃ (Cu‐BTC) with a large specific surface area and CuS with a high conductivity. The as‐prepared CuS@Cu‐BTC products are first applied as the anodes of lithium‐ion batteries (LIBs). The synergistic effect between Cu‐BTC and CuS components can not only accommodate the volume change and stress relaxation of electrodes but also facilitate the fast transport of Li ions. Thus, it can greatly suppress the transformation process from Li₂S to polysulfides by improving the reversibility of the conversion reaction. Benefiting from the unique structural features, the optimal CuS(70 wt%)@Cu‐BTC sample exhibits a remarkably improved electrochemical performance, showing an over‐theoretical capacity up to 1609 mAh g^?1 after 200 cycles (100 mA g^?1) with an excellent rate‐capability of ≈490 mAh g^?1 at 1000 mA g^?1. The outstanding LIB properties indicate that the CuS(70 wt%)@Cu‐BTC sample is a highly desirable electrode material candidate for high‐performance LIBs.     

O3‐Type Layered Ni‐Rich Oxide: A High‐Capacity and Superior‐Rate Cathode for Sodium‐Ion Batteries

Inspired by its high‐active and open layered framework for fast Li⁺ extraction/insertion reactions, layered Ni‐rich oxide is proposed as an outstanding Na‐intercalated cathode for high‐performance sodium‐ion batteries. An O3‐type Na_0.75Ni_0.82Co_0.12Mn_0.06O₂ is achieved through a facile electrochemical ion‐exchange strategy in which Li⁺ ions are first extracted from the LiNi_0.82Co_0.12Mn_0.06O₂ cathode and Na⁺ ions are then inserted into a layered oxide framework. Furthermore, the reaction mechanism of layered Ni‐rich oxide during Na⁺ extraction/insertion is investigated in detail by combining ex situ X‐ray diffraction, X‐ray photoelectron spectroscopy, and electron energy loss spectroscopy. As an excellent cathode for Na‐ion batteries, O3‐type Na_0.75Ni_0.82Co_0.12Mn_0.06O₂ delivers a high reversible capacity of 171 mAh g^?1 and a remarkably stable discharge voltage of 2.8 V during long‐term cycling. In addition, the fast Na⁺ transport in the cathode enables high rate capability with 89 mAh g^?1 at 9 C. The as‐prepared Ni‐rich oxide cathode is expected to significantly break through the limited performance of current sodium‐ion batteries.     

Construction of Bimetallic Selenides Encapsulated in Nitrogen/Sulfur Co‐Doped Hollow Carbon Nanospheres for High‐Performance Sodium/Potassium‐Ion Half/Full Batteries

Metallic selenides have been widely investigated as promising electrode materials for metal‐ion batteries based on their relatively high theoretical capacity. However, rapid capacity decay and structural collapse resulting from the larger‐sized Na⁺/K⁺ greatly hamper their application. Herein, a bimetallic selenide (MoSe₂/CoSe₂) encapsulated in nitrogen, sulfur‐codoped hollow carbon nanospheres interconnected reduced graphene oxide nanosheets (rGO@MCSe) are successfully designed as advanced anode materials for Na/K‐ion batteries. As expected, the significant pseudocapacitive charge storage behavior substantially contributes to superior rate capability. Specifically, it achieves a high reversible specific capacity of 311 mAh g^?1 at 10 A g^?1 in NIBs and 310 mAh g^?1 at 5 A g^?1 in KIBs. A combination of ex situ X‐ray diffraction, Raman spectroscopy, and transmission electron microscopy tests reveals the phase transition of rGO@MCSe in NIBs/KIBs. Unexpectedly, they show quite different Na⁺/K⁺ insertion/extraction reaction mechanisms for both cells, maybe due to more sluggish K⁺ diffusion kinetics than that of Na⁺. More significantly, it shows excellent energy storage properties in Na/K‐ion full cells when coupled with Na₃V₂(PO₄)₂O₂F and PTCDA@450 °C cathodes. This work offers an advanced electrode construction guidance for the development of high‐performance energy storage devices.     

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

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

Graphene‐Encapsulated FeS2 in Carbon Fibers as High Reversible Anodes for Na+/K+ Batteries in a Wide Temperature Range

Developing low cost, long life, and high capacity rechargeable batteries is a critical factor towards developing next‐generation energy storage devices for practical applications. Therefore, a simple method to prepare graphene‐coated FeS₂ embedded in carbon nanofibers is employed; the double protection from graphene coating and carbon fibers ensures high reversibility of FeS₂ during sodiation/desodiation and improved conductivity, resulting in high rate capacity and long‐term life for Na⁺ (305.5 mAh g^?1 at 3 A g^?1 after 2450 cycles) and K⁺ (120 mAh g^?1 at 1 A g^?1 after 680 cycles) storage at room temperature. Benefitting from the enhanced conductivity and protection on graphene‐encapsulated FeS₂ nanoparticles, the composites exhibit excellent electrochemical performance under low temperature (0 and ?20 °C), and temperature tolerance with stable capacity as sodium‐ion half‐cells. The Na‐ion full‐cells based on the above composites and Na₃V₂(PO₄)₃ can afford reversible capacity of 95 mAh g^?1 at room temperature. Furthermore, the full‐cells deliver promising discharge capacity (50 mAh g^?1 at 0 °C, 43 mAh g^?1 at ?20 °C) and high energy density at low temperatures. Density functional theory calculations imply that graphene coating can effectively decrease the Na⁺ diffusion barrier between FeS₂ and graphene heterointerface and promote the reversibility of Na⁺ storage in FeS₂, resulting in advanced Na⁺ storage properties.     

Mechanochemical Synthesis of γ‐Graphyne with Enhanced Lithium Storage Performance

γ‐Graphyne is a new nanostructured carbon material with large theoretical Li⁺ storage due to its unique large conjugate rings, which makes it a potential anode for high‐capacity lithium‐ion batteries (LIBs). In this work, γ‐graphyne‐based high‐capacity LIBs are demonstrated experimentally. γ‐Graphyne is synthesized through mechanochemical and calcination processes by using CaC₂ and C₆Br₆. Brunauer–Emmett–Teller, atomic force microscopy, X‐ray photoelectron spectroscopy, solid‐state ¹³C NMR and Raman spectra are conducted to confirm its morphology and chemical structure. The sample presents 2D mesoporous structure and is exactly composed of sp and sp²‐hybridized carbon atoms as the γ‐graphyne structure. The electrode shows high Li⁺ storage (1104.5 mAh g^?1 at 100 mA g^?1) and rate capability (435.1 mAh g^?1 at 5 A g^?1). The capacity retention can be up to 948.6 (200 mA g^?1 for 350 cycles) and 730.4 mAh g^?1 (1 A g^?1 for 600 cycles), respectively. These excellent electrochemical performances are ascribed to the mesoporous architecture, large conjugate rings, enlarged interplanar distance, and high structural integrity for fast Li⁺ diffusion and improved cycling stability in γ‐graphyne. This work provides an environmentally benign and cost‐effective mechanochemical method to synthesize γ‐graphyne and demonstrates its superior Li⁺ storage experimentally.     

A Robust and Conductive Black Tin Oxide Nanostructure Makes Efficient Lithium‐Ion Batteries Possible

SnO₂‐based lithium‐ion batteries have low cost and high energy density, but their capacity fades rapidly during lithiation/delithiation due to phase aggregation and cracking. These problems can be mitigated by using highly conducting black SnO_2?x , which homogenizes the redox reactions and stabilizes fine, fracture‐resistant Sn precipitates in the Li₂O matrix. Such fine Sn precipitates and their ample contact with Li₂O proliferate the reversible Sn → Li _x Sn → Sn → SnO₂/SnO_2?x cycle during charging/discharging. SnO_2?x electrode has a reversible capacity of 1340 mAh g^?1 and retains 590 mAh g^?1 after 100 cycles. The addition of highly conductive, well‐dispersed reduced graphene oxide further stabilizes and improves its performance, allowing 950 mAh g^?1 remaining after 100 cycles at 0.2 A g^?1 with 700 mAh g^?1 at 2.0 A g^?1. Conductivity‐directed microstructure development may offer a new approach to form advanced electrodes.     

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

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

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.     

Surface Coating Constraint Induced Anisotropic Swelling of Silicon in Si–Void@SiO x Nanowire Anode for Lithium‐Ion Batteries

Here a simple and an environmentally friendly approach is developed for the fabrication of Si–void@SiO_x nanowires of a high‐capacity Li‐ion anode material. The outer surface of the robust SiO_x backbone and the inside void structure in Si–void@SiO_x nanowires appropriately suppress the volume expansion and lead to anisotropic swelling morphologies of Si nanowires during lithiation/delithiation, which is first demonstrated by the in situ lithiation process. Remarkably, the Si–void@SiO_x nanowire electrode exhibits excellent overall lithium‐storage performance, including high specific capacity, high rate property, and excellent cycling stability. A reversible capacity of 1981 mAh g^?1 is obtained in the fourth cycle, and the capacity is maintained at 2197 mAh g^?1 after 200 cycles at a current density of 0.5 C. The outstanding overall properties of the Si–void@SiO_x nanowire composite make it a promising anode material of lithium‐ion batteries for the power‐intensive energy storage applications.     

High‐Performance Li–SeSx All‐Solid‐State Lithium Batteries

All‐solid‐state Li–S batteries are promising candidates for next‐generation energy‐storage systems considering their high energy density and high safety. However, their development is hindered by the sluggish electrochemical kinetics and low S utilization due to high interfacial resistance and the electronic insulating nature of S. Herein, Se is introduced into S cathodes by forming SeS_x solid solutions to modify the electronic and ionic conductivities and ultimately enhance cathode utilization in all‐solid‐state lithium batteries (ASSLBs). Theoretical calculations confirm the redistribution of electron densities after introducing Se. The interfacial ionic conductivities of all achieved SeS_x–Li₃PS₄ (x = 3, 2, 1, and 0.33) composites are 10^?6 S cm^?1. Stable and highly reversible SeS_x cathodes for sulfide‐based ASSLBs can be developed. Surprisingly, the SeS₂/Li₁₀GeP₂S₁₂–Li₃PS₄/Li solid‐state cells exhibit excellent performance and deliver a high capacity over 1100 mAh g^?1 (98.5% of its theoretical capacity) at 50 mA g^?1 and remained highly stable for 100 cycles. Moreover, high loading cells can achieve high areal capacities up to 12.6 mAh cm^?2. This research deepens the understanding of Se–S solid solution chemistry in ASSLB systems and offers a new strategy to achieve high‐performance S‐based cathodes for application in ASSLBs.     

A Heterostructure Coupling of Bioinspired,Adhesive Polydopamine,and Porous Prussian Blue Nanocubics as Cathode for High‐Performance Sodium‐Ion Battery

Prussian blue (PB) and its analogues are recognized as promising cathodes for rechargeable batteries intended for application in low‐cost and large‐scale electric energy storage. With respect to PB cathodes, however, their intrinsic crystal regularity, vacancies, and coordinated water will lead to low specific capacity and poor rate performance, impeding their application. Herein, nanocubic porous Na_xFeFe(CN)₆ coated with polydopamine (PDA) as a coupling layer to improve its electrochemical performance is reported, inspired by the excellent adhesive property of PDA. As a cathode for sodium‐ion batteries, the Na_xFeFe(CN)₆ electrode coupled with PDA delivers a reversible capacity of 93.8 mA h g^?1 after 500 cycles at 0.2 A g^?1, and a discharge capacity of 72.6 mA h g^?1 at 5.0 A g^?1. The sodium storage mechanism of this Na_xFeFe(CN)₆ coupled with PDA is revealed via in situ Raman spectroscopy. The first‐principles computational results indicate that Fe^II sites in PB prefer to couple with the robust PDA layer to stabilize the PB structure. Moreover, the sodium‐ion migration in the PB structure is enhanced after coating with PDA, thus improving the sodium storage properties. Both experiments and computational simulations present guidelines for the rational design of nanomaterials as electrodes for energy storage devices.