Novel Designed MnS-MoS2 Heterostructure for Fast and Stable Li/Na Storage:Insights into the Advanced Mechanism Attributed to Phase Engineering

Combining 2D MoS₂ with other transition metal sulfide is a promising strategy to elevate its electrochemical performances. Herein, heterostructures constructed using MnS nanoparticles embedded in MoS₂ nanosheets (denoted as MnS-MoS₂) are designed and synthesized as anode materials for lithium/sodium-ion batteries via a facile one-step hydrothermal method. Phase transition and built-in electric field brought by the heterostructure enhance the Li/Na ion intercalation kinetics, elevate the charge transport, and accommodate the volume expansion. The sequential phase transitions from 2H to 3R of MoS₂ and α to γ of MnS are revealed for the first time. As a result, the MnS-MoS₂ electrode delivers outstanding specific capacity (1246.2 mAh g⁻¹ at 1 A g⁻¹), excellent rate, and stable long-term cycling stability (397.2 mAh g⁻¹ maintained after 3000 cycles at 20 A g⁻¹) in Li-ion half-cells. Superior cycling and rate performance are also presented in sodium half-cells and Li/Na full cells, demonstrating a promising practical application of the MnS-MoS₂ electrode. This work is anticipated to afford an in-depth comprehension of the heterostructure contribution in energy storage and illuminate a new perspective to construct binary transition metal sulfide anodes.     

A General Route for Encapsulating Monodispersed Transition Metal Phosphides into Carbon Multi-Chambers toward High-Efficient Lithium-Ion Storage with Underlying Mechanism Exploration

Transition metal phosphides (MP_x) with high theoretical capacities and low cost are regarded as the most promising anodes for lithium-ion batteries (LIBs), but the large volume variations and sluggish kinetics largely restrict their development. To solve the above challenges, herein a generic but effective method is proposed to encapsulate various monodispersed MP_x into flexible carbon multi-chambers (MP_x@NC, MNi, Fe, Co, and Cu, etc.) with pre-reserved voids, working as anodes for LIBs and markedly boosting the Li⁺ storage performance. Ni₂P@NC, one representative example of MP_x@NC anode, shows high reversible capacity (613 mAh g⁻¹, 200 cycles at 0.2 A g⁻¹), and superior cycle stability (475 mAh g⁻¹, 800 cycles at 2 A g⁻¹). Full cell coupled with LiFePO₄ displays a high reversible capacity (150.1 mAh g⁻¹ at 0.1 A g⁻¹) with stable cycling performance. In situ X-ray diffraction and transmission electron microscope techniques confirm the reversible conversion reaction mechanism and robust structural integrity, accounting for enhanced rate and cycling performance. Theoretical calculations reveal the synergistic effect between MP_x and carbon shells, which can significantly promote electron transfer and reduce diffusion energy barriers, paving ways to design high-energy-density materials for energy storage systems.     

Construction of VS2/VOx Heterostructure via Hydrolysis-Oxidation Coupling Reaction with Superior Sodium Storage Properties

Heterostructure engineering is one of the most promising modification strategies for reinforcing Na⁺ storage of transition metal sulfides. Herein, based on the spontaneous hydrolysis-oxidation coupling reaction of transition metal sulfides in aqueous media, a VO_x layer is induced and formed on the surface of VS₂, realizing tight combination of VS₂ and VO_x at the nanoscale and constructing homologous VS₂/VO_x heterostructure. Benefiting from the built-in electric field at the heterointerfaces, high chemical stability of VO_x, and high electrical conductivity of VS₂, the obtained VS₂/VO_x electrode exhibits superior cycling stability and rate properties. In particular, the VS₂/VO_x anode shows a high capacity of 878.2 mAh g⁻¹ after 200 cycles at 0.2 A g⁻¹. It also exhibits long cycling life (721.6 mAh g⁻¹ capacity retained after 1000 cycles at 2 A g⁻¹) and ultrahigh rate property (up to 654.8 mAh g⁻¹ at 10 A g⁻¹). Density functional theory calculations show that the formation of heterostructures reduces the activation energy for Na⁺ migration and increases the electrical conductivity of the material, which accelerates the ion/electron transfer and improves the reaction kinetics of the VS₂/VO_x electrode.     

Low Volume-Expansion,Insertion-Type Layered Silicate Hierarchical Structure For Superior Storage Of Li,Na, K

A hierarchical structure is successfully synthesized by coating polypyrrole (PPy) on the surface of carbon/saponite superlattice (denoted as PPy@C/SAP), and applied as low volume-expansion insertion-type anode for Li, Na, K storage.The synergistic effect of metal Ni, Fe doping, carbon/silicate superlattice, abundant oxygen vacancies and PPy coating leads to a good electronic conductivity and large current discharging capability. As a Si-based material, PPy@C/SAP has excellent storage capability for Li (659 mAh g⁻¹ after 1000 cycles at 2 A g⁻¹ and 550 mAh g⁻¹ after 1000 cycles at 5 A g⁻¹), Na (maximum specific capacity of 533 and 327 mAh g⁻¹ after 50 cycles) as well as K (236 mAh g⁻¹ after 100 cycles). XPS, XANES, XRD, FTIR, HRTEM, SEM are used to detect the hybrid mechanism (bulk insertion and surface conversion) with a volume expansion as low as 9%. Insertion reaction driven by valence state change of Ni, Fe, Si (Ni⁰⇔Ni²⁺, Fe0⇔Fe³⁺, Si²⁺⇔Si⁴⁺) in laminates and conversion reactions between LiOH/Li₂CO₃ and LiH/Li₂C₂ catalyzed by Ni° contribute to the high performance. In the whole electrochemical process, layered structure is retained while the conversion reactions of LiOH (prodeced by laminates dehydroxylation) and Li₂CO₃ (electrolyte decomposition) cause the dynamic evolution of solid ectrolyte interphase. This study develops a promising Si-based anode material for lithium ion batteries, sodium ion batteries and potassium ion batteries, which is significant for designing long cycle life rechargeable batteries.     

Optimized Ti?O Subcompounds and Elastic Expanded MXene Interlayers Boost Quick Sodium Storage Performance

To develop quick-charge sodium-ion battery, it is significant to optimize insertion-type anode to afford fast Na⁺ diffusion rate and excellent electron conductivity. First-principles calculations reveal the Ti O subcompound superiority for Na⁺ diffusion following Ti(II) O > Ti(III) O > Ti(IV) O. Hence, in situ growth of amorphous Ti O subcompounds with rich oxygen defects based on Ti₃C₂T_x-MXene is developed. Meanwhile, the composite presents expanded MXene interlayer spacing and much enhanced conductivity. The synergistic effect of enhanced electron/ion conduction gives a high capacity of 107 mAh g⁻¹ at 50 A g⁻¹, which gives 50% and 150% increasements compared with one counterpart without valence adjustment and another one without MXene expansion. It only needs 20 s (at 30 A g⁻¹) to complete the discharge/charge process and obtains a capacity of 144.5 mAh g⁻¹, which also shows a long-term cycling stability at quick-charge mode (121 mAh g⁻¹ after 10000 cycles at 10 A g⁻¹). The enhanced performance comes from fast electron transfer among Ti O subcompounds contributed by rich-defect amorphous TiO_2–x, and a reversible change of elastic MXene with interlayer spacing between 1.4 and 1.9 nm during Na⁺ insertion/extraction process. This study provides a feasible route to boost the kinetics and develop quick-charge sodium-ion battery.     

On the Practical Applicability of Rambutan-like SiOC Anode with Enhanced Reaction Kinetics for Lithium-Ion Storage

Silicon oxycarbide (SiOC) possesses great potential in lithium-ion batteries owing to its tunable chemical component, high reversible capacity, and small volume expansion. However, its commercial application is restricted due to its poor electrical conductivity. Herein, rambutan-like vertical graphene coated hollow porous SiOC (Hp-SiOC@VG) spherical particles with an average diameter of 302 nm are fabricated via a hydrothermal treatment combined CH₄ pyrolysis strategy for the first time. As-prepared Hp-SiOC@VG exhibits a large reversible capacity of 729 mAh g⁻¹ at 0.1 A g⁻¹, remarkable cycling stability of 98% capacity retention rate after 600 cycles at 1.0 A g⁻¹ and high rate capability of 289 mAh g⁻¹ at 5.0 A g⁻¹ owing to the unique structure of the particles and the electrical conductivity of the vertical graphene. Density functional theory calculations reveal that the higher contents of SiO₃C and SiO₂C₂ structural units in the SiOC are beneficial to enhance the Li⁺ storage capacity. Additionally, the full-cell assembled with Hp-SiOC@VG and LiFePO₄ delivers up to 74% capacity retention rate after 100 cycles at 0.2 A g⁻¹. This work reports a new way for the facile preparation of template-free hollow porous materials and expands the application prospects of SiOC-based anode for lithium-ion batteries.     

Unveiling the Effects of Cr Single Atoms with Controllable Configurations on Solid Electrolyte Interphase and Storage Mechanism of Sodium Ions

Single atomic metal (SAM) doping is reported as an effective strategy to promote the electrochemical property of carbon-based anode materials for high-power sodium-ion batteries (SIBs). However, the effects of SAM with different configurations on solid electrolyte interphase (SEI) and energy storage mechanism of Na⁺ are not revealed. Herein, Cr single atoms (CrSAs) are reported with controllable configurations (Cr–N₄ or Cr–N₂) implanted on the N, P co-doped carbon (NPC) anode materials (denoted as CrN₄SAs/NPC or CrN₂SAs/NPC). The CrN₄SAs/NPC anode displays a high specific capacity (318.2 mAh g⁻¹ at 0.05 A g⁻¹) and outstanding rate performance (145.1 mAh g⁻¹ at 5 A g⁻¹), better than those of CrN₂SAs/NPC and NPC. The superiority is originated from the difference of SEI and the energy storage mechanism of sodium ions during electrochemical process, which are unveiled through ex situ characterization and theoretical calculation. The full cell assembled with CrN₄SAs/NPC anode and Na₃V₂(PO₄)₂F₃@C cathode displays a high energy density at a high power density.     

Si/SiO2@Graphene Superstructures for High-Performance Lithium-Ion Batteries

The superstructure composed of various functional building units is promising nanostructure for lithium-ion batteries (LIBs) anodes with extreme volume change and structure instability, such as silicon-based materials. Here, a top-down route to fabricate Si/SiO₂@graphene superstructure is demonstrated through reducing silicalite-1 with magnesium reduction and depositing carbon layers. The successful formation of superstructure lies on the strong 3D network formed by the bridged-SiO₂ matrix coated around silicon nanoparticles. Furthermore, the mesoporous Si/SiO₂ with amorphous bridged SiO₂ facilitates the deposition of graphene layers, resulting in excellent structural stability and high ion/electron transport rate. The optimized Si/SiO₂@graphene superstructure anode delivers an outstanding cycling life for ≈1180 mAh g⁻¹ at 2 A g⁻¹ over 500 cycles, excellent rate capability for ≈908 mAh g⁻¹ at 12 A g⁻¹, great areal capacity for ≈7 mAh cm⁻² at 0.5 mA cm⁻², and extraordinary mechanical stability. A full cell test using LiFePO₄ as the cathode manifests a high capacity of 134 mAh g⁻¹ after 290 loops. More notably, a series of technologies disclose that the Si/SiO₂@graphene superstructure electrode can effectively maintain the film between electrode and electrolyte in LIBs. This design of Si/SiO₂@graphene superstructure elucidates a promising potential for commercial application in high-performance LIBs.     

Designing and Understanding the Superior Potassium Storage Performance of Nitrogen/Phosphorus Co-Doped Hollow Porous Bowl-Like Carbon Anodes

Potassium-ion batteries (PIBs) are promising alternatives to lithium-ion batteries because of the advantage of abundant, low-cost potassium resources. However, PIBs are facing a pivotal challenge to develop suitable electrode materials for efficient insertion/extraction of large-radius potassium ions (K⁺). Here, a viable anode material composed of uniform, hollow porous bowl-like hard carbon dual doped with nitrogen (N) and phosphorus (P) (denoted as N/P-HPCB) is developed for high-performance PIBs. With prominent merits in structure, the as-fabricated N/P-HPCB electrode manifests extraordinary potassium storage performance in terms of high reversible capacity (458.3 mAh g⁻¹ after 100 cycles at 0.1 A g⁻¹), superior rate performance (213.6 mAh g⁻¹ at 4 A g⁻¹), and long-term cyclability (205.2 mAh g⁻¹ after 1000 cycles at 2 A g⁻¹). Density-functional theory calculations reveal the merits of N/P dual doping in favor of facilitating the adsorption/diffusion of K⁺ and enhancing the electronic conductivity, guaranteeing improved capacity, and rate capability. Moreover, in situ transmission electron microscopy in conjunction with ex situ microscopy and Raman spectroscopy confirms the exceptional cycling stability originating from the excellent phase reversibility and robust structure integrity of N/P-HPCB electrode during cycling. Overall, the findings shed light on the development of high-performance, durable carbon anodes for advanced PIBs.     

Metal-Electronegativity-Induced,Synchronously Formed Hetero- and Vacancy-Structures of Selenide Molybdenum for Non-Aqueous Sodium-Based Dual-Ion Storage

Sodium-based dual-ion batteries (SDIBs) have attracted increasing research interests in energy storage systems because of their advantages of high operating voltage and low cost. However, exploring desirable anode materials with high capacity and stable structures remains a great challenge. Here, an elaborate design is reported, starting from well-organized MoSe₂ nanorods and introducing metal-organic frameworks, which simultaneously forms a bimetallic selenide/carbon composite with coaxial structure via electronegativity induction. By rationally adjusting the vacancy concentration and combining heterostructure engineering, the optimized MoSe_2-x/ZnSe@C as anode material for Na-ion batteries achieves rapid electrochemical kinetics and satisfactory reversible capacities. The systematic electrochemical kinetic analyses combined with theoretical calculations further unveil the synergistic effect of Se-vacancies and heterostructure for the enhanced sodium storage, which not only induces more reversible Na⁺ storage sites but also improves the pseudocapacitance and reduce charge transfer resistance, thereby providing a great contribution to accelerating reaction kinetics. Furthermore, the as-constructed SDIB full cell based on the MoSe_2-x/ZnSe@C anode and the expanded graphite cathode demonstrates impressively excellent rate performance (131 mAh g⁻¹ at 4.0 A g⁻¹) and ultralong cycling life over 1000 cycles (100 mAh g⁻¹ at 1.0 A g⁻¹), demonstrating its practical applicability in a wide range of sodium-based energy storage devices.     

Inorganic Filler Enhanced Formation of Stable Inorganic-Rich Solid Electrolyte Interphase for High Performance Lithium Metal Batteries

Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, a composite gel polymer electrolyte (GPE), formed through in situ polymerization of pentaerythritol tetraacrylate with fumed silica fillers, is developed to achieve high performance lithium metal batteries (LMBs). As evidenced theoretically and experimentally, the presence of SiO₂ not only accelerates Li⁺ transport but also regulates Li⁺ solvation sheath structures, thus facilitating fast kinetics and formation of stable LiF-rich interphase and achieving uniform Li depositions to suppress Li dendrite growth. The composite GPE-based Li||Cu half-cells and Li||Li symmetrical cells display high Coulombic efficiency (CE) of 90.3% after 450 cycles and maintain stability over 960 h at 3 mA cm⁻² and 3 mAh cm⁻², respectively. In addition, Li||LiFePO₄ full-cells with a LM anode of limited Li supply of 4 mAh cm⁻² achieve capacity retention of 68.5% after 700 cycles at 0.5 C (1 C = 170 mA g⁻¹). Especially, when further applied in anode-free LMBs, the carbon cloth||LiFePO₄ full-cell exhibits excellent cycling stability with an average CE of 99.94% and capacity retention of 90.3% at the 160th cycle at 0.5 C.     

In Situ Synthesis of Graphene-Coated Silicon Monoxide Anodes from Coal-Derived Humic Acid for High-Performance Lithium-Ion Batteries

Silicon monoxide (SiO) is attaining extensive interest amongst silicon-based materials due to its high capacity and long cycle life; however, its low intrinsic electrical conductivity and poor coulombic efficiency strictly limit its commercial applications. Here low-cost coal-derived humic acid is used as a feedstock to synthesize in situ graphene-coated disproportionated SiO (D-SiO@G) anode with a facile method. HR-TEM and XRD confirm the well-coated graphene layers on a SiO surface. Scanning transmission X-ray microscopy and X-ray absorption near-edge structure spectra analysis indicate that the graphene coating effectively hinders the side-reactions between the electrolyte and SiO particles. As a result, the D-SiO@G anode presents an initial discharge capacity of 1937.6 mAh g⁻¹ at 0.1 A g⁻¹ and an initial coulombic efficiency of 78.2%. High reversible capacity (1023 mAh g⁻¹ at 2.0 A g⁻¹), excellent cycling performance (72.4% capacity retention after 500 cycles at 2.0 A g⁻¹), and rate capability (774 mAh g⁻¹ at 5 A g⁻¹) results are substantial. Full coin cells assembled with LiFePO₄ electrodes and D-SiO@G electrodes display impressive rate performance. These results indicate promising potential for practical use in high-performance lithium-ion batteries.     

Fe2VO4 Nanoparticles Anchored on Ordered Mesoporous Carbon with Pseudocapacitive Behaviors for Efficient Sodium Storage

Iron vanadates are attractive anode materials for sodium-ion batteries (SIBs) because of their abundant resource reserves and high capacities. However, their practical application is restricted by the aggregation of materials, sluggish reaction kinetics, and inferior reversibility. Herein, Fe₂VO₄ nanoparticles are anchored on the ordered mesoporous carbon (CMK-3) nanorods to assemble 3D Fe₂VO₄@CMK-3 composites, by solvothermal treatment and subsequent calcination. The resulting composites provide abundant active sites, high electrical conductivity, and excellent structural integrity. The pseudocapacitive-controlled behavior is the dominating sodium storage mechanism, which facilitates a fast charge/discharge process. The Fe₂VO₄@CMK-3 composites exhibit stable sodium-ion storage (219 mAh g⁻¹ under 100 mA g⁻¹ after 300 cycles), good rate performance (144 mAh g⁻¹ at 3.2 A g⁻¹), and excellent cycling performance (132 mAh g⁻¹ at 1 A g⁻¹ with capacity retention of 96.4% after 800 cycles). When coupled with a NaNi_1/3Fe_1/3Mn_1/3O₂ cathode, the sodium-ion full cell displays excellent cycling stability (94 mAh g⁻¹ after 500 cycles at 500 mA g⁻¹). These findings point to the potential of Fe₂VO₄@CMK-3 for application as anodes in SIBs.     

Engineering Se/N Co-Doped Hard CNTs with Localized Electron Configuration for Superior Potassium Storage

The earth-abundant hard carbons have drawn great concentration as potassium-ion batteries (KIBs) anode materials because of their richer K-storage sites and wider interlayer distance versus graphite, but suffer from a low electrochemical reversibility. Herein, the novel Se/N co-doped hard-carbon nanotubes (h-CNTs) with localized electron configuration are demonstrated by creating unique N Se C covalent bonds stemmed from the precise doping of Se atoms into carbon edges and the subsequent bonding with pyrrole-N. The strong electron-donating ability of Se atoms on d-orbital provides abundant free electrons to effectively relieve charge polarization of pyrrole-N-C bonds, which contributes to balance the K-ion adsorption/desorption, therefore greatly boosting reversible K-ion storage capacity. After filtering into self-standing anodes with weights of 1.5–12.4 mg cm⁻², all of them deliver a high reversible gravimetric capacity of 341 ± 4 mAh g⁻¹ at 0.2 A g⁻¹ and a linear increasing areal capacity to 4.06 mAh cm⁻². The self-standing anode can still maintain 209 mAh g⁻¹ at 8.0 A g⁻¹ (93.3% retention) for a long period of 2000 cycles with a constant Se/N content.     

An In Situ Electrochemical Amorphization Electrode Enables High-Power High-Cryogenic Capacity Aqueous Zinc-Ion Batteries

Quick-charge technology is of great significance for the development of aqueous zinc-ion batteries. In this study, an unreported in situ electrochemical amorphization mechanism is highlighted to unlock the ultrafast-kinetics electrode. Multiple characterizations, density functional theory calculation, and molecular dynamic simulation are applied to uncover the storage mechanism of electrodes, as well as the evolution of structure, and reaction kinetics after reconstruction. As revealed, the long-range ordered ZnV₂O₄ crystalline can be reconstructed to a short-range ordered Zn_0.44V₂O₄ electrode, which exhibits significantly improved active sites, shortened diffusion path, and enhanced zinc ions capture ability. Notably, by pairing with the modified Zn anode, it can display ultrahigh rate capability (212 mAh g⁻¹ at 50 A g⁻¹) with a maximum power density of 23.2 kW kg⁻¹, as well as good cycle performance (217.2 mAh g⁻¹ after 3000 cycles at 20 A g⁻¹). Unexpectedly, such reconstructed amorphous electrodes can also retain superior storage capability even at cryogenic conditions. A high specific capacity of 251 mAh g⁻¹ can be delivered at −25°C and 1 A g⁻¹, as well as an 84.3% capacity retention after 500 cycles. This brand-new in-situ electrochemical amorphization mechanism is expected to provide new insight into understanding the high-performance aqueous zinc-ion batteries.     

Controlled Nitrogen Doping in Crumpled Graphene for Improved Alkali Metal-Ion Storage under Low-Temperature Conditions

The significant performance decay in conventional graphite anodes under low-temperature conditions is attributed to the slow diffusion of alkali metal ions, requiring new strategies to enhance the charge storage kinetics at low temperatures. Here, nitrogen (N)-doped defective crumpled graphene (NCG) is employed as a promising anode to enable stable low-temperature operation of alkali metal-ion storage by exploiting the surface-controlled charge storage mechanisms. At a low temperature of −40 °C, the NCG anodes maintain high capacities of ≈172 mAh g⁻¹ for lithium (Li)-ion, ≈107 mAh g⁻¹ for sodium (Na)-ion, and ≈118 mAh g⁻¹ for potassium (K)-ion at 0.01 A g⁻¹ with outstanding rate-capability and cycling stability. A combination of density functional theory (DFT) and electrochemical analysis further reveals the role of the N-functional groups and defect sites in improving the utilization of the surface-controlled charge storage mechanisms. In addition, the full cell with the NCG anode and a LiFePO₄ cathode shows a high capacity of ≈73 mAh g⁻¹ at 0.5 °C even at −40 °C. The results highlight the importance of utilizing the surface-controlled charge storage mechanisms with controlled defect structures and functional groups on the carbon surface to improve the charge storage performance of alkali metal-ion under low-temperature conditions.     

Effective Coupling of Amorphous Selenium Phosphide with High-Conductivity Graphene as Resilient High-Capacity Anode for Sodium-Ion Batteries

It is of great importance to develop high-capacity electrodes for sodium-ion batteries (SIBs) using low-cost and abundant materials, so as to deliver a sustainable technology as alternative to the established lithium-ion batteries (LIBs). Here, a facile ball milling process to fabricate high-capacity SIB anode is devised, with large amount of amorphous SeP being loaded in a well-connected framework of high-conductivity crystalline graphene (HCG). The HCG substrate enables fast transportation of Na ions and electrons, while accommodating huge volumetric changes of the active anode matter of SeP. The strong glass forming ability of NaxSeP helps prevent crystallization of all stable compounds but ultrafine nanocrystals of Na2Se and Na3P. Thus, the optimized anode delivers excellent rate performance with high specific capacities being achieved (855 mAh g⁻¹ at 0.2 A g⁻¹ and 345 mAh g⁻¹ at 5 A g⁻¹). More importantly, remarkable cycling stability is realized to maintain a steady capacity of 732 mAh g⁻¹ over 500 cycles, when the SeP in the SeP@HCG still remains 86% of its theoretical capacity. A high areal capacity of 2.77 mAh is achieved at a very high loading of 4.1 mg cm⁻² anode composite.     

Laser-Induced Graphene Assisting Self-Conversion Reaction for Sulfur-Free Aqueous Cu-S Battery

In aqueous/nonaqueous metal-sulfur batteries, sulfur-based redox couple exhibits significant challenges mainly due to its low electrochemical kinetics, potential shuttle effect, and large volume change. Although massive researches have been conducted to optimize or replace metal anode and cathode composite, major challenges caused by the dependency on sulfur-based redox couple still remain. In this study, a novel redox couple of CuS/Cu₂S, which provides the same theoretical capacity (based on conventional S/S²⁻ redox couple) by changing the valence of ion charge carrier, is proposed. For achieving high reversibility, commercially viable laser-induced graphene (LIG) is fabricated and used for the first time in aqueous metal-sulfur batteries. By virtue of the synergism between novel redox couple and LIG, aqueous CuS/Cu₂S battery delivers a highly reversible capacity of 1654.9 mAh g⁻¹ in the initial cycle and retains 91.2% with 1509.5 mAh g⁻¹ after 328 cycles. When being cycled at 2.8 A g⁻¹, its reversible capacity still retains 92.1% after 410 cycles. This study provides a new choice by using a sulfur-free redox couple from screening thermodynamic parameters and analyzes the functional mechanism of LIG by density functional theory, aiming to innovate the energy storage mechanism of aqueous metal-sulfur batteries.     

Mg-Doped Na4Fe3(PO4)2(P2O7)/C Composite with Enhanced Intercalation Pseudocapacitance for Ultra-Stable and High-Rate Sodium-Ion Storage

Na₄Fe₃(PO₄)₂(P₂O₇) (NFPP) is considered as a promising cathode material for sodium-ion batteries (SIBs) due to its low cost, non-toxicity, and high structural stability, but its electrochemical performance is limited by the poor electronic conductivity. In this study, Mg-doped NFPP/C composites are presented as cathode materials for SIBs. Benefiting from the enhanced electrochemical kinetics and intercalation pseudocapacitance resulted from the Mg doping, the optimal Mg-doped NFPP/C composite (NFPP-Mg5%) delivers high rate performance (capacity of ≈40 mAh g⁻¹ at 20 A g⁻¹) and ultra-long cycling life (14 000 cycles at 5 A g⁻¹ with capacity retention of 80.8%). Moreover, the in situ X-ray diffraction and other characterizations reveal that the sodium storage process of NFPP-Mg5% is dominated by the intercalation pseudocapacitive mechanism. In addition, the full SIB based on NFPP-Mg5% cathode and hard carbon anode exhibits the discharge capacity of ≈50 mAh g⁻¹ after 200 cycles at 500 mA g⁻¹. This study demonstrates the feasibility of improving the electrochemical performance of NFPP by doping strategy and presents a low-cost, ultra-stable, and high-rate cathode material for SIBs.     

A Self-Growth Strategy for Simultaneous Modulation of Interlayer Distance and Lyophilicity of Graphene Layers toward Ultrahigh Potassium Storage Performance

Herein, a simple but effective self-growth strategy to simultaneously modulate the interlayer distance and lyophilicity of graphene layers, which results in ultrahigh potassium-storage performances for carbon materials, is reported. This strategy involves the uniform adsorption of individual metal ions on the oxygen-containing groups on graphene oxide via electrostatic/coordination interactions and in situ self-conversion reaction between the metal ions and the oxygen-containing groups to form lyophilic ultrasmall metal oxide nanoparticles modified/intercalated graphene skeleton (OM-G) with precisely regulated interlayer distance. The synergistic effect of expanded interlayer distance and enhanced lyophilicity is revealed for the first time to significantly reduce the ion diffusion barrier and enhance ion transport kinetics by experimental and theoretical analysis. As a result, such unique OM-G monolith as free-standing anode for potassium-ion battery (PIB) delivered an ultrahigh reversible capability of 496.4 mAh g⁻¹ at 0.1 A g⁻¹, excellent rate capability (306.6 mAh g⁻¹ at 10 A g⁻¹), and remarkable long-term cycling stability (96.3% capacity retention over 2000 cycles at 1 A g⁻¹), which are not only much better than those of previous graphene/carbon materials but also among the best performances for all PIB anodes ever reported. This study provides new fundamental insights for boosting the electrochemical properties of electrode materials.