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Aluminum-organic batteries (AIBs) have gained significant popularity for large-scale energy storage due to their abundance of aluminum reserves, cost-effectiveness, and environmental friendliness. However, the current aluminum-organic batteries primarily relied on ionic liquid electrolytes suffer from slow reaction kinetics and limited cycle life. Herein, we report a novel and efficient aluminum-organic battery that addresses these limitations by utilizing a molten salt electrolyte and designing a strongly interacting organic cathode. By enhancing π-π stacking interactions, we induced a transition in commercial PTCDA (Perylene-3,4,9,10-tetracarboxylic dianhydride) molecules from the β-phase to the highly interactive α-phase, known as PA450. This transformation not only stabilizes the structure of the PA450 electrode, preventing dissolution in the molten salt electrolyte, but also significantly improves electron conductivity. The Al||PA450 molten salt battery demonstrates exceptional electrochemical performance, exhibiting a high reversible capacity of 135 mAh g–1 and outstanding cyclability for up to 2000 cycles at 10 A g−1. Additionally, the structural rearrangement and ion transport properties induced by the co-intercalation of Al3+ and AlCl 2 + were studied are investigated. This work provides deep insights into the unique characteristics of organic materials for ultrafast energy storage in molten salt electrolytes. [Display omitted] • Introduced an aluminum-organic battery with robust π-π interactions organic cathodes and advanced molten salt electrolytes. • Battery offers excellent rate performance and durability (110 mAh g−1 at 10A g−1, over 2000 cycles). • Verified Al storage mechanism via theoretical analysis and in-situ characterization, showing AlCl2+ and Al3+ co-insertion. [ABSTRACT FROM AUTHOR]

The cobalt-free high - nickel layered oxide possesses high capacity and controllable cost, positioning it as a prospective option for cathode materials in the future lithium-ion batteries (LIBs). However, the charge compensation effect and high nickel content usually cause serious cation mixing, resulting in poor capacity stability, and hindering its practical application. Here, three types of LiNi 0.9 Mn 0.1 O 2 microspheres with varying levels of cation mixing are constructed by simply adjusting the calcination temperatures, and the impacts of cation mixing on the electrochemical performance in LIBs are systematically investigated. By using XRD and cross-section STEM to characterize the levels of cation mixing, the resulting LiNi 0.9 Mn 0.1 O 2 after treated at 780 °C (denoted as NM91–780) shows a lower degree of cation mixing compared to other samples (NM91–720 and NM91–840). As a proof-of-concept application in LIBs, the NM91–780 exhibits remarkable cycling stability with 92.4% capacity retention after 100 cycles, along with excellent rate capability of 132.5 mAh g−1 at 10 C. In situ XRD analysis shows that the low cation mixing of NM91–780 inhibits harmful volumetric strain during the electrochemical process, providing structural and chemical stability for its long-term cycling. This investigation contributes to the advancement of commercializing cobalt-free high-nickel layered oxide LiNi 0.9 Mn 0.1 O 2 for use in LIBs. [Display omitted] • The relationship between temperature and cation mixing was investigated. • lower cation mixing promoted the consistency of the internal structure. • The electrochemical performance of NM91 was enhanced by reducing cation mixing. • The structure change caused by cation mixing in electrochemical process was explained. [ABSTRACT FROM AUTHOR]

Realizing stable cycling performance with high areal capacity is a great challenge for metal-ion battery anodes. Achieveing high areal capacity generally requires the electrode in a high active loading with increased electrode thickness, which is not beneficial to the cycling stability. In this work, novel nanosheet-assembled compact CaV 4 O 9 microflowers are firstly synthesized through a facile method, which exhibit both high areal capacity and stable cycling performance at high mass loadings. The compact microflower structure leads to an increased tap density of the electrode materials, benefiting to reduce the anode thickness at high mass loadings. Meanwhile, the assembled nanosheets maintain the nano-effects of the active materials for favorable electrochemical reactions. These merits together with the intrinsic superior electrochemical properties of CaV 4 O 9 , result in the outstanding electrochemical performance. When used as Li-ion battery anodes, a high areal capcity of ~2.5 mAh cm −2 at a high mass loading of 4.4 mg cm −2 is obtained, and a stable cycling over 400 cycles with the areal capacity over 1.5 mAh cm −2 is demonstrated. Besides, the superior electrochemical performance at high mass loadings is also observed for Na storage. These achievements may pave the way for constructing applicable high-capacity and stable anode materials in metal-ion batteries. [ABSTRACT FROM AUTHOR]

The delivery of cathodes with both high capacity and excellent cycling stability is a great challenge in the development of sodium-ion batteries (SIBs) for energy storage systems. Here, we exploited a novel potassium-ion-intercalated layered iron/manganese-based material (K 0.7 Fe 0.5 Mn 0.5 O 2 ). On the basis of advanced in situ and ex situ X-ray diffraction analysis, we confirm that K 0.7 Fe 0.5 Mn 0.5 O 2 can provide highly reversible layer spacing variations and an ultra-stable skeleton structure during the sodiation/desodiation processes. As a result, K 0.7 Fe 0.5 Mn 0.5 O 2 displays superior performance, with both high capacity and superior cycling stability, as a cathode for SIBs. A high discharge capacity of 181 mAh g −1 is achieved at 100 mA g −1 . Remarkably, even when cycled at high rate of 1000 mA g −1 , 85% of the initial discharge capacity is maintained after 1000 cycles. These results indicate that K 0.7 Fe 0.5 Mn 0.5 O 2 is a promising candidate for high-capacity and long-life SIBs. Additionally, this work will provide a unique insight into the development of high-performance cathodes for energy storages. [ABSTRACT FROM AUTHOR]

T-Nb 2 O 5 as a promising candidate anode has attracted great interest for ultrafast lithium-ion batteries (LIBs) due to its good ion conductivity and safety. However, the relatively inferior electric conductivity and low capacity greatly limit its commercial application. Herein, a trace Co doping strategy is reported to enhance the electric conductivity and redox chemistry of T-Nb 2 O 5. The original Nb sites are partially replaced by Co, which endows Co-Nb 2 O 5 with high electronic conductivity without affecting the crystalline host structure, meanwhile induces multielectron redoxes of Nb5+/Nb4+ and Nb4+/Nb3+ during lithium-ion insertion process. As a LIB anode, the resulting Co-Nb 2 O 5 nanoparticles display a high discharge capacity (256.1 mAh g−1 at 0.1 A g−1), superior rate capability (141.7 mAh g−1 at 5 A g−1) and good cycling stability (179.7 mAh g−1 at 1 A g−1 after 500 cycles). The ultrafast lithium storage and high-capacity electrochemical performance of Co-Nb 2 O 5 owing to its high electric conductivity and multielectron redox upon lithiation/delithiation. The selective transition metal doping strategy provides a new direction for the development of new insertion-type oxide anodes towards fast charging and high-capacity LIBs. [Display omitted] • For Co-Nb 2 O 5 nanoparticles, trace Co transition metal dopants partial occupy the Nb sites with low coordination. • Co-Nb 2 O 5 delivers high electronic conductivity , meanwhile maintains crystalline host structure, and exhibits ultrafast lithium storage. • Trace Co can induce multielectron redoxes of Nb5+/Nb4+ and Nb4+/Nb3+, resulting in higher specific capacity. • The introduction of metal dopants into insertion-type materials offers a new idea for fast-charging and high-capacity LIBs. [ABSTRACT FROM AUTHOR]

NASICON structured NaTi 2 (PO 4 ) 3 with stable and open framework has become a promising electrode material for sodium-ion batteries. However, the intrinsic low electronic conductivity of NaTi 2 (PO 4 ) 3 leads to inferior rate capability and poor active material utilization. Herein, we first report the synthesis of carbon-coated hierarchical NaTi 2 (PO 4 ) 3 mesoporous microflowers (NTP/C-F), via a facile and controllable solvothermal method and subsequent annealing treatment. The unique structural features endow the NTP/C-F with excellent structural stability, enhanced charge transfer kinetics, and suppressed polarization. This architecture exhibits superior sodium storage performance: high initial capacity (125 mA h g −1 at 1 C), outstanding rate capability (95 mA h g −1 at 100 C), and ultra-long cycling stability (capacity retention of 77.3% after 10,000 cycles at 20 C). Time-resolved in-situ X-ray diffraction study reveals a typical two-phase electrochemical reaction with reversible structure change. This work suggests the integration of hierarchical structure and carbon coating provides a promising approach for boosting the electrochemical performances of battery electrode materials. [ABSTRACT FROM AUTHOR]

Three-dimensional (3D) hierarchical heterostructures have been widely studied for energy storage because of their amazing synergistic effect. However, a detailed characterization how the branched structure affects the backbone structure during electrochemical cycling, and the specific relationship between the backbone and the branched heterogeneous structure (namely synergistic effect) have been rarely revealed. In addition, the controllable synthesis of this system still remains a great challenge. Herein, we developed a one-step gradient hydrothermal method to obtain a series of 3D hierarchical heterogeneous nanostructures, including V 2 O 5 /NaV 6 O 15 , V 2 O 5 /ZnV 2 O 6 and V 2 O 5 /CoV 2 O 6 , through controlling the sequence of nucleation and growth processes of different structural units in the same precursor. On the basis of time-resolved in situ X-ray diffraction (XRD) characterizations, we clearly elucidated the synergistic effect between the branched and backbone structure. During the synergistic effect, the branched NaV 6 O 15 helps to reduce the potential barrier during lithium-ion insertion/extraction, buffers the impact of crystal-system transformations during the charge/discharge process; the backbone V 2 O 5 is beneficial to increase the charge/discharge capacity, inhibits the self-aggregation of branched NaV 6 O 15 and maintains the stability of 3D structure. Consequently, 3D V 2 O 5 /NaV 6 O 15 hierarchical heterogeneous microspheres exhibit the best electrochemical performance than pure V 2 O 5 and V 2 O 5 /NaV 6 O 15 physical mixture in lithium-ion batteries (LIBs). When tested at a high rate of 5 A g −1 , 92% of the initial capacity can be maintained after 1000 cycles. We believe this method will be in favor of the construction of 3D hierarchical heterostructures and this specific synergistic effect investigated by in situ XRD will be significant for the design of better electrodes. [ABSTRACT FROM AUTHOR]

As promising electrode materials for aluminum-ion batteries (AIBs), transition metal sulfides have attracted significant attention. However, the relative low energy density and poor rate property restrict their further applications. Herein, channels-rich VS 4 nanowire clusters were synthesized via an amine ions-assisted method. When assessed as a cathode for rechargeable AIB, the VS 4 nanowire clusters exhibit superior electrochemical performances, specifically, outstanding rate property (103.32 mAh g-1 at 800 mA g-1), good cycling stability and a high reversible capacity of 252.51 mAh g-1 (at 100 mA g-1). Moreover, ex-situ X-ray diffraction (XRD) and in-situ Raman techniques reveal that the as-prepared VS 4 nanowire clusters have stable channels-rich structures, which is favorable for the mass transfer in electrochemical reaction. A mechanism of intercalation is proposed for the electrochemical process. This work takes a step toward the development of high-performance electrode materials for AIBs and provides new insights into the chemistry of AIBs for electrochemical energy storage. Three-dimensional channels-rich VS 4 nanowire clusters were assessed as a rechargeable aluminum-ion batteries (AIBs) cathode for the first time. The VS 4 nanowire clusters exhibit superior electrochemical performance for Al3+ storage among existing cathode materials, exhibiting a high reversible capacity of 252.51 mAh g-1 (at 100 mA g-1), outstanding rate property (103.32 mAh g-1 at 800 mA g-1) and good cycling stability. Through ex-situ X-ray diffraction and in-situ Raman techniques, the insertion/extraction mechanism of VS 4 in AIBs are elucidated. Image 1 • Three-dimensional channels-rich VS 4 nanowire clusters were assessed as a rechargeable aluminum-ion batteries (AIBs) cathode for the first time. • The VS 4 nanowire clusters exhibit superior electrochemical performance for Al3+ storage among existing cathode materials, exhibiting a high reversible capacity of 252.51 mAh g-1 (at 100 mA g-1), outstanding rate property (103.32 mAh g-1 at 800 mA g-1) and good cycling stability. • Through ex-situ X-ray diffraction and in-situ Raman techniques, the insertion/extraction mechanism of VS 4 in AIBs are elucidated. [ABSTRACT FROM AUTHOR]

The intrinsically limited rate capability of batteries by the diffusion-controlled ionic storage mechanism is still existing, and long-service batteries are always required for low-cost grid-scale energy storage. Herein, we design and construct a series of Ni x Zn y HCF (x + y = 3, x = 1, 1.5 or 2) bimetallic Prussian blue analogues as cathode materials for aqueous potassium-ion batteries. On the basis of electrochemical and structural analysis, a synergistic effect between stable Ni2+ and high-voltage Zn2+ in Ni 2 Zn 1 HCF is demonstrated, which simultaneously promises ultrafast near-pseudocapacitance intercalation and super-stable potassium storage. As presented, Ni 2 Zn 1 HCF cathode shows an extraordinary high-rate capability of 1000C with a capacity retention of 66% and a high capacity recovery of 95.3%, which derives from the large sufeace area and fast near-pseudocapacitive intercalation mechanism. When cycled at 1000C for 80,000 times, a negligible capacity decay of 0.000385% per cycle further proves this cathode to be high-rate and ultra-stable. In addition, the highly reversible solid-solution K+ intercalation/extraction mechanism in the Ni 2 Zn 1 HCF cathode is illustrated by the in-situ X-ray diffraction. This work presents a promising cathode for building ultrafast and long-service aqueous potassium-ion batteries. Near-pseudocapacitance intercalation and synergistic effect enhanced Ni 2 Zn 1 HCF bimetallic Prussian blue analogues cathode for aqueous potassium-ion batteries is designed. This cathode exhibits excellent rate performance in a wide rate range of 5–1000C, and an ultralong lifespan of 80,000 cycles at 1000C. Image 1 • Ni 2 Zn 1 HCF cathode shows a near-pseudocapacitive K+ intercalation/extraction mechanism. • This cathode enables excellent rate performance and exhibits an ultralong lifespan of 80,000 cycles at 1000C. • A synergistic effect between Ni2+ and Zn2+ in bimetallic Ni 2 Zn 1 HCF is demonstrated. [ABSTRACT FROM AUTHOR]

Surface engineering has been applied to resolve the problem of cycling instability in conversion/alloying reaction electrodes which can have high capacity but suffer from large volumetric change and pulverization in electrochemical cycles. However, due to structural instability, most of the surface coatings are still fragile and unstable in electrochemical cycles. Here, a facile low-temperature melting method has been developed to fabricate a uniform and ultrathin metal-organic framework (MOF) shell on various oxides electrode materials, followed by a gradient heat treatment process. A uniform and ultrathin N-doped carbon (NC) shell is formed as a robust coating to keep the integrity of materials and provide a highly conductive pathway for both electron and ions. This carbon confinement strategy can be easily applied to diverse ternary metal oxides with high bonding energy, such as Zn 2 SiO 4 , Zn 2 WO 4 and Zn 2 TiO 4. The obtained carbon-confined Zn 2 SiO 4 (Zn 2 SiO 4 @NC) nanowires have achieved enhanced lithium storage performances compared to pure Zn 2 SiO 4 nanowires. As revealed by in situ transmission electron microscopy, in the process of lithiation the Zn 2 SiO 4 @NC nanowires have lower radical expansion and faster kinetics than pure Zn 2 SiO 4 nanowires, and the N-doped carbon shell remains stable. This work provides a new approach for the design and construction of carbon-based nanostructures which have great potential in energy-related applications. A general method for fabricating a strong coating layer of N-doped-carbon to confine target nanostructures has been developed via a facile and efficient low temperature melting method of forming metal-organic framework (MOF) and subsequent controlled pyrolysis, to boost the cycling stability of electrode materials run on conversion/alloying reactions for lithium-ion battery. Image 1 • A low-temperature melting method is developed to fabricate a robust MOF derived N-doped carbon shell as a uniform coating for oxides. • The carbon-confined Zn2SiO4 nanowires exhibit enhanced lithium storage performance compared to pure Zn2SiO4 nanowires. • In situ transmission electron microscopy has revealed that the N-doped carbon shell remains intact in lithiation. • The carbon-confined Zn2SiO4 nanowires have lower radical expansion and faster kinetics than pure Zn2SiO4 nanowires. [ABSTRACT FROM AUTHOR]

[Display omitted] Potassium-ion batteries (PIBs) have aroused considerable interest as a promising next-generation advanced large-scale energy storage system due to the abundant potassium resources and high safety. However, the K+ with large ionic radius brings restricted diffusion kinetics and severe volume expansion in electrode materials, resulting in inferior actual rate characteristics and rapid capacity fading. Designing electrode materials with one-dimensional (1D) nanostructure can effectively enhance various electrochemical properties due to the well-guided electron transfer pathways, short ionic diffusion channels and high specific surface areas. In this review, we summarize the recent research progress and achievements of 1D nanostructure electrode materials in PIBs, especially focusing on the development and application of cathode and anode materials. The nanostructure, synthetic methods, electrochemical performances and structure-performance correlation are discussed in detail. The advanced characterizations on the reaction mechanisms of 1D nanostructure electrode materials in PIBs are briefly summarized. Furthermore, the main future research directions of 1D nanostructure electrode materials are also predicted, hoping to accelerate their development into the practical PIBs market. [ABSTRACT FROM AUTHOR]

The conversion of biomass waste into functional carbon materials is an environmentally friendly solution with diverse applications for a sustainable world. Here, we report an approach to fabricate the Ganoderma Lucidum waste-derived erythrocyte-like N, O self-doped porous biomass carbon (GL800) with a high graphitization degree by a facile carbonization and activation method. The prepared GL800 showed a relatively high specific surface area (2407.5 m2 g−1) and a porous structure like the red blood cell, which affords enough space to accommodate active sites and are easy for electrolytes to infiltrate. Due to the synergistic effect of the rich N, O self-doped elements and porous structures, GL800 shows strong chemical adsorption and physical confinement for polysulfide. Lithium-sulfur batteries using GL800 electrodes exhibited a high discharge capacity of 1367.8 mA g−1 at 0.1C and desirable rate performance. Furthermore, the battery has a capacity retention rate after 300 cycles at 0.5C with high coulombic efficiency (99%). Together with the good biocompatibility and biodegradability of the prepared material, it has a high potential for diverse applications in energy storage, environmental remediation, wearable electronics, biomedicine, and other areas, providing a Nature-derived solution with good sustainability. The reasonable conversion of biomass waste into functional carbon materials is an environmentally friendly and sustainable choice for processing biological waste. An erythrocyte-like N, O self-doped porous biological carbon (GL800) with high specific surface area (2407.5 m2 g−1) and high degree of graphitization is fabricated. As a result, lithium-sulfur batteries assembled with GL800/S cathode exhibit excellent electrochemical performances, including a high discharge capacity of 1367.8 mA g−1 at 0.1C and a desirable rate performance. Furthermore, the battery has a capacity retention rate of 72.3% after 300 cycles at 0.5C with high coulombic efficiency (99%). This work is environmentally friendly and shows a great potential for practical applications of biomass carbon material in energy, catalysis, biomedical and other related fields. [Display omitted] [ABSTRACT FROM AUTHOR]