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1.
    
Cation-disordered rocksalts (DRXs) have emerged as a new class of high-capacity Li-ion cathode materials. One unique advantage of the DRX chemistry is the structural flexibility that substantially lessens the elemental constraints in the crystal lattice, such as Li content, choice of transition metal redox center paired with appropriate d0 metal, and incorporation of F anion, which allows optimization of the key redox reactions. Herein, a series of the DRX oxyfluorides based on the Mn redox have been designed and synthesized. By tailoring the stoichiometry of the DRX compositions, high-capacity cycling by promoting the cationic Mn2+/Mn4+ redox reactions while suppressing those from anionic O is successfully demonstrated. A highly fluorinated DRX compound, Li1.2Mn0.625Nb0.175O1.325F0.675 (M0.625F0.675), delivers a capacity of ≈170 mAh g−1 at C/3 for 100 cycles. This work showcases the concept of balancing the cationic and anionic redox reactions in the DRX cathodes for improved electrochemical performance through the rational composition design.  相似文献   

2.
    
As the dominant means of energy storage technology today, the widespread deployment of lithium-ion batteries (LIBs) would inevitably generate countless spent batteries at their end of life. From the perspectives of environmental protection and resource sustainability, recycling is a necessary strategy to manage end-of-life LIBs. Compared with traditional hydrometallurgical and pyrometallurgical recycling methods, the emerging direct recycling technology, rejuvenating spent electrode materials via a non-destructive way, has attracted rising attention due to its energy efficient processes along with increased economic return and reduced CO2 footprint. This review investigates the state-of-the-art direct recycling technologies based on effective relithiation through solid-state, aqueous, eutectic solution and ionic liquid mediums and thoroughly discusses the underlying regeneration mechanism of each method regarding different battery chemistries. It is concluded that direct regeneration can be a more energy-efficient, cost-effective, and sustainable way to recycle spent LIBs compared with traditional approaches. Additionally, it is also identified that the direct recycling technology is still in its infancy with several fundamental and technological hurdles such as efficient separation, binder removal and electrolyte recovery. In addressing these remaining challenges, this review proposes an outlook on potential technical avenues to accelerate the development of direct recycling toward industrial applications.  相似文献   

3.
    
A sodium‐ion battery operating at room temperature is of great interest for large‐scale stationary energy storage because of its intrinsic cost advantage. However, the development of a high capacity cathode with high energy density remains a great challenge. In this work, sodium super ionic conductor‐structured Na3V2?xCrx(PO4)3 is achieved through the sol–gel method; Na3V1.5Cr0.5(PO4)3 is demonstrated to have a capacity of 150 mAh g?1 with reversible three‐electron redox reactions after insertion of a Na+, consistent with the redox couples of V2+/3+, V3+/4+, and V4+/5+. Moreover, a symmetric sodium‐ion full cell utilizing Na3V1.5Cr0.5(PO4)3 as both the cathode and anode exhibits an excellent rate capability and cyclability with a capacity of 70 mAh g?1 at 1 A g?1. Ex situ X‐ray diffraction analysis and in situ impedance measurements are performed to reveal the sodium storage mechanism and the structural evolution during cycling.  相似文献   

4.
锂离子电池正极材料研究进展   总被引：2，自引：0，他引：2  
主要介绍了传统锂离子电池正极材料的改性研究和新型锂离子电池正极材料的研究现状和发展方向.重点综述了正硅酸盐Li2MSiO4(M=Fe,Mn)类正极材料,含V的正极材料,有机物正极材料以及其他新型锂离子电池正极材料的研究现状和性能改进方法.  相似文献   

5.
    
How to tune the activity and reversibility of oxygen anion redox (OAR) is a critical issue for O3-type sodium-ion battery (SIB) cathodes. Herein, the key role of electronegativity-difference configuration on the activation of OAR is find out, and further tune electronegativity-difference configuration with La incorporation to construct non-bonded O 2p orbitals and achieve the reversible anionic redox in O3-type NaMn1/3Fe1/3Ni1/3O2. Owing to the special extranuclear electronic structure of La3+ [Xe], the La electron cloud is difficult to be disturbed by the O electron cloud, and some O electrons do not participate in the formation of ionic bonds, thus retaining the non-bonded electrons of O 2p and activating OAR. Moreover, La3+ doping also decreases the Coulomb force between Na+ and O2− favoring Na+ migration as well as strengthening the La─O bonds inhibiting the irreversible phase transition. La2O3 coating layer also plays a role on inhibiting the reaction between molecular oxygen and the electrolyte, and making OAR reversible. After modification, the cycling stability is significantly improved (86.9% vs 27.3%@2C@200cycles; 90.8% vs 52.9%@5C@300 cycles). This study presents some insights on OAR activation mechanism and offers a facile strategy to improve the activity and reversibility of OAR for designing high performance SIBs cathodes.  相似文献   

6.
    
Cathodes in lithium-ion batteries with anionic redox can deliver extraordinarily high specific capacities but also present many issues such as oxygen release, voltage hysteresis, and sluggish kinetics. Identifying problems and developing solutions for these materials are vital for creating high-energy lithium-ion batteries. Herein, the electrochemical and structural monitoring is conducted on lithium-rich cathodes to directly probe the formation processes of larger voltage hysteresis. These results indicate that the charge-compensation properties, structural evolution, and transition metal (TM) ions migration vary from oxidation to reduction process. This leads to huge differences in charge and discharge voltage profile. Meanwhile, the anionic redox processes display a slow kinetics process with large hysteresis (≈0.5 V), compared to fast cationic redox processes without any hysteresis. More importantly, a simple yet effective strategy has been proposed where fine-modulating local oxygen environment by the lithium/oxygen (Li/O) ratio tunes the anionic redox chemistry. This effectively improves its electrochemical properties, including the operating voltage and kinetics. This is also verified by theoretical calculations that adjusting anionic redox chemistry by the Li/O ratio shifts the TM 3d—O 2p bands and the non-bonding O 2p band to a lower energy level, resulting in a higher redox reaction potential.  相似文献   

7.
    
With the rapid growth in energy consumption, renewable energy is a promising solution. However, renewable energy (e.g., wind, solar, and tidal) is discontinuous and irregular by nature, which poses new challenges to the new generation of large-scale energy storage devices. Rechargeable batteries using aqueous electrolyte and multivalent ion charge are considered more suitable candidates compared to lithium-ion and lead-acid batteries, owing to their low cost, ease of manufacture, good safety, and environmentally benign characteristics. However, some substantial challenges hinder the development of aqueous rechargeable multivalent ion batteries (AMVIBs), including the narrow stable electrochemical window of water (≈1.23 V), sluggish ion diffusion kinetics, and stability issues of electrode materials. To address these challenges, a range of encouraging strategies has been developed in recent years, in the aspects of electrolyte optimization, material structure engineering and theoretical investigations. To inspire new research directions, this review focuses on the latest advances in cathode materials for aqueous batteries based on the multivalent ions (Zn2+, Mg2+, Ca2+, Al3+), their common challenges, and promising strategies for improvement. In addition, further suggestions for development directions and a comparison of the different AMVIBs are covered.  相似文献   

8.
    
The development of high‐energy and high‐power density sodium‐ion batteries is a great challenge for modern electrochemistry. The main hurdle to wide acceptance of sodium‐ion batteries lies in identifying and developing suitable new electrode materials. This study presents a composition‐graded cathode with average composition Na[Ni0.61Co0.12Mn0.27]O2, which exhibits excellent performance and stability. In addition to the concentration gradients of the transition metal ions, the cathode is composed of spoke‐like nanorods assembled into a spherical superstructure. Individual nanorod particles also possess strong crystallographic texture with respect to the center of the spherical particle. Such morphology allows the spoke‐like nanorods to assemble into a compact structure that minimizes its porosity and maximizes its mechanical strength while facilitating Na+‐ion transport into the particle interior. Microcompression tests have explicitly verified the mechanical robustness of the composition‐graded cathode and single particle electrochemical measurements have demonstrated the electrochemical stability during Na+‐ion insertion and extraction at high rates. These structural and morphological features contribute to the delivery of high discharge capacities of 160 mAh (g oxide)?1 at 15 mA g?1 (0.1 C rate) and 130 mAh g?1 at 1500 mA g?1 (10 C rate). The work is a pronounced step forward in the development of new Na ion insertion cathodes with a concentration gradient.  相似文献   

9.
Lithium‐rich manganese‐based layered oxides show great potential as high‐capacity cathode materials for lithium ion batteries, but usually exhibit a poor cycle life, gradual voltage drop during cycling, and low thermal stability in the highly delithiated state. Herein, a strategy to promote the electrochemical performance of this material by manipulating the electronic structure through incorporation of boracic polyanions is developed. As‐prepared Li[Li0.2Ni0.13Co0.13Mn0.54](BO4)0.015(BO3)0.005O1.925 shows a decreased M‐O covalency and a lowered O 2p band top compared with pristine Li[Li0.2Ni0.13Co0.13Mn0.54]O2. As a result, the modified cathode exhibits a superior reversible capacity of 300 mA h g?1 after 80 cycles, excellent cycling stability with a capacity retention of 89% within 300 cycles, higher thermal stability, and enhanced redox couple potentials. The improvements are correlated to the enhanced oxygen stability that originates from the tuned electronic structure. This facile strategy may further be extended to other high capacity electrode systems.  相似文献   

10.
    
Demand for energy in day to day life is increasing exponentially. However, existing energy storage technologies like lithium ion batteries cannot stand alone to fulfill future needs. In this regard, potassium ion batteries (KIBs) that utilize K ions in their charge storage mechanism have attracted considerable attention due to their unique properties and are therefore established as one of the future battery systems of interest among the scientific community. Nevertheless, the development and identification of appropriate electrode materials is very essential for practical applications. This review features the current development in KIBs electrode and electrolyte materials, the present challenges facing this technology (in the commercial aspect), and future aspects to develop fully functional KIBs. The potassium storage mechanisms, evolution of the KIBs, and the advantages and disadvantages of each category of materials are included. Additionally, various approaches to enhance the electrochemical performances of KIBs are also discussed. This review is not only an amalgamation of different viewpoints in literature, but also contains concise perspectives and strategies. Moreover, the potential emergence of a novel class of K‐based dual ion batteries is also analyzed for the first time.  相似文献   

11.
    
Cation-disordered metal oxides as cathode materials for Li ion batteries have been overlooked from early studies due to to the restriction of Li ion diffusion, leading to poor electrochemical performance. However, the discovery of a new disordered rocksalt (DRX) structured material Li1.211Mo0.467Cr0.3O2 with a high capacity of >260 mAh g−1 at 0.05 C opened new research prospects in this emerging field and established DRX materials as a promising alternative with wider choices of transition metal elements compared with currently widely used layered cathode materials. Some of the major obstacles of the DRX materials include γ-LiFeO2 type cation short-range-order that impedes Li ion diffusion, irreversible oxygen loss, and transition metal dissolution, which also present challenges for appropriate characterization techniques. Several performance optimization strategies have been employed, including fluorine incorporation, high entropy modification, and surface coating. This review article focuses on advancements in characterization techniques to uncover underlying mechanisms of Li ion diffusion and degradation of the DRX cathode materials to address the abovementioned challenges and provide inspiration for future studies of this class of materials.  相似文献   

12.
    
Rechargeable sodium ion batteries (SIBs) are surfacing as promising candidates for applications in large‐scale energy‐storage systems. Prussian blue (PB) and its analogues (PBAs) have been considered as potential cathodes because of their rigid open framework and low‐cost synthesis. Nevertheless, PBAs suffer from inferior rate capability and poor cycling stability resulting from the low electronic conductivity and deficiencies in the PBAs framework. Herein, to understand the vacancy‐impacted sodium storage and Na‐insertion reaction kinetics, we report on an in‐situ synthesized PB@C composite as a high‐performance SIB cathode. Perfectly shaped, nanosized PB cubes were grown directly on carbon chains, assuring fast charge transfer and Na‐ion diffusion. The existence of [Fe(CN)6] vacancies in the PB crystal is found to greatly degrade the electrochemical activity of the FeLS(C) redox couple via first‐principles computation. Superior reaction kinetics are demonstrated for the redox reactions of the FeHS(N) couple, which rely on the partial insertion of Na ions to enhance the electron conduction. The synergistic effects of the structure and morphology results in the PB@C composite achieving an unprecedented rate capability and outstanding cycling stability (77.5 mAh g?1 at 90 C, 90 mAh g?1 after 2000 cycles at 20 C with 90% capacity retention).  相似文献   

13.
采用并流共沉淀法制备了前驱体Ni0.8Co0.2(OH)2,然后采用高温固相反应法制备了锂离子电池正极材料LiNi0.8Co0.2O2,通过热重分析(TG)、X射线衍射(XRD)、扫描电子显微镜(SEM)与恒流充放电测试等研究了烧结温度对所制备材料物相结构、微观形貌和电化学性能的影响。结果表明,在卧式管式炉中空气气氛下进行两段控温烧结:第一段烧结温度为700℃,第二段烧结温度为750℃时,合成的LiNi0.8Co0.2O2具有良好的六方晶系α-NaFeO2层状结构;在0.5C充放电倍率下和2.7-4.3 V电压范围内,其首次放电比容量为153.0 mAh/g,20次循环后的容量保持率高达98.5%。  相似文献   

14.
    
Organic batteries are considered as environmentally friendly alternative to lithium-ion batteries due to the application of transition metal-free redox-active polymers. One well-established polymer is poly(3-vinyl-N-methylphenothiazine) (PVMPT) with a fast reversibility of the electrochemical redox reaction at a potential of 3.5 V versus Li|Li+. The oxidized PVMPT is soluble in many standard battery electrolytes, which diminishes its available specific capacity but at the same time can lead to a unique charge/discharge mechanism involving a redeposition process upon discharge. Herein, the influence of different conductive carbon additives and their properties, e.g., specific surface area, pore size distribution, and electrical conductivity, on the dissolution behavior of oxidized PVMPT is investigated. Compared to the state-of-the-art conductive carbon Super C65 employed in many organic battery electrodes, Ketjenblack EC-300J and EC-600J reduce the dissolution of the oxidized PVMPT due to better immobilization on the carbon additive and in the resulting 3D structure of the electrode, as assessed by N2-physisorption, electrochemical, UV–vis spectroscopy and scanning electron microscopy investigations. The studies demonstrate that a dense packing of the carbon particles in the electrode is decisive for the stable immobilization of PVMPT while maintaining its long-term cycling performance.  相似文献   

15.
    
P2-type layered oxide material Na2/3Ni1/3Mn2/3O2 is a competitive candidate for sodium-ion batteries (SIBs). Nevertheless, it suffers from the strong P2–O2 phase transition during charging to the high voltage regime, rendering drastic volume variations and poor cycling performance. Here, a Quasi-zero strain P2-Na0.75Li0.15Mg0.05Ni0.1Mn0.7O2 cathode is synthesized, which reflects the vanishing P2–O2 transition with a volume change as low as 0.49%, thus resulting in the material an excellent cycling performance (83.9% capacity retention after 500 cycles at 5 C). The low-volume strain can be attributed to two aspects: (1) the Mg2+ riveted in the Na layer can act as a “pillar” to stabilize the crystal structure under the condition of sodium removal, thus restricting the structural changes under high voltage. (2) The entry of Li+ into the transition metal (TM) layer can mitigate the electron localization in the highly desodiation state and can effectively immobilize the coordination oxygen atoms, thus suppressing the slip of P2–O2 transition. This study not only provides a new insight of Li and Mg synergetic substitution effect on the structural stability of P2-type cathode, but also an efficient avenue for developing cathode materials of SIBs with ultralow bulk strain.  相似文献   

16.
The active role of alumina, pentalithium aluminate (Li5AlO4, Li-aluminate), and pentasodium aluminate (Na5AlO4, Na-aluminate) as the surface protection coatings produced via atomic layer deposition on Li and Mn-rich NCM cathode materials 0.33Li2MnO3·0.67LiNi0.4Co0.2Mn0.4O2 is discussed. A notable improvement in the electrochemical behavior of the coated cathodes has been found while tested in Li-coin cells at 30 °C. Though all the coated cathodes demonstrate enhanced electrochemical cycling and rate performances, Na-aluminate coated cathodes exhibit exemplary behavior. Prolonged cycling and rate capability testing demonstrate that after more than 400 cycles at 1 C rate, the uncoated cathode delivers only 63 mAh g−1, while those with alumina, Li-aluminate, and Na-aluminate coatings exhibit approximately two times higher specific capacities. The coated cathodes display steady average discharge potential and lower evolution of the voltage hysteresis during prolonged cycling compared to the uncoated cathode. Importantly, Na-aluminate coated cathode shows a lowering in gases (O2, CO2, H2, etc.) evolution. Post-cycling analysis of the electrodes demonstrates higher morphological integrity of the coated cathode materials and lower transition metals dissolution from them. The coatings mitigate undesirable side reactions between the electrodes and the electrolyte solution in the cells.  相似文献   

17.
钠离子电池电极材料研究进展   总被引：1，自引：0，他引：1  
钠是地球上储量较丰富的元素之一,与锂的化学性能类似,因此也可能适用于锂离子电池体系。钠离子电池相比锂离子电池有诸多优势,如成本低,安全性好,随着研究的深入,钠离子电池将越来越具有成本效益,并有望在未来取代锂离子电池而被广泛应用。介绍了钠离子电池正极材料、负极材料的最新研究进展,分析了该电池未来的研究发展方向。  相似文献   

18.
    
Lithium-rich transition metal cathodes can deliver higher capacities than stoichiometric materials by exploiting redox reactions on oxygen. However, oxidation of O2− on charging often results in loss of oxygen from the lattice. In the case of Li2MnO3 all the capacity arises from oxygen loss, whereas doping with Ni and/or Co leads to the archetypal O-redox cathodes Li[Li0.2Ni0.2Mn0.6]O2 and Li[Li0.2Ni0.13Co0.13Mn0.54]O2, which exhibit much reduced oxygen loss. Understanding the factors that determine the degree of reversible O-redox versus irreversible O-loss is important if Li-rich cathodes are to be exploited in next generation lithium-ion batteries. Here it is shown that the almost complete eradication of O-loss with Ni substitution is due to the presence of a less Li-rich, more Ni-rich (nearer stoichiometric) rocksalt shell at the surface of the particles compared with the bulk, which acts as a self-protecting layer against O-loss. In the case of Ni and Co co-substitution, a thinner rocksalt shell forms, and the O-loss is more abundant. In contrast, Co doping does not result in a surface shell yet it still suppresses O-loss, although less so than Ni and Ni/Co doping, indicating that doping without shell formation is effective and that two mechanisms exist for O-loss suppression.  相似文献   

19.
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20.
    
Chloride ion batteries (CIBs) are regarded as promising energy storage systems due to their large theoretical volumetric energy density, high abundance, and low cost of chloride resources. Herein, the synthesis of CoFe layered double hydroxide in the chloride form (CoFe–Cl LDH), for use as a new cathode material for CIBs, is demonstrated for the first time. The CoFe–Cl LDH exhibits a maximum capacity of 239.3 mAh g?1 and a high reversible capacity of ≈160 mAh g?1 over 100 cycles. The superb Cl? ion storage of CoFe–Cl LDH is attributed to its unique topochemical transformation property during the charge/discharge process: a reversible intercalation/deintercalation of Cl? ions in cathode with slight expansion/contraction of basal spacing, accompanied by chemical state changes in Co2+/Co3+ and Fe2+/Fe3+ couples. First‐principles calculations reveal that CoFe–Cl LDH is an excellent Cl? ion conductor, with extremely low energy barriers (0.12?0.25 eV) for Cl? diffusion. This work opens a new avenue for LDH materials as promising cathodes for anion‐type rechargeable batteries, which are regarded as formidable competitors to traditional metal ion‐shuttling batteries.  相似文献   

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