Anode Material For Lithium-ion Batteries Research Articles

Encapsulating Antimony metal nanoparticles in hierarchical porous carbon skeleton as high-performance potassium- and lithium-ion batteries anodes

Metallic antimony (Sb) as alkaline metal battery anode material, being thoroughly researched for its high theoretical specific capacity, but there is still a huge expansion problem with repeated insertion/de-insertion., We reported a unique composite material that encapsulates Sb nanoparticles in hierarchical porous carbon skeletons (Sb@HPCs) in this work, to explore the effect of the hierarchical porous carbon structure on the electrochemical performance of the Sb@HPCs as potassium-ion batteries (KIBs) and lithium-ion batteries (LIBs) anode materials. The macropores could promote the penetration of electrolyte, thus reducing the internal impedance of the battery. The mesopores provide a short ion diffusion path and a large diffusion region, which plays a crucial role in facilitating rapid ionic migration in both KIBs and LIBs. The micropores in the electrode material contribute to a larger specific surface area, which provides more surface area for charge storage, thus enhancing the energy density of the material. Importantly, when the Sb@HPCs composite material is applied as anode material of KIBs, it exhibits an outstanding specific capacity of 360 mAh g−1 after 100 cycles at 100 mA g−1. In the LIBs, the specific capacity of the composite material is 595.2mAh g−1 after 100 cycles at a current density of 0.1 A g−1; even at a high current density of 1.0 A g−1, the specific capacity still maintains at 320.4 mAh g−1 after 800 cycles, indicating an excellent cycling stability. The development of hierarchical porous three-dimensional structure offers a practical solution to the capacity degradation issues of metal anode in KIBs/LIBs.

Enhanced reversible reaction of hexagonal SnS2@rGO as anode materials for lithium-ion batteries: Analysis of the morphological change mechanism

Tin-based materials have attracted attention as a promising anode material for lithium-ion batteries due to their high theoretical capacity and alloy metal characteristics. However, the structure tends to easily collapse with repetitive charging and discharging processes, leading to volume expansion. The conversion step in the SnS2 reaction mechanism is also sometimes considered irreversible. To address these challenges, this study synthesized layered hexagonal 2D structure-type SnS2 using the oleylamine as surfactant through a wet chemical process. Subsequently, SnS2@rGO was synthesized after compounding with reduced graphene oxide (rGO), utilizing a smaller amount of nanomaterials compared to rGO, showing optimal efficiency. The morphological changes in SnS2 and SnS2@rGO during the charging and discharging processes was revealed that pulverization occurred more slowly in SnS2@rGO compared to SnS2. We quantified the volume expansion rates of SnS2 and SnS2@rGO electrodes, demonstrating that rGO effectively reduces volume expansion. Additionally, an analysis of lithiation mechanism through a comprehensive analysis method using CV, ex-situ XRD, and ex-situ TEM demonstrated that SnS2@rGO enhanced Li+ storage characteristics compared to SnS2, resulting in more reversible chemical changes. rGO and bare SnS2 show poor capacities 307.23 mAh/g and 87.17 mAh/g after 120 cycles, respectively. However bare SnS2 anchored on the surface of rGO exhibits increased electrical conductivity and improved performance (711 mAh/g after 120 cycles), confirming that rGO plays an important role. SnS2@rGO showed enhanced cycling stability and discharge capacity as shown in the electrochemical testing.

Iodine- and nitrogen-CO-doped carbon flower materials for the anode electrode of lithium-ion batteries

As green anode materials with wide distribution, controllable cost, and diversified structure, carbon materials have received more attention. In this paper, iodine- and nitrogen-co-doped carbon flower materials were prepared. The flower-like structure of the material ensures the rapid diffusion of lithium ions, and the synergistic effect of iodine and nitrogen atoms improves the pore size distribution, the conductivity and the active sites of carbon materials realizing the high ion storage and the fast charge diffusion. As the anode material of lithium-ion batteries, the iodine- and nitrogen-co-doped carbon flower could have the capacitance of 410 mAh g[Formula: see text] at the current density of 0.1 A g[Formula: see text] after 150 cycles and 181 mAh g[Formula: see text] at the high current density of 2.0 A g[Formula: see text] after 1000 cycles. The results of electrochemical impedance spectroscopy, kinetics, and GITT show this material has fast charge transport kinetics and excellent rate performance.

In situ steam oxidation of nickel phosphide/carbon composite nanofibers as anode materials for lithium-ion batteries

The synthesis of self-standing nickel phosphide/carbon (NixP/C) composite nanofibers is accomplished through a one-pot electrospinning and in situ steam oxidation after the carbothermal reduction process. Control over the levels of in situ steam oxidizers in the forms of crystal water and nitrates in the precursor fibers is achieved by systematically adjusting the drying temperature before the high-temperature heat treatment. This led to structural modifications in the final products analyzed through comprehensive characterizations. Mechanistic insights into the in situ steam oxidation process are provided, emphasizing its potential in optimizing electrode materials. Electrochemical assessments reveal significantly improved performance in the sample prepared from the media with optimal content of oxidizers, attributed to a tailored surface oxide layer, electronic configuration, and microstructure, enabling enhanced reaction kinetics and minimizing volume expansion. This results in exceptional cycling stability and notable capacity retention during prolonged charge-discharge cycles. Thus, NixP/C achieves the highest initial charge capacity of 719.5 mAh g−1 with an initial Coulombic efficiency of 61% and maintains a high capacity of 590.7 mAh g−1 after 100 cycles at a current density of 0.1 A g−1.

Spontaneous Electrochemical Reconstruction of NiNb2O6@C for High-Rate Lithium-Ion Batteries

Niobium oxides are widely active in the arena of lithium-ion batteries due to their distinctive structure and rapid charging capability, nevertheless facing the serious challenge from their inherently low electrical conductivity. Herein, a molten salt method is proposed to prepare nickel niobate (NiNb2O6) anode materials for lithium-ion batteries, and a carbon coating derived from mesophase pitch is fabricated to construct NiNb2O6@C composites. Importantly, NiNb2O6@C undergoes spontaneous electrochemical reconstruction to generate metallic Ni and amorphous Nb2O5 during the initial charge/discharge cycle. The presence of the outer carbon layer not only serves as a uniform conductive coating to improve the conductivity and thereby deliver superior rate performance, but also effectively inhibits the stripping of Ni0 to guarantee a great cycling stability. The synergistic effects of the dual conductive interfaces, consisting of the carbon layer and the Mott-Schottky heterojunction between amorphous Nb2O5 and metallic Ni, culminate in exceptional electrochemical performance. Specifically, NiNb2O6@C-10% delivers impressive specific capacity of 436.3 mAh g−1 at 0.5C and conspicuous cycling stability, maintaining 86.3% capacity retention after 800 cycles at 10C. This work underscores the substantial potential of nickel niobate anode materials in advancing the development of next-generation lithium-ion batteries.

Elucidating the role of embedding dispersed cobalt sites in nitrogen-doped carbon frameworks in Si-based anodes for stable and superior storage

Unsatisfactory conductivity and volume effects have hindered the commercial application of silicon-based materials as advanced anode materials for high-performance lithium-ion batteries. Herein, nitrogen doped carbon silicon matrix composite with atomically dispersed Co sites (Si/Co-N-C) is obtained via the design of the frame structure loaded with nano-components and the multi-element hybrid strategy. Co atoms are uniformly fixed to the N-C frame and tightly packed with nanoscale silicon particles as an activation and protection building block. The mechanism of the N-C framework of loaded metal Co in the Si alloying process is revealed by electrochemical kinetic analysis and ex situ characterization tests. Impressively, the nitrogen-doped Co site activates the intercalation of the outer carbon matrix to supplement the additional capacity. The Co nanoparticles with high conductivity and support enhance the conductivity and structural stability of the composite, accelerating the Li+/Na+ diffusion kinetics. Density functional theory (DFT) calculation confirms that the hetero-structure Si/Co-N-C adjusts the electronic structure to obtain good lithium-ion adsorption energy, reduces the Li+/Na+ migration energy barrier. This work provides meaningful guidance for the development of high-performance metal/non-metal modified anode materials.

Topological Transformation of Hydrogen-Terminated Germanium to Germanium Nanosheets for Fast Lithium Storage.

Germanium has been recognized as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and excellent lithium-ion diffusivity. Nonetheless, it is challenging to enhance both the high-rate performance and long-term cycling stability simultaneously. This study introduces a novel heterostructure composed of germanium nanosheets integrated with graphene (Ge NSs@Gr). These nanosheets undergo an in situ phase transformation from a hydrogen-terminated multilayer germanium compound termed germanane (GeH) derived via topochemical deintercalation from CaGe2. This approach mitigates oxidation and prevents restacking by functionalizing the exfoliated germanane with octadecenoic organic molecules. The resultant germanium nanosheets retain their structural integrity from CaGe2 and present an exposed, active (111) surface that features an open crystal lattice, facilitating swift lithium-ion migration conducive to lithium storage. The composite material delivers a substantial reversible capacity of 1220 mA h g-1 at a current density of 0.2 C and maintains a capacity of 456 mA h g-1 even at an ultrahigh current density of 10 C over extended cycling. Impressively, a capacity of 316 mA h g-1 remains after 5000 cycles. The exceptional high-rate performance and durable cycling stability underscore the Ge NSs@Gr anode's potential as a highly viable option for LIBs.

Experimental study on the mechanical and electrochemical properties of aqueous emulsifiable diphenylmethane diisocyanate-modified silicon-carbon composite electrodes.

Aqueous emulsifiable diphenylmethane diisocyanate (EMDI) can form strong chemical bonds with aqueous adhesives due to the large number of isocyanate (-NCO) groups, which can enhance the mechanical performance of the adhesives. Currently, sodium carboxymethyl cellulose (CMC)-styrene butadiene rubber (SBR) emulsion aqueous bonding agents are widely used in the preparation of anode materials for lithium-ion batteries (LIBs). In this study, EMDI was added to a porous silicon-carbon composite electrode prepared from CMC-SBR, and the evolution of the mechanical properties of the electrode with the EMDI content was first investigated via quasi-static uniaxial tensile and interfacial strength tests. Subsequently, the effect of the EMDI content on the electrochemical properties of the electrodes was analysed by electrochemical impedance spectroscopy (EIS) and constant-current (CC) charge/discharge performance tests. Finally, material characterisation of the electrodes was carried out by Fourier transform infrared (FTIR) spectroscopy and specific surface area (Brunauer-Emmett-Teller (BET)) analysis. The results show that the addition of EMDI with a mass ratio of 10-20% to the CMC-SBR binder can enhance the mechanical performance of the active layer and the interfacial performance between the active layer and the current collector of the silicon-carbon composite electrode; simultaneously, EMDI can significantly reduce the electrochemical impedance of the electrode material and improve the capacity retention of the electrode. This study provides a new solution for modifying silicon-carbon composite electrodes and promotes the development of high-performance silicon-carbon electrodes.

Si@porous carbon fiber fabricated via wet spinning as a high-performance anode material for lithium-ion battery

Si/C composites are considered as attractive anode candidates for high-energy-density lithium-ion batteries and have been extensively researched. The carbon fiber (CF) fabricated by wet spinning is a well-established technology. However, there are scarce reports on Si/CF anodes fabricated by wet spinning. In this study, Si@porous carbon fiber (Si@PCF) composite were synthesized via wet spinning and subsequent thermal treatment. The porous carbon (PC) can effectively buffer the huge volume changes of Si nanoparticles during the charge-discharge process, promote the diffusion and transport of lithium ions, and compensate for the poor electronic conductivity of Si. The Si@PCF composite maintained a high capacity of 1178 mA h g−1 at 0.5 A g−1 after 100 cycles, suggesting potential for commercial application of the Si/PCF anode due to the excellent electrochemical performance and preparation technology suitable for large-scale production.

Mesoporous carbon hollow spheres with controllable pore structure for efficient lithium and aluminum ion storage

Mesoporous carbon hollow nanospheres (MCHS), synthesized via a block copolymer-mediated supramolecular self-assembly process, serve as both anode materials for lithium-ion batteries (LIBs) and cathode materials for aluminum-ion batteries (AIBs). By adjusting the carbonization temperature and the dosage of the pore extender, 1,3,5-trimethylbenzene (TMB), insights into the relationships among pore structure, crystal structure, and electrochemical properties of MCHS in Li/Al-ion batteries are gained. Their exceptional properties, including hierarchically porous structure, large surface area, tailored inner voids, mesoporous shells, and high electronic conductivity, contribute to high specific capacity, improved rate performances, and remarkable electrochemical stability. Crystallographic insights reveal that highly porous MCHS facilitate the intercalation of ionic lithium and aluminum species into the carbon crystal lattices while maintaining structural integrity. The appropriate mesopore size significantly impacts the storage of lithium or aluminum ions, with relatively larger mesopore sizes being more beneficial for aluminum ion storage compared to lithium ions. The optimal MCHS exhibit a stable discharge specific capacity of 330.8 mAh·g−1 after 800 cycles at a current density of 372 mA·g−1 (1C) in LIBs and 41.6 mAh·g−1 after 500 cycles at 74.4 mA·g−1 in AIBs.

Effects of cation substitution effects of dicarboxylic acid for energy storage applications

Organic materials (OMs) can accept alkali ions and function as energy storage systems, displaying several advantages such as low cost, ease of synthesis, and utilization of recyclable materials. Owing to their higher theoretical capacity, OMs exhibit a higher energy density, cheaper price, and easy recover than those of inorganic materials such as graphite, silicon, and metal oxides, respectively. This study reports the use of potassium 4-oxo-4H-pyran-2,6-dicarboxylic acid (K2CDA) and potassium 4-oxo-4H-pyran-2,6-dicarboxylic acid (K2CDO) as anode materials for potassium-ion batteries (KIBs) and lithium-ion batteries (LIBs). Although they share similar lightweight, carbonyl, and carboxylate functional groups, both materials display distinct reaction behaviors owing to differences in electronegative heteroatoms N and O. In this study, two alkaline salts (KFSI and LiFSI) have been discussed on the substitution effect of doping/ de-doping processes. K2CDA and K2CDO. Consequently, after 200 cycles, the K2CDA anodes deliver capacities of 310 (KFSI) and 485 (LiFSI) mAh g−1, respectively, at 0.1 C. The larger size of K+ compared with Li+ negatively impacts the performance of K2CDA. A similar trend is observed in the case of K2CDO in capacities of 220 (KFSI) and 405 mAh g‒1 (LiFSI), with 1.5 and 2.86 K+ ions participated in the corresponding redox reactions on the Fourier-transfer infrared spectroscopy analysis. The presence of N‒H in the K2CDA structure contributes to its superior performance and rate capability compared with K2CDO. In addition to the cation effect, the structural differences between K2CDA and K2CDO also influence their electrochemical activity.

Fabrication of heteroatom-doped cobalt oxide yolk–shell microsphere using recycled solution from waste materials and their excellent electrochemical properties as an anode material for lithium-ion batteries

Fabrication of heteroatom-doped cobalt oxide yolk–shell microsphere using recycled solution from waste materials and their excellent electrochemical properties as an anode material for lithium-ion batteries

Ice template-induced assembly coupled with carbonization strategy for preparation of sulfur-doped porous carbon nanosheets from lignite as high-capacity anode for lithium-ion batteries

Two-dimensional (2D) porous carbon nanosheets with heteroatom doping are promising anode materials for lithium-ion batteries (LIBs) due to their distinctive sheet-like structure and excellent electrical conductivity. Limited by high preparation costs and cumbersome preparation processes, the large-scale production of carbon nanosheets remains a major challenge. Herein, a series of sulfur-doped porous carbon nanosheets (SCNSs) are successfully synthesized through ice template-induced assembly coupled with a carbonization approach using aromatic ring fragments exfoliating from lignite as the precursor and K2SO4 as the sulfur source. The prepared SCNSs exhibit well-defined sheet-like structures, abundant hierarchical nanopores, large specific surface areas (∼1761 m2·g−1), and high sulfur doping contents (∼7.72 at%). Such unique microstructure characteristics of SCNSs not only provide favorable and efficient channels for the lithium-ions/electrons transportation but also offer sufficient available space or active sites for lithium-ions storage. When used as anode materials for LIBs, the SCNS-3 shows high reversible capacity (1620 mAh·g−1 at 0.05 A·g−1), excellent rate performance (315 mAh·g−1 at 2 A·g−1), and superior cycling stability (901 mAh·g−1 at 1 A·g−1 after 500 cycles). Lithium storage behavior analysis indicated that the capacitance enhancement in SCNSs anodes is primarily due to improved capacitive behavior. This study provides a novel and effective route for the large-scale production of sulfur-doped carbon nanosheets using aromatic ring fragments exfoliated from lignite, which demonstrates promising industrial application potential in LIBs anode materials.

A multi-strategic exploration towards significantly enhanced electrochemical performance of Co3O4-based anodes for lithium-ion batteries

Electroactive cobalt oxide (Co3O4) exhibits great promise as an anode material for lithium-ion batteries (LiBs) owing to its high theoretical capacity. However, its potential application faces challenges posed by low conductivity and poor cycling stability. In this study, a comprehensive multi-strategic approach was employed to fabricate a high-performance Co3O4-based anode. The approach involved utilizing Co–Cu bimetallic metal-organic frameworks (MOFs) anchored on a stainless-steel mesh (SSM) as the precursor. The resulting free-standing anode comprises Cu-doped porous Co3O4 nanosheets, offering several advantageous characteristics such as being binder-free, possessing a hierarchically porous architecture, and demonstrating improved conductivity and structure stability. This combination of merits results in a material that exhibits significantly enhanced electrochemical performance, featuring high specific capacity, excellent cycling stability, and remarkable rate performance. This multi-strategic exploration of metal oxides with tailored surface area and pore size enables the precise design and fabrication of advanced anodes, specifically optimized for the demanding requirements of LiBs.

Empowering lithium-ion batteries: The potential of 2D o-Al2N2 as an exceptional anode material through DFT analysis

Finding an appropriate new anode material with high electrochemical performance for lithium-ion batteries (LIBs) is considered one of the significant challenges for both the academic and industrial research communities. Herein, we propose to explore the efficiency of a newly designed two-dimensional (2D) material, named orthorhombic dialuminium dinitride (o-Al2N2), as an alternative anode material for LIB systems through first-principles calculations and ab initio molecular dynamics (AIMD) simulations. The obtained results show that orthorhombic-Al2N2 exhibits a high specific capacity of 1144.2913 mAhg−1, an operating voltage around 0.575 V, and a low kinetic diffusion barrier of 0.26 eV. These results prove the suitability of the o-Al2N2 monolayer as a promising anode material for LIBs with high structural stability, strong binding energy towards lithium adsorbent, fast lithium diffusion, and a high theoretical capacity. These features rank the 2D o-Al2N2 monolayer among the best choices for the anode part of the next-generation rechargeable LIBs.

Enhanced electrochemical performance of MgFeO4 spinel as anode materials for Lithium-ion batteries through manganese doping

Existing graphite anode materials are reaching their limits, and iron-based AB2O4 spinel materials are considered as potential anodes for Li-ion batteries owing to their significant theoretical capacities. In this work, novel nanocrystalline MgFe2-xMnxO4 (x = 0, 0.1, 0.2, and 0.3) spinel ferrites were evaluated as anode materials for high-capacity Li-ion batteries. The Mn-doped MgFe2-xMnxO4 (x = 0, 0.1, 0.2, and 0.3) spinel ferrites were synthesized through a facile sol-gel synthesis method coupled with an annealing process. Their crystal structure, morphology, and purity were examined via X-ray diffraction (XRD), Raman spectroscopy, and scanning electron microscopy (SEM). The X-ray diffraction analyses with Rietveld refinement of the synthesized ferrites reveal pure cubic structure with a characteristic Fd3̅m space group for all prepared samples. This was confirmed by Raman spectroscopy by revealing five spinel Raman active modes. The SEM images showed interconnected nanosized particles for all compositions, which led to a porous morphology. Their electrochemical proprieties as anode materials for Li-ion batteries were examined by cyclic voltammetry and galvanostatic charge-discharge tests. For all compositions, the cyclic voltammetry plots demonstrate the conversion type for the Li-ion storage mechanism. At an applied current density of 150 mA g−1, the compositions x = 0, 0.1, 0.2, and 0.3 show initial discharge/charge capacities of 1235/712, 1187/680, 1542/938, and 1239/768 mAh g−1, respectively. After 100 operational cycles, their galvanostatic charge/discharge capacities remain 529/534, 612/606, 642/663, and 700/700 mAh g−1. However, the compositions x = 0.2 and 0.3 exhibit excellent cycling stability during 100 cycles, even at higher rates. As a result, the Mn doping led to enhanced specific capacity and cycling stability of the MgFe2O4 spinel. The optimized compositions with x = 0.2 and 0.3 are, thus, proposed as promising anodes materials compositions for Li-ion batteries.

Constructing heterojunction-induced oxygen vacancies of N-doped carbon-encapsulated Sn/SnOx microplates for boosting lithium storage capability

Heterogeneous Sn/SnOx@N-doped carbon (Sn/SnOx@NC) microplates with oxygen vacancies evolved from plate-like SnO powders are successfully fabricated, in which SnO powders are converted into Sn, SnO2, and Sn2O3 phases by rationally sintering and are perfectly in situ encapsulated by polyaniline-derived NC layer. By elaborately constructing the particular structure, high discharge specific capacity of 730.4 mAh/g and capacity retention ratio of 98.3 % after 110 cycles at 0.1 A/g are realized for optimal Sn/SnOx@NC composite electrode. Benefiting from enhanced electronic conductivity and Li+ ions diffusion kinetics, the assembled cell delivers reversible discharge specific capacity of 487.3 mAh/g at 1.0 A/g after 500 cycles. First principles calculation and in/ex situ characterization reveal that in situ formed heterostructure with oxygen vacancies and NC layer synergistically improve interfacial charge transfer and reaction reversibility to promote lithium storage capability. Therefore, fabricating Sn/SnOx@NC microplates may provide a practical strategy to design heterogeneous and oxygen-deficient Sn-based anode materials for high-performance lithium-ion batteries.

Arc-Discharge In Situ Synthesis of Dual-Carbonaceous-Layer-Coated SnS Nanoparticles with High Lithium-Ion Storage Capacity.

SnS-based carbon composites have garnered considerable concentration as prospective anode materials (AMs) for lithium-ion batteries (LIBs). Nevertheless, most SnS-based carbon composites underwent a two-phase or multistep preparation process and exhibited unsatisfactory LIB performance. In this investigation, we introduce a straightforward and efficient one-step arc-discharge technique for the production of dual-layer carbon-coated tin sulfide nanoparticles (SnS@C). The as-prepared composite is used as an AM for LIBs and delivers a high capacity of 1000.4 mAh g-1 at 1.0 A g-1 after 520 cycles. The SnS@C still maintains a capacity of 476 mAh g-1 after 390 cycles despite a higher current of 5.0 A g-1. The high specific capacity and long life are mainly attributed to a unique dual-carbon layers coating structure. The dual-carbon layers not only could effectively improve electrical conductivity and reduce charge-transfer resistance but also limit the alteration in bulk and self-aggregation of SnS nanoparticles. The SnS@C produced by the arc-discharge technique emerges as a promising applicant for AM in LIBs, and the arc-discharge technique provides an alternative way for synthesizing other transition metal sulfides supported on carbonaceous materials.

Structural modulation of Nb2O5 for enhanced Lithium-ion battery Performance: Insights from density functional theory and electrochemical characterization

Lithium-ion batteries (LIBs), extensively utilized today, encounter challenges with anode materials, such as capacity degradation and shortened cycle life during prolonged cyclic charging and discharging. These issues significantly hinder further advancements and applications of LIBs. Among various innovative anode materials, niobium pentoxide (Nb2O5) has garnered considerable interest due to its high specific capacity and exceptional cycling stability. However, different crystal types of Nb2O5 have different structures and properties, so they need to be studied in depth to find better anode materials for LIBs. In this paper, pseudo-hexagonal (TT-Nb2O5), orthorhombic (T-Nb2O5), and monoclinic (H-Nb2O5) crystalline forms of Nb2O5 have been prepared by simple ball milling and calcination methods. We have calculated the structural model of the material based on the density flooding theory (DFT), and the results have demonstrated that the T-Nb2O5 has a large structural advantage, which is characterized by a very low diffusion energy barrier, a low internal resistance, and a higher conductivity. The electrochemical properties of the material were also analyzed, and T-Nb2O5 has excellent cycling stability and rate performance. After 200 cycles (at 0.1A/g), the specific capacity of T-Nb2O5 was maintained at 440.8mAh/g. 3000 cycles at high current (at 5A/g) maintained a specific capacity of 95mAh/g. T-Nb2O5 has great potential, which has already been proved. With the continuous pursuit and development of energy storage technology, we believe that the research of different crystalline types of Nb2O5 will provide us with more efficient and reliable energy storage solutions.

Role of the Microstructure in the Li-Storage Performance of Spinel-Structured High-Entropy (Mn,Fe,Co,Ni,Zn) Oxide Nanofibers

High-entropy oxides with spinel structure (SHEOs) are promising anode materials for next-generation lithium-ion batteries (LIBs). In this work, electrospun (Mn,Fe,Co,Ni,Zn) SHEO nanofibers produced under different conditions are evaluated as anode materials in LIBs and thoroughly characterised by a combination of analytical techniques. The variation of metal load (19.23 or 38.46 wt% relative to the polymer) in the precursor solution and of calcination conditions (700 °C/0.5 h, or 700 °C/2 h followed by 900 °C/2 h) affects the morphology, microstructure, crystalline phase, and surface composition of the pristine SHEO nanofibers and the resulting electrochemical performance, whereas mechanism of Li+ storage does not substantially change. Causes of long-term (≥650 cycles) capacity fading are elucidated via ex situ synchrotron X-ray absorption spectroscopy. The results evidence that the larger amounts of Fe, Co, and Ni cations irreversibly reduced to the metallic form during cycling are responsible for faster capacity fading in nanofibers calcined under milder conditions. The microstructure of the active material plays a key role. Nanofibers composed by larger and better-crystallized grains, where a stable solid/electrolyte interphase forms, exhibit superior long-term stability (453 mAh g−1 after 550 cycles at 0.5 A g−1) and rate-capability (210 mAh g−1 at 2 A g−1).