Using High‐Entropy Configuration Strategy to Design Spinel Lithium Manganate Cathodes with Remarkable Electrochemical Performance

Small, Год журнала: 2025, Номер 21(7)

Опубликована: Янв. 6, 2025

Abstract Owing to its abundant manganese source, high operating voltage, and good ionic diffusivity attributed 3D Li‐ion diffusion channels. Spinel LiMn 2 O 4 is considered a promising low‐cost positive electrode material in the context of reducing scarce elements such as cobalt nickel from advanced lithium‐ion batteries. However, rapid capacity degradation inadequate rate capabilities induced by Jahn–Teller distortion dissolution have limited large‐scale adoption spinel for decades. In this study, 1.98 Mg 0.005 Ti Sb Ce (HE‐LMO) with remarkable interfacial structural cycling stability developed based on complex concentrated doping strategy. The initial discharge retention HE‐LMO are 111.51 mAh g −1 90.55% after 500 cycles at 1 C. as‐prepared displays favorable stability, significantly surpassing pristine sample. Furthermore, theoretical calculations strongly support above finding. has higher more continuous density states Fermi energy level robust bonded electrons among Mn─O atom pairs. This research contributes field high‐entropy modification establishes facile strategy designing manganese‐based batteries (LIBs).

Язык: Английский

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Chromium-doped tunnel-structured VO2(B) nanorods as high-capacity and stable cathode materials for aqueous zinc-ion batteries

Journal of Energy Storage, Год журнала: 2025, Номер 114, С. 115826 - 115826

Опубликована: Фев. 14, 2025

Язык: Английский

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Functionalized MOF enables stable cycling of nickel-rich layered oxides for lithium-ion batteries

Chemical Engineering Journal, Год журнала: 2024, Номер 497, С. 154608 - 154608

Опубликована: Авг. 9, 2024

Язык: Английский

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Designing Isocyanate‐Containing Elastomeric Electrolytes for Antioxidative Interphases in 4.7 V Solid‐State Lithium Metal Batteries

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 9, 2024

Abstract To facilitate the use of solid polymer electrolytes (SPEs) with high‐nickel (Ni) cathodes in high‐voltage lithium (Li) metal batteries (LMBs), it is crucial to address challenges low oxidative stability and formation vulnerable interphases. In this study, isocyanate groups (−N═C═O) are incorporated develop an SPE a bi‐continuous structure, consisting elastomeric plastic crystal phases. This rationally designed exhibits high ionic conductivity (0.9 × 10 −3 S cm −1 at 25 °C), excellent elasticity (elongation break 330%), enhanced (over 4.8 V vs. Li/Li⁺). A full cell, incorporating thin Li foil 40 µm, high‐Ni LiNi 0.8 Co 0.1 Mn O 2 (NCM811) cathode operating 4.7 Li/Li⁺, demonstrates cyclability, retaining 70% its initial capacity after 200 cycles under C‐rate 1C °C. The extended cycling isocyanate‐containing Li/Li⁺ attributed robust compact inorganic‐rich interphases enabled by antioxidative −N−C═O components, as well uniform deposition structured SPE. study suggests that system promising candidate for solid‐state LMBs constructing stable

Язык: Английский

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Consolidating Surface Lattice via Facile Self‐Anchored Oxygen Layer Reconstruction Toward Superior Performance and High Safety Nickel‐Rich Oxide Cathodes

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract Nickel‐rich oxide materials have been recognized as promising cathodes for state‐of‐art high energy lithium‐ion batteries; however, challenges remain in their commercialization due to chemical and structural degradation, poor thermal stability related oxygen lattice destabilization. Herein, this work reports a straightforward approach stabilizing the surface framework by inducing reconstruction via swift proton exchange heat treatment argon atmosphere. The robust structure with localized disordered phase domains effectively suppresses interfacial parasitic reactions highly delithiated reduces detrimental degradation. Enabled strongly anchored framework, consolidated also reinforces cathode featured higher decomposition temperature reduced release under stress. In comparison unmodified counterpart, reconstructed nickel‐rich demonstrates improved cycling rate capability. This reveals critical role of regulating on electrochemical performance behaviors, explores potential feasible modification advanced batteries.

Язык: Английский

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Formation and Variation of the Superstructure of Cation Ordering in Layered Cathode Materials

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Фев. 17, 2025

This study employs aberration-corrected transmission electron microscopy to provide definitive evidence of cation ordering within the superstructure LiNi0.5Co0.2Mn0.3O2 (NCM523), a prominent Ni-rich ternary cathode material, characterized by wave vector q = 1/3(2a* – b*). We show that this can be enhanced through controlled heating. Comparative analysis LiNixCoyMnzO2 samples with different compositions revealed Mn ions are crucial for formation. The battery performance test shows has no obvious effect on voltage platform during charge–discharge cycle, but negative cycle and structural stability. elucidates origin detrimental effects superstructures, advancing understanding their impact performance, which is vital future development materials.

Язык: Английский

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Facilitating Sodium‐Ion Diffusion in Fe‐Doped Co₃O₄ for High‐Rate Performance

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 28, 2025

Due to its high theoretical capacity, cobalt oxide (Co3O4) has attracted attention sodium-ion battery (SIB) anodes. However, low conductivity and poor rate performance have limited practical application. This work proposes a co-precipitation doping strategy synthesize iron-doped Co3O4 nanoparticles (FexCo3-xO4 NPs). Both experimental results confirm that iron (Fe) at octahedral sites within spinel structures is critical factor in enhancing performance. The decreased bandgap enlarged ion transport spacing originate Fe doping. effectively facilitates the electron Na-ion (Na+) during discharge/charge processes, delivering an impressive capability of 402.9 mAh g-¹ 3 A g-¹. FexCo3-xO4 NPs demonstrate remarkable cycling stability. They maintain specific capacity 786.2 even after 500 cycles 0.5 g-¹, with no noticeable fading. When assembled into full cell, discharge 105 g-1 stable attained. provides valuable insights functional design high-rate electrodes, offering promising approach addressing challenges faced by sodium

Язык: Английский

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Surface Chemical Coordination Stabilizes Ni-Rich Cathodes for High-Energy Li-Metal Batteries

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 4, 2025

The stability of the electrode-electrolyte interface is a critical factor influencing electrochemical performance Li-metal batteries. However, on delithiated Ni-rich cathode surface, strong catalytic effects transition metals with coordination deficiency significantly aggravate parasitic reactions Li-metal-compatible ether-based electrolytes, thereby reducing cycling high-voltage Here, we propose an sp2-induction mechanism to address through coupling interfacial orbitals between molecules and surface. Sp2-hybrid high-fluorinated olefins, characterized by unsaturated bonds, exhibit highly delocalized electronic properties (electron delocalization index >0.95 au) elevated anodic (ionization potential >10 eV). These characters ensure robust stable interactions cathode, facilitating formation induced orbitals. low-energy accommodate Ni 3d electrons, effectively mitigating inhibiting surface side reactions. Among sp2-hybrid (perfluorobutyl)ethylene (PFBE) identified as optimal inducing molecule due its strongest interaction excellent complementarity PFBE-based electrolyte alleviates degradation structure demonstrates remarkable cyclic stability, achieving 80% capacity retention over 320 cycles for 4.4 V Li||LiNi0.8Mn0.1Co0.1O2 (30 μm Li, high load 3.7 mAh cm-2 NMC811) full cell, compared 175 PFBE-absent electrolyte. This work elucidates passivating high-catalytic interface, paving way durable, high-energy aggressive

Язык: Английский

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Formulation principles and synergistic effects of high-voltage electrolytes

Chemical Society Reviews, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

The energy density of lithium-ion batteries (LIBs) is primarily determined by the working potential devices and specific capacity cathode compounds. Carbonate-based electrolytes have received considerable attention due to their significance for advancing current cell-assembly process. However, commercially available liquid LiPF6 based cannot withstand harsh high-voltage environment effects cathode, issues such as undesired oxidative decomposition ethylene carbonate (EC), catalytic influence dissolved transition metal ions (TMs), poor performance interphases with unstable morphologies components. Furthermore, complex mechanisms (HVEs) are not fully understood. This review presents a comprehensive summary HVEs, including physical properties, solvation structures, interface chemistry. Specifically, chemical compounds failure commercial investigated, followed discussion expected functions HVEs. Then, screening criteria single-component electrolytes, considering oxidation resistance mechanism, mechanism interphase species explored on level positions. Next, cross-scale evolution framework proposed, from structure characteristics, aimed at uncovering formulation principles synergistic Operational systematically scrutinized, starting conventional tuning incorporation multiple components further role entropy-driven effects, all which will favor understanding effects. Finally, integration advanced computational methods mature experimental techniques foster development novel perspectives promising electrolyte candidates.

Язык: Английский

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A functional slurry additive for robust interphase and stabilized high-voltage nickel-rich cathodes in lithium-ion batteries

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 161446 - 161446

Опубликована: Март 1, 2025

Язык: Английский

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