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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Fundamentals, Status and Promise of Li‐Rich Layered Oxides for Energy‐Dense Li‐Ion Batteries

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 17, 2025

Abstract Li‐ion batteries (LIBs) are the dominant electrochemical energy storage devices in global society, which cathode materials key components. As a requirement for higher energy‐dense LIBs, Li‐rich layered oxides (LLO) cathodes that can provide specific capacity urgently needed. However, LLO still face several significant challenges before bringing these to market. In this Review, fundamental understanding of is described, with focus on physical structure‐electrochemical property relationships. Specifically, various strategies toward reversible anionic redox discussed, highlighting approaches take basic structure battery into account. addition, application all‐solid‐state and consider prospects assessed.

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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Noninvasive rejuvenation strategy of nickel-rich layered positive electrode for Li-ion battery through magneto-electrochemical synergistic activation

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Ноя. 26, 2024

Nickel-rich layered oxides are one of the most promising positive electrode active materials for high-energy Li-ion batteries. Unfortunately, practical performance is inevitably circumscribed by structural deterioration deriving from Ni/Li antisite disorder, leading to severe capacity loss and life attenuation. Herein, we propose an economical facile rejuvenation strategy employing magneto-electrochemical synergistic activation targeting in assembled This approach induces a transition Ni3+ high-spin low-spin, reducing super-exchange interaction Ni-O-transition metal (TM). Meanwhile, electrochemical reaction drives Li+ host material promotes reoccupy TM layer, recovering intrinsic Li site extending cycle life. The demonstrates that low-quality electrodes can be converted high-quality ones. Notably, method revitalize aged pouch cell (SiC||NCM811, 8 Ah nominal capacity) via optimizing cation occupancy increase its 10% 6.49 7.14 at 1 C, illustrating benefits upcycling process. Severe disorder nickel-rich leads degradation decay Here, authors report noninvasive magnetoelectrochemical realize ordered rearrangement recovery battery capacity.

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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In Situ Surficial Polymerization of Ultrahigh-Nickel Cathode Material for Stable Solid-State Lithium Batteries

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Апрель 1, 2025

Ultrahigh-nickel cathode active materials (CAMs) suffer from detrimental side reactions when coupled with poly(ethylene oxide) (PEO)-based electrolytes in solid-state lithium-metal batteries (SLMBs). To circumvent this issue, here we propose a surface modification strategy for ultrahigh-nickel CAMs self-assembled nanoscale polymer coating. Without requiring additional initiators, the residual lithium compounds inherent on of are used as initiators to induce situ anionic polymerization monomer. Meanwhile, oxygen vacancies generated through coordination -C = O and ≡ N transition metal ions, which reduces diffusion barrier Li+ their vicinity. Benefiting high voltage stability, rapid transfer, elasticity coating layer, coated LiNi0.9Co0.06Mn0.04O2 exhibits capacity retention 92% after 100 cycles matched PEO-based electrolytes. The pouch cell enables stable operation 500 at 1C. In addition, measure MW recycled PEO cycling by gel permeation chromatography, is direct evidence that decomposition (cleavage ether linkages) inhibited. As vision, efficient, high-yield, simple method expected promote commercial application SLMBs.

Язык: Английский

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Oxygen Vacancy Engineering for High-Performance Li-Rich Manganese Cathodes: Advances and Prospects

Energy storage materials, Год журнала: 2025, Номер unknown, С. 104321 - 104321

Опубликована: Май 1, 2025

Язык: Английский

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Enhanced Electrochemical Stability of Sulfide Electrolytes with Surface Modification for High‐Performance LiNiO₂ Based All‐Solid‐State Lithium Batteries

Small, Год журнала: 2025, Номер unknown

Опубликована: Май 24, 2025

Abstract All‐solid‐state lithium batteries (ASSLBs) equipped with layered Ni‐rich cathodes hold great promise for achieving high‐specific energy and enhanced safety. Although LiNiO 2 (LNO) cathode theoretically offers superior specific capacity (≈275 mAh g −1 ) cost efficiency, its practical application in ASSLBs is hindered by significant interfacial incompatibility solid electrolytes, resulting parasitic side reactions sluggish charge transport, particularly under high‐voltage operation. Here, a facile ball‐milling strategy presented to engineer an situ protective layer on Li 5.5 PS 4.5 Cl 1.5 (LPSC) through spontaneous chemical reaction SO 4 , which effectively mitigates electrochemical instability. This modified electrolyte enables LNO achieve record‐high discharge of 231.3 at 0.2 C 45 °C, alongside remarkable cycling stability (95% retention after 200 cycles 4.4 V). Additionally, even ultra‐high voltage 4.6 V, the battery can still retain 95% over 140 cycles. Multimodal spectroscopic analyses confirm that designed coating suppresses decomposition while maintaining rapid Li⁺ transport. work establishes scalable, cost‐effective approach engineering, unlocking potential LNO‐based applications.

Язык: Английский

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