3d‐Orbital High‐Spin Configuration Driven From Electronic Modulation of Fe₃O₄/FeP Heterostructures Empowering Efficient Electrocatalyst for Lithium−Sulfur Batteries

Advanced Functional Materials, Год журнала: 2024, Номер 34(49)

Опубликована: Авг. 29, 2024

Abstract The intricate lithium polysulfides (LiPSs) shuttle and uncontrollable dendrite growth critically hinder the commercialization of lithium−sulfur (Li−S) batteries. rational orderly assignment multi‐electron induced flow is critical link in sulfer redox reaction. Herein, yolk‐shell Fe 3 O 4 /FeP@C heterostructure nanoreactors are fabricated to modulate electronic structure, including spin‐related charge behavior orbital orientation control, which can demonstrate interaction between catalytic activity spin‐state conformation. spin splitting induces electron transition from low‐spin high‐spin, where non‐degenerate orbitals contribute energy level up‐shift, guiding migration FeP , activating more states d orbitals. Spin polarization guides sulfur closed‐loop conversion, confirmed by DFT simulations situ Raman. Hence, electrochemical performances remarkable at ultra‐high current density loading. Even an initial specific capacity 928.5 mAh g −1 a Li−S pouch cell reveals practical prospect /FeP@C/PP separator. Li//Li symmetric cycles steadily for 4000 h, confirming interlayer simultaneously promotes evolution kinetics sieves ions. This work deciphers principles spin‐orbit coupling, achieving topological modulation “charge−spin−orbit” toward electrocatalysts.

Язык: Английский

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Homogenized Upcycling for Spent LiNi_0.5Co_0.2Mn_0.3O₂: Modulating O Vacancies toward Enhanced Structural Stability

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Fascinated by the high value and low pollution, direct recycling of spent LiNi 0.5 Co 0.2 Mn 0.3 O 2 (S‐NCM) has triggered plenty exploring activities. Considering different industry sources, they always display various particle sizes surface traits. Therefore, simple recovery chemical defects hardly meets market demand. Herein, homogenized strategy, containing physical crushing recovering, is introduced to regenerate morphology components S‐NCM, where successfully regenerated samples displayed uniform size stable lattice. Assisted crushing, precursors show a large contacting area with oxygen during reconstruction, accompanied effective repairing internal More significantly, unique manner induces vacancies (OVs) lowering Li/Ni disorder, bringing about enhanced structural stability. Moreover, redox activity improvement binding energy are further revealed theoretical calculations. The as‐optimized considerable capacity 139.6 mAh g −1 remarkable retention 94% at 1.0 C. Even 5.0 C, its could be kept ≈80.8% after 150 loops. Given this, this work expected provide guidance for NCM regenerations, meanwhile offering an in‐depth understanding morphology/lattice reconstruction.

Язык: Английский

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D‐Band Center Modulation of Fe‐Doping CoSe₂ to Accelerate Polysulfide Conversion for High‐Performance Lithium–Sulfur Battery

Advanced Sustainable Systems, Год журнала: 2025, Номер unknown

Опубликована: Март 20, 2025

Abstract As prospective energy storage devices surpass conventional lithium‐ion systems, lithium–sulfur batteries confront operational challenges, including polysulfide dissolution and slow redox dynamics. This work reports an iron doping methodology to engineer CoSe 2 ‐based electrocatalysts with optimized electronic configurations. The strategic introduction of dopants induces valence electron redistribution between metallic centers, systematically tuning the d‐orbital level alignment relative Fermi energy. Such modification substantially enhances phase transformation kinetics soluble LiPS intermediates insoluble Li S deposition. Hence, Fe(0.05)‐CoSe catalyst display more excellent cyclic lifespan, rate performance, specific capacities than those catalyst. It delivers initial discharge capacity 1473 mAh g −1 , 444 after 1000 cycles at 1.0C. provides efficient strategy accelerate conversion polysulfides on system.

Язык: Английский

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Win-win cooperation of boron-doped C3N5 porous nanosheets and CoSe2 nanorods for promoting cathodic sulfur conversion in lithium–sulfur batteries

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 161776 - 161776

Опубликована: Март 1, 2025

Язык: Английский

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Synergistic Promotion of Adsorption-Conversion for Lithium Polysulfides through Ion/Electron Coconductive Catalytic Triple-Phase Interface by the Geometric Torsion of Lithium Lanthanum Titanate Electrocatalyst

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

Опубликована: Март 27, 2025

Rationally designing and constructing ionic/electronic coconductor electrocatalysts with adjustable active sites to enhance the redox kinetics of lithium–sulfur batteries (LSBs) in lean electrolyte conditions is a challenge. Herein, this study presents promotion for lithium polysulfides (LiPSs) through construction ion/electron coconductive catalytic triple-phase interface using lanthanum titanate/carbon (LLTO/C) nanofibers, which due manipulating geometric torsion BO6 octahedron LLTO. Experiments theoretical calculations demonstrate that changes coordination environment O–Ti–O LLTO causes oxygen vacancy lattice distortion. This enhances local electronic state density, ion migration rate, high activity LLTO, thereby resulting synergistic effect good chemisorption rapid conversion LiPSs. Therefore, when modified separator used, LSBs electrocatalyst realize discharge capacity 1024 mA h·g–1 at current rate 2 C. Upon sulfur loading 9 mg ·cm–2 electrolyte/sulfur ratio 4 μL· mg–1, an acceptable areal 9.1 h· cm–2 achieved. work provides new perspective rational design catalysts LSBs.

Язык: Английский

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N, S Co-doped Carbon-Enhanced FeS2 Yolk–Shell Structure: Overcoming Volume Expansion and Polysulfide Shuttle Issues in Sodium-Ion Battery Anodes

Electrochimica Acta, Год журнала: 2025, Номер unknown, С. 146120 - 146120

Опубликована: Март 1, 2025

Язык: Английский

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A Keggin-type polyoxometalate/COF thin separator for improving the performance of lithium–sulfur batteries

Journal of Materials Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

POMs/DTQ-COF composites were prepared by post-synthesis strategy and applied to the improvement of lithium–sulfur battery separator. The electrochemical performance was effectively improved.

Язык: Английский

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Defect-Engineered Nico2s4-X Nanosheets on Hollow Carbon Spheres as Bifunctional Separator Coating for Long-Life Lithium–Sulfur Batteries

Опубликована: Янв. 1, 2025

Язык: Английский

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MoO₂–Stabilized MoS₂ Heterojunction Catalyst for Enhanced Lithium–Sulfur Battery

Industrial & Engineering Chemistry Research, Год журнала: 2025, Номер unknown

Опубликована: Апрель 23, 2025

Язык: Английский

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Spontaneous built-in electric field in W-W2C@C heterostructure: Accelerating Sn2- directed migration in Li-S batteries

Chemical Engineering Journal, Год журнала: 2024, Номер unknown, С. 156291 - 156291

Опубликована: Сен. 1, 2024

Язык: Английский

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