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

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(49)

Published: Aug. 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.

Language: Английский

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Regional Electron Delocalization Regulation Internalizes the Reduced‐Order‐Transformation of Polysulfides

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 15, 2024

Abstract The step‐order or disproportionation conversion of lithium polysulfides (LiPSs) is still a blind box in LiS batteries (LSBs) system. cation‐doped electrocatalyst (Fe‐CoS 2 @HCNF) designed through modulating electron‐surrounding situation the central atomic d‐band to promote regional electron‐directed LiPSs reduced‐order‐transformation (especially, Li S 4 S). Fe‐CoS @HCNF satisfies requirement mass (electron/ion) transfer reaction, quantizing as multi‐osmosis‐connected transportation channels and an all‐encompassing interior space for sulfur reduction occurring. Based on experiments DFT calculations, introduced Fe presents local electron deficiency state toward regulating delocalization between Co matrix, which induces metal site, strengthening 3d orbital coupling interaction with 2− LiPSs, further guiding order‐transformation intermediate LiPSs. Consequently, electrode has excellent electrochemical properties, performing at 3.0 C 0.064 % capacity decay per cycle, even maintaining super cycle stability high loadings. In addition, pouch cell assembled can also reach initial specific 1070.3 mAh g −1 0.1 C, show good long‐term stability. This work provides valuable prospect analyzing SRR by flow regulation practical LSBs.

Language: Английский

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Steering sulfur reduction kinetics of lithium-sulfur batteries by interfacial microenvironment modulation

Energy storage materials, Journal Year: 2024, Volume and Issue: 71, P. 103622 - 103622

Published: July 4, 2024

Language: Английский

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Enhancing Li-S Battery Performance by Harnessing the Power of Single Atoms on 2D Borophene

Electrochimica Acta, Journal Year: 2025, Volume and Issue: unknown, P. 145831 - 145831

Published: Feb. 1, 2025

Language: Английский

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Boosting Polysulfide Conversion on Fe‐Doped Nickel Diselenide Toward Robust Lithium–Sulfur Batteries

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 17, 2025

Abstract Sulfur offers a high‐energy‐density, low‐cost, and sustainable alternative to traditional battery cathodes, but its practical use is limited by sluggish uneven reaction polysulfide dissolution, necessitating electrocatalytic additives enhance conversion efficiency. Generating unpaired spin electrons has proven effective in enhancing performance Co‐based electrocatalysts. These increase adsorption weakening S─S bonds, facilitating their cleavage during sulfur reduction reactions. This work extends the strategy Fe–Ni‐based catalysts. The synthesis of NiSe 2 Fe‐doped particles reported investigate impact Fe doping on electronic structure, catalytic activity, introduced as coating cathode side Li–S (LSB) separator. Experimental analyses first‐principles calculations reveal that Fe‐rich cores surface density states at Fermi level introduce electrons, boosting LiPS conversion. synergistic effects significantly improve performance, cycling stability, overall LSB cells. Specifically, cells based ‐based separators achieve specific capacities 1483 mAh g⁻¹ 0.1C 1085 1C, along with remarkable retaining 84.4% capacity after 800 cycles. High sulfur‐loading tests further validate multifunctional membrane's effectiveness, showing significant retention reduced loss.

Language: Английский

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First-principles study of sulfur-host materials utilizing single-atom catalysts embedded within g-C3N4

Surfaces and Interfaces, Journal Year: 2024, Volume and Issue: 48, P. 104315 - 104315

Published: April 15, 2024

Language: Английский

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Addressing adsorption and catalysis of lithium polysulfide via electronic distribution of molybdenum carbide host

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 669, P. 466 - 476

Published: April 26, 2024

Language: Английский

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Peripheral group-induced spin-state switch of metal macrocyclic molecule for enhanced redox kinetics in lithium-sulfur batteries

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 491, P. 151990 - 151990

Published: May 10, 2024

Language: Английский

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Selenide in 3D structure of polyhedra branching out nanotubes for collaborative facilitated conversion and capturing of polysulfide in Li–S batteries

Rare Metals, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 23, 2024

Language: Английский

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Yolk Double-Shell Cathode for Encapsulating Polysulfides and Initialing Redox Kinetics toward High-Performance Lithium–Sulfur Batteries

Industrial & Engineering Chemistry Research, Journal Year: 2024, Volume and Issue: 63(28), P. 12468 - 12478

Published: July 7, 2024

Lithium–sulfur batteries (LSBs) sustain a series of serious challenges, such as unreasonable cathode configuration, unsatisfactory mass transfer kinetics, disgusting lithium polysulfide (LiPSs) shuttle escape, and so on, which have obstructed the further exploration commercialization process. In this study, "yolk double-shell" structure materials Fe3O4@FeP@C accommodates active sulfur guides unobstructed transformation intermediates, state-of-art-shaped yolk double-shell architecture prevents LiPSs from escaping into electrolyte, meanwhile, doped-N substances enhance chemisorption LiPSs, promoting transfer-reaction kinetics. Based on above advantages, excellent electrochemical performances been obtained, S/yolk–shells-2 exhibits an initial specific capacity 1250.38 mAh g–1 at 0.5 C, maintaining 368.39 2.0 C for 1000 stable cycles, discharging capacities keep 549.25 454.99 after 250 cycles 4.0 5.0 respectively. Surprisingly, displays high 1014.79 ultrahigh loading 6.23 mg cm–2. The study elaborately designed fabricated host encapsulating accelerating reactions toward high-performance LSBs.

Language: Английский

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