Constructing Iron Vacancies in Thiospinel FeIn₂S₄ to Modulate Fe D‐Band Center and Accelerate Sodiation Kinetics Enabling High‐Rate and Durable Sodium Storage

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract The bimetallic synergies effect and combined conversion/alloying mechanism endow thiospinel FeIn 2 S 4 with great potential as an anode material for sodium‐ion batteries (SIBs). However, their inconsistent synthesis, severe volumetric expansion, sluggish reaction kinetics typically lead to unsatisfactory cyclic stability rate capability. Herein, organic framework derived @N/S‐C microrods Fe vacancies is presented fast, durable, reversible sodium storage. presence of significantly modulates the d ‐band center decreases strength Fe─S bond facilitating sodiation jointly. Moreover, a thin stable solid electrolyte interface film inorganic‐rich components formed by induction. Combined N, co‐doped porous carbon matrix, optimal sample delivers excellent capability 381 mAh g −1 at 10 A performance (448 after 500 cycles 1 ). Furthermore, assembled full‐cells also exhibit superior electrochemical 87.5% capacity retention long‐term evaluations. This work presents promising strategy structural regulation sulfides advanced anodes SIBs.

Язык: Английский

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Advanced Cathode Designs for High‐Energy Lithium/Sodium–Selenium Battery

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 28, 2025

Abstract Selenium, with its superior conductivity, serves as a promising cathode material in lithium–selenium (Li–Se) and sodium–selenium (Na–Se) batteries, exhibiting faster electron transfer processes volumetric capacity. Nonetheless, challenges such volume expansion, the shuttle effect, slow redox reaction kinetics, low conductivity of discharged products still hinder their commercial application. Extensive research has been conducted on design optimization materials to overcome these issues. This review summarizes latest advancements Se within Li/Na–Se systems, based electrochemical mechanisms batteries origins related challenges. The comprehensive principle advanced stable selenium cathodes is put forward, key role carbon structure analyzed, strategies improve affinity selenide kinetics are discussed. Additionally, it introduces representative polymer‐based metal–organic framework (MOF)‐based cathodes. Some potential modification for active also highlighted, including sulfide composite lithium cathodes, which can significantly enhance Se‐based batteries. Finally, existing research, insights directions future development proposed.

Язык: Английский

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Coupling Bifunctional Scaffolds with Slow Photon Effect for Synergistically Enhanced Photoassisted Lithium–Sulfur Battery Properties

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Янв. 25, 2025

Photoassisted lithium-sulfur (Li-S) batteries offer a promising approach to enhance the catalytic transformation kinetics of polysulfide. However, development is greatly hindered by inadequate photo absorption and severe photoexcited carriers recombination. Herein, photonic crystal sulfide heterojunction structure designed as bifunctional electrode scaffold for photoassisted Li-S batteries. Inverse opal (IO) structures utilize slow photon effect that originates from their adjustable band gaps, giving them distinctive optical response characteristics. The incorporation SnS/ZnS within these IO frameworks further broadens light spectrum enhances charge transfer process. This efficient hybrid not only adsorption conversion polysulfides at cathode but also induces uniform Li nucleation anode. These contribute full output high reversible capability 1072 mAh g-1 maintain stable cycling 50 cycles. Additionally, specific capacity 698.8 still obtained even under sulfur loading up 4 mg cm-2. present strategy on battery properties can be extended rationally construct other energy storage devices.

Язык: Английский

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A Review of Advances in Heterostructured Catalysts for Li–S Batteries: Structural Design and Mechanism Analysis

Small, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 15, 2024

Lithium-sulfur (Li-S) batteries, acclaimed for their high energy density, cost-effectiveness, and environmental benefits, are widely considered as a leading candidate the next-generation storage systems. However, commercialization is impeded by critical challenges, such shuttle effect of lithium polysulfides sluggish reaction kinetics. These issues can be effectively mitigated through design heterojunction catalysts. Despite remarkable advancements in this field, comprehensive elucidation underlying mechanisms structure-performance relationships catalysts sulfur electrocatalysis systems remains conspicuously absent. Here, it expounded upon heterostructure engineering Li-S batteries latest guided these multifarious examined. Furthermore, illuminates groundbreaking paradigms design, encompassing realms composition, structure, function, application. Finally, research trends future development directions novel materials extensively deliberated. This study not only provides profound understanding but also facilitates exploration new electrocatalyst

Язык: Английский

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Activating Transition-Metal Oxides through In Situ Regulation of Lower Hubbard Band for Catalytic Conversion of Lithium Polysulfides

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Апрель 30, 2025

Catalytic conversion of lithium polysulfides (LiPSs) is regarded as an effective avenue to tackle the shuttle effect lithium-sulfur (Li-S) batteries, especially based upon transition-metal oxides (TMOs). However, activity origin and corresponding mechanistic insights into such catalytic systems remain elusive. Herein, activated state associated with lower Hubbard band (LHB) transition proposed elucidate TMOs by taking Mn3O4 a model electrocatalyst. Specifically, broadening LHB width, upshift position, orbital rearrangement LHB, triggered in situ substitution O atoms S LiPSs under working conditions, synergistically enable fast electron transfer modulate adsorption capability moderate level. Benefiting from these advantages, electrocatalyst converted torpid for expediting LiPS conversion. Eventually, Li-S batteries assembled deliver excellent rate performance over 6 C outstanding cycling stability 1000 cycles. Moreover, Ah-scale pouch cell constructed delivers notable energy density 388.1 W h kg-1. Our work offers promising pathway on regulation designing high-performance electrocatalysts beyond.

Язык: Английский

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High Spin‐State Modulation of Catalytic Centers by Weak Ligand Field for Promoting Sulfur Redox Reaction in Lithium‐Sulfur Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 8, 2024

The spin state of transition-metal compounds in lithium-sulfur batteries (LSBs) significantly impacts the electronic properties and kinetics sulfur redox reactions (SRR). However, accurately designing remains challenging, which is crucial for understanding structure-performance relationship developing high-performance electrocatalysts. Herein, CoF

Язык: Английский

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Engineering Bi/V/Mo‐Based Multicomponent Heterostructure Electrocatalyst Toward Robust Lithium–Sulfur Batteries and Mechanistic Insights into the Self‐Reconstruction

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 13, 2025

Abstract The sluggish reaction kinetics and formidable shuttle effect of soluble lithium polysulfides (LiPSs) are thorny problems for the future industrialization lithium–sulfur (Li–S) batteries. Therefore, exploring efficient electrocatalysts to capture LiPSs accelerate their conversion is highly desirable yet tremendously challenging. Herein, a high‐efficiency Bi/Bi 2 O 3 /VMoN@rGO electrocatalyst with multifunctional active sites multilevel heterointerfaces elaborately designed Li–S Noteworthy, can greatly modulate electron distribution, facilitate charge transfer, optimize chemical absorption, enhance intrinsic activity, while rGO contributes high electrical conductivity, sufficient sites, robust structural stability. Thanks synergy different components, batteries employing functional separators exhibit impressive electrochemical performance sulfur utilization even under loading. More importantly, it discovered that Bi experience an phase evolution generate S amorphous crystalline phases, thereby bringing in unexpected enhancement. Furthermore, experimental results theoretical calculations authenticate reduced Li decomposition energy barrier achieved after situ reconstruction. This work not only provides new mechanistic insights into developing but also sheds light on regulating catalytic activity via self‐reconstruction.

Язык: Английский

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Selective Adsorption-Catalysis Sites of Lithium Polysulfides Induced by the Competition between Spin Polarization and Electronegativity in High-Entropy Alloy Electrocatalysts

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Март 18, 2025

High-entropy alloy (HEA) electrocatalysts have attracted increasing attention for improving sulfur reaction kinetics and anchoring lithium polysulfides (LiPSs) in lithium-sulfur batteries (LSBs). However, fundamentally understanding the relationship between components of HEAs adsorption catalysis LiPSs remains a challenge. Here, FeCoNiMnRu are employed as model to first disclose selective adsorption-catalysis effect LiPSs, induced by competition spin polarization electronegativity Ni−Co−Ru sites HEAs. By correlating electron structure, we find that high-electronegativity Ru induce transfer from Co sites, generating local delocalization, while Ni adopt high-spin state. Specifically, with stronger Ni−S covalency can sustainably anchor electron-delocalized Co−Ru function better LiPS conversion. Consequently, benefiting LSBs FeCoNiMnRu/CNF interlayers deliver exceptional cycling performance (0.06% per cycle over 500 cycles at 1 C, an outstanding areal capacity 11.2 mAh cm−2 0.1 C). This work offers key insights extending enable high-performance LSBs.

Язык: Английский

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Expanded Nanofibrous Cellulose Electrode Binder: Declustering Lithium Polysulfides for Lean‐Electrolyte Li‒S Batteries

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 7, 2025

Abstract Despite their potential as an alternative to commercial lithium (Li)‒ion batteries, Li–sulfur (Li–S) batteries face challenges related energy density limitations caused by the considerable amount of electrolyte required. Lean electrolytes have proven effective in mitigating this issue. However, they tend exacerbate Li polysulfides (LiPS) clustering, resulting incomplete S utilization and sluggish conversion kinetics. Here, 2,2,6,6‐tetramethylpiperidin‐1‐oxyl radical (TEMPO)‐oxidized cellulose nanofiber (TOCN) is presented expanded nanofibrous electrode binder for lean‐electrolyte Li‒S batteries. Owing its 1D fibrous structure inter‐glucose chain distance, TOCN offers more accessible active sites intermolecular interactions with LiPS. Consequently, LiPS cluster formation effectively suppressed even at a low content 1 wt%, while high loading 72 wt% achieved. The cathode enables cells exhibit remarkable specific capacity 1221 mAh g sulfur −1 under constrained conditions (low electrolyte‐to‐sulfur ratio 2.0 µL mg 0.927 mL ), yielding cell‐level 503 Wh kg that surpasses those previously reported cathodes based on conventional synthetic polymer binders.

Язык: Английский

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Mo/VONC as a polysulfide immobilizer and catalyst to enhance performance of Lithium sulfur batteries

Journal of Electroanalytical Chemistry, Год журнала: 2025, Номер unknown, С. 119143 - 119143

Опубликована: Апрель 1, 2025

Язык: Английский

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