Activation of MOF Catalysts with Low Steric Hindrance via Undercoordination Chemistry for Efficient Polysulfide Conversion in Lithium–Sulfur Battery

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

Published: July 3, 2024

Abstract Lithium–sulfur (Li–S) batteries promise high theoretical energy density and cost‐effectiveness but grapple with challenges like the polysulfide shuttle effect sluggish kinetics. Metal–organic framework (MOF) catalysts emerge as a leading solution, despite limited conductivity steric hindrance. This study employs undercoordination chemistry to modify Zn–Co bimetallic MOFs (D‐ZIF L), removing organic ligands from active centers. process mitigates spatial hindrance, thereby promoting comprehensive contact between sulfur species metal centers, consequently enhancing catalytic efficiency of MOFs. Moreover, treatment centers induces electron redistribution, augmenting at Fermi level elements, ameliorating intrinsic conductivity. Leveraging these advantages, fabricated Li–S employing D‐ZIF L exhibited markedly mitigated shuttling effects accelerated conversion Notably, substantial reverse areal capacity 5.0 mAh cm⁻ 2 is achieved after 100 cycles an evaluated loading 5.5 mg . Furthermore, practical pouch cell demonstrated initial 1.8 Ah 85.8 mA stable cycling for 50 cycles. underscores potential in development highly conductive MOF minimized advancing prospects battery technology.

Language: Английский

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Lattice Strain and Charge Localization Dual Regulation of Phosphorus‐Doped CoSe₂/MXene Catalysts Enable Kinetics‐Enhanced and Dendrite‐Free Lithium‐Sulfur Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(38)

Published: June 21, 2024

Abstract Phase engineering is considered an effective strategy to regulate the electrocatalytic activity of catalysts for Li–S batteries (LSBs). However, underlying origin phase‐dependent catalytic ability remains be determined, which significantly impedes design principles high‐performance materials LSBs. Herein, heteroatom‐doped can trigger phase transformation from mixed‐phased cubic and orthorhombic cobalt diselenide into pure structure with a tensile strain enhanced charge localization. The upshift d ‐band center Bader at Se sites synergistically strengthen interaction Li S in polysulfide species, thus endowing transformed P‐MoSe 2 /MXene high uniform lithium deposition Consequently, P‐CoSe demonstrate high‐rate capability 603 mAh g −1 4C, excellent cyclability 652 1C over 500 cycles degradation rate 0.076% per cycle. work provides in‐depth insight fundamental

Language: Английский

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Clustering Bimetallic M–N–C Catalyst: A Synergistic Approach to Advancing Sulfur Conversion Kinetics for High‐Performance Lithium‐Sulfur Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(31)

Published: July 3, 2024

Abstract Lithium–sulfur (Li–S) batteries stand out as a promising candidate for future energy storage, characterized by their notable density and affordability. However, the impediments raised polysulfide shuttling sluggish reaction kinetics pose substantial challenges to widespread implementation of this technology. Herein, unique Fe–Co bimetallic single‐atom‐cluster catalyst (FeCo‐SACC) Li–S are developed. The synergistic integration single atoms clusters guarantees not only commendable specific catalytic activity but also high metal loading up 25 wt%. Meanwhile, intermetallic interactions regulate electronic structure, enabling higher sulfur affinity faster conversion kinetics. 3D‐ordered mesoporous (3DOM) carbon architecture further affords conducive accommodation, efficient active site exposure, facile ion/mass transfer. As result, stable electrochemistry is realized, contributing excellent cyclability over 1000 cycles rate capability 5 C. Decent cell performances can still be achievable under practical criteria, e.g., 15 mg cm −2 , lean electrolyte 4.6 µL −1 1.91‐Ah pouch configuration. This work establishes novel paradigm development advanced electrocatalysts high‐performance batteries.

Language: Английский

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Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 1, 2024

Language: Английский

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Modification of polypropylene separator with nickel and manganese oxide-decorated carbon nanotubes toward high-performance lithium-sulfur batteries

Journal of Power Sources, Journal Year: 2025, Volume and Issue: 633, P. 236353 - 236353

Published: Feb. 5, 2025

Language: Английский

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Synergistic Adsorption-Catalysis Co/Mo-based Heterostructures for Enhanced Lithium Polysulfides Conversion in High-Rate Lithium-Sulfur Batteries

Electrochimica Acta, Journal Year: 2025, Volume and Issue: unknown, P. 145830 - 145830

Published: Feb. 1, 2025

Language: Английский

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Bimetallic Metal–Organic Framework Catalyst to Accelerate Sulfur Conversion Kinetics for High-Performance Lithium–Sulfur Batteries

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 20, 2025

Lithium-sulfur (Li-S) batteries are highly attractive due to their exceptional theoretical energy density (2600 Wh kg-1) and low cost. However, practical deployment is limited by critical issues, including pronounced polysulfide shuttling slow reaction kinetics. In this study, we report the development of a novel Mo-Zn bimetallic ZIF-8 catalyst designed address these issues. Compared with pristine ZIF-8, Mo-ZIF-8 exhibited an effectively tuned surface area pore structure, significantly enhancing its ability trap polysulfides. Moreover, optimized architecture increased exposure active sites, strengthening chemical interactions between sulfur species thereby accelerating The incorporation Mo also induced redistribution electronic structure around Zn boosting intrinsic conductivity reducing electrochemical diffusion resistance during redox processes. synergistic design sites further enhanced adsorption lithium polysulfides catalytic conversion species. As result, Li-S Mo-ZIF-8-modified separators exhibit minimal capacity decay (0.04% per cycle) over 1000 cycles at 1C. Under high loading 5.8 mg cm-2, they achieve areal mAh retaining 5.0 cm-2 after 100 cycles. These findings highlight potential metal-organic framework (MOF) catalysts in advancing battery performance.

Language: Английский

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Sieving effect integration with asymmetrically coordinated catalytic chemistry Realize optimized polysulfide regulation in Lithium-Sulfur batteries

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161182 - 161182

Published: March 1, 2025

Language: 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, Journal Year: 2025, Volume and Issue: unknown

Published: March 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.

Language: Английский

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Alloying Strategy Balances the Adsorption‐Reduction‐Oxidation Process of Sulfur Species Across Wide Temperature Ranges

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 28, 2025

Abstract Transition metal‐based catalysts have been demonstrated to effectively anchor and utilize lithium polysulfides (LiPSs), thereby enhancing the capacity of lithium‐sulfur batteries (LSBs). However, immobilized d ‐band electronic structure a single transition metal is inadequate for achieving satisfactory adsorption catalytic conversion. In this study, an alloying strategy employed modulate with aim optimal LiPSs. For purpose, cobalt (Co)‐nickel (Ni) encapsulated in nitrogen‐doped carbon nanotubes as bimetallic (CoNi/NCNT) are synthesized. The theory calculations experimental analysis demonstrate that by hybridizing ‐orbitals Co Ni, CoNi modulated be at central position. This configuration leads moderate detachment LiPSs on surface catalysts, balancing “adsorption‐reduction‐oxidation” process sulfur (S) species. Therefore, LSBs CoNi/NCNT separator able achieve good cycling room temperature (capacity decay rate 0.086% after 500 cycles 0.5 C). modified can excellent performance across wide range 0.057% 100 0 °C, 0.34% 60 °C).

Language: Английский

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