Chip-Inspired Design of High-Performance Lithium–Sulfur Batteries by Integrating Monodisperse Sulfur Nanoreactors on Graphene

ACS Nano, Journal Year: 2024, Volume and Issue: 18(24), P. 15638 - 15650

Published: June 7, 2024

For practical application of lithium–sulfur batteries (LSBs), designing devices with an overall optimal structure instead modifying electrode materials is significant. Herein, we report a chip-inspired design vertically integrated as LSB cathode by implanting Mo2C nanoparticles and nanosulfur into the reduced graphene oxide (rGO) matrix. This configuration enabled synthesis isolated sulfur nanoreactors (S-NRs) in tandem array on rGO, generating chip-like LSBs. The spatial confinement/protection concentration gradient S-NRs effectively avoided dissolution, diffusion, loss polysulfides, thereby enhancing utilization redox reaction kinetics. Additionally, adaptive storage energy can be improved utilizing tandem, isolation, synergistic multiplicative effect among nanoreactor units. As result, obtained excellent electrochemical performances initial capacity 1392 mAh g–1 at 0.1C, low decay rate 0.017% per cycle during 1500 cycles operation 0.5C, superior performance. work provides rational idea method further advancing precise preparation high-performance devices.

Language: Английский

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Physical Field Effects to Suppress Polysulfide Shuttling in Lithium–Sulfur Battery

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

Published: Oct. 14, 2024

Lithium-sulfur batteries (LSB) with high theoretical energy density are plagued by the infamous shuttle effect of lithium polysulfide (LPS) and sluggish sulfur reduction/evolution reaction. Extensive research is conducted on how to suppress effects, including physical structure confinement engineering, chemical adsorption strategy, design redox catalysts. Recently, rational mitigate effects enhance reaction kinetics based field has been widely studied, providing a more fundamental understanding interactions species. Herein, focused their methods mechanisms interaction summarized systematically LPS. Overall, working principle LSB system, origin effect, kinetic trouble in briefly described. Then, mechanism application materials concepts external field-assisted elaborated, electrostatic force, built-in electric field, spin state regulation, strain magnetic photoassisted other strategies pivotally elaborated discussed. Finally, potential directions enhancing performance weakening high-energy anticipated.

Language: Английский

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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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Ultralight Hierarchical Fe₃O₄/MoS₂/rGO/Ti₃C₂T_x MXene Composite Aerogels for High-Efficiency Electromagnetic Wave Absorption

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(28), P. 36962 - 36972

Published: July 3, 2024

Aerogel-based composites, renowned for their three-dimensional (3D) network architecture, are gaining increasing attention as lightweight electromagnetic (EM) wave absorbers. However, attaining high reflection loss, broad effective absorption bandwidth (EAB), and ultrathin thickness concurrently presents a formidable challenge, owing to the stringent demands precise structural regulation incorporation of magnetic/dielectric multicomponents with synergistic loss mechanisms within 3D networks. In this study, we successfully synthesized hierarchical porous Fe

Language: Английский

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Built-in electric field in NiO-CuO heterostructures to regulate the hydroxide adsorption sites for 5-hydroxymethylfurfural electrooxidation assisted hydrogen production

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 673, P. 301 - 311

Published: May 31, 2024

Language: Английский

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Dependence of Interlayer or Sulfur Host on Hollow Framework of Lithium–Sulfur Battery

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 19, 2024

Abstract Lithium–sulfur batteries are recognized as the next generation of high‐specific energy secondary owing to their satisfactory theoretical specific capacity and density. However, commercial application is greatly limited by a series problems, including disordered migration behavior, sluggish redox kinetics, serious shuttle effect lithium polysulfides. One most efficient approaches physically limit rational design hollow framework sulfur host. influence structure on interlayers has not been clearly reported. In this study, Mo 2 C/C catalysts with hollow(H‐Mo C/C) solid(S‐Mo frameworks rationally designed explore dependence interlayer or contrast physical limitations host, inhibited lithium‐ion diffusion, resulting in poor electrochemical properties at high current densities. Based superiority various frameworks, H‐Mo C/C@S | S‐Mo C/C@PP Li cells assembled displayed excellent performance. This work re‐examines requirements principles catalyst different battery units.

Language: Английский

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A Lithium‐Affinitive Covalent Organic Polymer Network Functionalized Separator for Dendrite‐Free and High‐Durability Lithium–Sulfur Batteries under Harsh Conditions

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(37)

Published: May 7, 2024

Abstract Lithium–Sulfur (Li─S) batteries are renowned for their high theoretical specific capacity and cost‐effectiveness. Nevertheless, performance could be impeded by obstacles including lithium dendrite growth polysulfide (LiPS) shuttle, particularly under harsh conditions. Herein, an economical strategy is reported modifying polyolefin separators (PP) with covalent organic polymer networks (TPE) to alter Li solvent structure, enhance lithium‐ion transport, suppress shuttle effects. Combining in situ/ex situ characterization calculations, it demonstrated that the lithiophilic groups (‐C═N‐) TPE@PP separator form strong interaction lithium, facilitating dissociation of Li─Solvent/LiPS‐solvent release freer ion shape a stable solid electrolyte interface rich LiF 3 N. The network serves as “highway” accelerates transport promotes uniform nucleation behavior. Therefore, Li|TPE@PP|CNT/S cell enables 60% retention after 2000 cycles at 1.0 C exhibits cycling 100 from ‐40 80 °C. Moreover, pouch maintains more than 600 mA h g −1 30 0 This study provides promising avenue application high‐performance environment perspective engineering.

Language: Английский

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Integrated Design for Discrete Sulfur@Polymer Nanoreactor with Tandem Connection as Lithium–Sulfur Battery Cathodes

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(31)

Published: May 23, 2024

Abstract Apart from electrode material modification, architecture design and optimization are important approaches for improving lithium–sulfur battery performance. Herein, an integrated structure with tandem connection is constructed by confining nanosulfur (NS) in conductive poly(3,4‐ethylenedioxythiophene) (PEDOT) reaction chambers, forming interface of discrete independent nanoreactor units bonded onto carbon nanotubes (noted as CNT/NS@PEDOT). The unique spatial confinement concentration gradients sulfur@PEDOT nanoreactors (SP‐NRs) can promote kinetics while facilitating rapid polysulfide transformation minimizing dissolution diffusion losses. Meanwhile, overall ultrahigh energy input output achieved through nanotubes, isolation PEDOT coating, synergistic multiplicative effects among SP‐NRs. As a result, it delivers high initial discharge capacity 1246 mAh g −1 at 0.1 C 918 1 C, the low decay rate per lap 0.011 % current density after 1000 cycles. This research emphasizes innovative structural to provide fresh trajectory further advancement high‐performance storage devices.

Language: Английский

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Surface functionalization of PS/PEI-derived hierarchical porous carbons doped with nitrogen and oxygen using melamine activation for supercapacitors

Surfaces and Interfaces, Journal Year: 2024, Volume and Issue: 51, P. 104531 - 104531

Published: May 29, 2024

Language: Английский

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Achieving a smooth “adsorption-diffusion-conversion” of polysulfides enabled by MnO2-ZnS p-n heterojunction for Li-S battery

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 666, P. 322 - 330

Published: April 2, 2024

Language: Английский

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