Strategically Engineered Metal Cluster–Rare Earth Oxide Heterojunction Catalyst for High-Performance Lean Electrolyte Lithium–Sulfur Batteries

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 11, 2025

Developing high-energy-density lithium–sulfur batteries faces serious polysulfide shuttle effects and sluggish conversion kinetics, often necessitating the excessive use of electrolytes, which in turn adversely affects battery performance. Our study introduces a meticulously designed electrocatalyst, Cu–CeO2–x@N/C, to enhance lean-electrolyte This catalyst, featuring situ synthesized Cu clusters, regulates oxygen vacancies CeO2 forms Cu–CeO2–x heterojunctions, thereby diminishing sulfur barriers hastening reaction kinetics through generation S32–/S3*– intermediates. Besides, three-dimensional conductive networks, composed nitrogen-doped carbon matrices with high electrolyte affinity, effectively confine sparse electrolytes proximal catalyst locations, facilitating rapid transport Li+/electron active sites. As result, 1% Cu–CeO2–x@N/C cell demonstrated robust performance, achieving an initial discharge capacity 793.2 mAh/g at 5 C over 500 cycles maintaining 719.9 0.3 electrolyte-to-sulfur ratio μL mg–1 loading 5.4 mg cm–2 after 60 cycles. These findings highlight design for high-performance batteries, further paving way their commercialization.

Language: Английский

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Lightweight Materials for High Energy Density Lithium–Sulfur Batteries

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

Published: Feb. 28, 2025

Abstract At present, electronic devices such as electric vehicles and mobile phones have increasing requirements for battery energy density. Lithium–sulfur batteries (LSBs) a high theoretical density are considered potential choice realizing the next generation of (2600 W h kg −1 ) batteries. However, actual LSBs is much lower than due to poor conductivity sulfur, serious LiPSs shuttle, low sulfur utilization, so on. Many lightweight materials characterized by surface area designability. The reasonable design modify can reduce proportion inactive substances optimizing electrochemical performance, which crucial improving LSBs. few reviews discuss effect on from perspective whole system. Herein, application in six aspects: liquid electrolyte, solid cathode, anode, separator, current collector discussed. significance use further improvement summarized prospected.

Language: Английский

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Axial Coordination Regulating Electronic Delocalization of p‐Block In−N₄ Sites to Accelerate Sulfur Reduction Reaction

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

Published: April 21, 2025

Abstract Modulating the electron delocalization of catalysts can improve activation and conversion capabilities lithium polysulfides (LiPSs) in lithium‐sulfur batteries, while precise mechanism underlying this enhancement remains unclear. Herein, a p‐block In single‐atom (In‐N 4 ) is constructed with moderate via axial coordination engineering gallium nitride (GaN), which exhibits best adsorption electrocatalytic activity toward LiPSs. situ characterization analysis combined advanced theoretical calculations demonstrate that In‐N‐Ga induces transfer from sites N GaN unconventional sp 3 d 2 hybridization interactions sites. This further helps to optimize configuration through orbital between hybrid p S atoms LiPSs, namely − hybridization, weaken S−S covalent bonds LiPSs significantly accelerate sulfur reduction reaction. Accordingly, capacity decay battery In−SA/GaN catalyst only 0.040% per cycle over 800 cycles at 5 C. The stacked pouch cell delivers reversible 600 mAh after 100 cycles. work elaborates on origin metal provides new perspective designing for other catalytic systems.

Language: Английский

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Catalysis‐Driven Sulfur Conversion: From Electrolyte‐Flooded to Solid‐State Batteries

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

Published: Feb. 14, 2025

Abstract Lithium‐sulfur (Li–S) batteries are widely recognized as highly promising energy storage devices owing to their exceptional theoretical density. However, the prevalent use of flooded electrolytes in Li–S significantly restricts To enhance density batteries, transitioning from a flooded‐electrolyte lean‐electrolyte system proves be effective. Additionally, replacing organic liquid electrolyte with solid‐state addresses associated safety concerns. Concurrently, practical application encounters numerous challenges, particularly sluggish electrochemical conversion kinetics and systems. Hence, it is imperative develop suitable catalysts tailored for various battery configurations. This review comprehensively reviews applications development strategies diverse systems, specific focus on outlook explores future direction catalysts, aiming guide rational design facilitate realization high‐energy‐density batteries.

Language: Английский

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Spatial-Confinement in Biomimetic Catalysts: Enhancing Homolytic Sulfur-Chain Reactions and Enzyme-like Activity for High-Performance Lithium-Sulfur Batteries

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: July 19, 2024

The most burning issue for high-energy-density lithium-sulfur batteries is developing high-efficient catalyst to address sulfur reaction kinetics and lithium polysulfide shuttling effects. In this work, we present Fe-TCPP@Cu-BTC, a biomimetic that mimics cytochrome c oxidase, by encapsulating porphyrin-based small molecules into metal-organic frameworks, high-performance batteries. Through series of in-situ spectroscopic analyses theoretical simulations, it was found the Cu-Fe bimetallic center within spatially confined Fe-TCPP@Cu-BTC significantly promotes homolytic cleavage Li₂S₆ LiS₃, accelerates their subsequent conversion Li₂S. enzyme-like properties were further evaluated using Michaelis-Menten kinetics, confirming can increase rate nearly 100-fold. As result, pouch delivered an energy density exceeding 300 Wh/kg. This work demonstrates tremendous potential component structural regulation enzymes in reactions metal-sulfur

Language: Английский

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