Reliable Sulfur Cathode Design for All‐Solid‐State Lithium Metal Batteries Based on Sulfide Electrolytes

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

Published: March 6, 2025

Abstract Sulfide electrolytes are considered the most promising technique for all‐solid‐state lithium–sulfur batteries (ASLSBs) due to relatively high ionic conductivity and superior chemical compatibility with composite sulfur cathodes. However, cathodes based on sulfide feature large volume expansion, unstable interfacial contact, inherent insulating nature, which impedes practical application of ASLSBs. Therefore, a systematic design cathode side ASLSBs is crucial ensuring well‐contacted, electrochemically stable cathode–electrolyte interface, an effective ion‐electron transfer network. Here, comprehensive discussion latest strategies will be delivered, highlighting their effectiveness in improving performances First, major challenges including slow oxidation kinetics significant expansion dissected. Then, focus shifted degradation processes at interface between electrolyte. Subsequently, improvement stability by structural modulation elaborated. Finally, progress, we present new perspective constructing efficient transport network cathode‐electrolyte offers insights directions achieving future.

Language: Английский

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High Performance Lithium–Sulfur Battery with a Multifunctional Organic Nitrogen–Fluorine Compounds-Modified Electrolyte

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

Published: March 31, 2025

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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Dual‐Interface Regulation for High‐Performance Magnesium–Sulfur Batteries

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

Published: May 8, 2025

Abstract Magnesium–sulfur (Mg–S) batteries are promising candidates for high‐energy‐density storage systems, but their performance is critically dependent on the interfacial properties of both anode and cathode. This study explores a dual‐interface regulation strategy to enhance Mg–S battery via tailored electrolyte additives. For anode, tetrabutylammonium bromide (TBABr) added commercially available chlorine‐free Mg(TFSI) 2 ‐based electrolytes, forming robust bromide‐containing solid interphase (SEI) that extend cycle life Mg//Mg cells. cathode, 1,3,5‐benzenetrithiol (BTT) introduced as cathode‐electrolyte interface (CEI) modifier promote formation an organopolysulfide layer effectively mitigates polysulfide shuttling. approach greatly increase lives cells magnesium–selenium (Mg–Se) work underscores importance holistic engineering provides valuable insights development high‐performance batteries.

Language: Английский

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Relay Catalyst for Accelerating Lithium Polysulfide Conversion Kinetics and Long-life Lithium Sulfur Batteries

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110896 - 110896

Published: March 1, 2025

Language: Английский

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Targeting Acceleration of the Rate-Determining Step in Sulfur Redox and Dendrite-Free Lithium: Heterointerface and Electron Structural Engineering

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 26, 2025

Currently, most catalysts for lithium-sulfur batteries suffer from some shortcomings, including restricted active sites and poor catalytic kinetics. Herein, we developed an advanced catalyst of V-MXene@octahedral porous carbon (MX@OPC), which features a "built-in interfacial electric field" (BIEF) "dual-functional sites" (DCASs), to target the accelerated rate-determining step in polysulfide redox kinetics dendrite-free lithium behaviors. The well-designed heterointerface forms BIEF due differences work function charge distribution, contributing enhanced electron transfer low lithium-ion diffusion barriers. DCASs with superior Li2S4 desorption efficiently catalyze conversion Li2S2 by distribution relaxation times (DRT) analysis density functional theory (DFT) calculations. V-MXene exhibits strong lithophilicity, facilitates uniform nucleation growth lithium. As result, battery MX@OPC delivers capacity fade rate per cycle as 0.017% over 1200 cycles at 2 C. Furthermore, renders Li||Li symmetric cell maintain stable overpotential 16 mV 2500 h. This provides inspiring insights into directed catalysis generation toward accelerating rate-determining-step sulfur deposition Li-S batteries.

Language: Английский

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Modulating carrier-catalyst heterointerfaces to boost catalytic polysulfide conversion in lithium-sulfur batteries

Energy Materials, Journal Year: 2025, Volume and Issue: 5(9)

Published: May 16, 2025

Enhancing the catalytic activity of sulfur cathode hosts is critical for suppressing shuttle effect and accelerating polysulfides redox kinetics in lithium-sulfur (Li-S) batteries. However, efficient polysulfide adsorption catalysis conversion rely on synergistic interactions between catalyst supporting carrier, particularly optimizing site density electron/ion transport rates. Herein, we modulate carrier-catalyst heterointerface to enhance conversion. Metallic 1T-phase MoS2 nanospheres are uniformly dispersed onto nitrogen-doped graphene (N-G) sheets, forming a composite host material (1T-MoS2/N-G) Li-S N-G serves as both conductive substrate charge transfer support loading, while 1T-MoS2, rich sites, functions an electrocatalyst, promoting ion diffusion, adsorbing soluble polysulfides, their transformation into solid lithium sulfide. Benefiting from these structural advantages, S/1T-MoS2/N-G exhibits initial capacity 1,296.8 mAh g-1 at 0.2 C demonstrates outstanding cycle stabilization, with decay rate only 0.015% per over 500 cycles 1.0 C. Even under demanding conditions, such loading 6.5 mg cm-2 lean electrolyte 7 µL mg-1, provides areal 7.2 retains 4.8 after 100 cycles. These findings offer new insights design advanced materials high-performance cathodes broader electrocatalytic applications.

Language: Английский

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Weakly Solvating Electrolyte: Regulating Polysulfide Intermediates for High‐Performance Lithium‐Sulfurized Polyacrylonitrile Batteries

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

Published: May 29, 2025

Abstract Electrolyte engineering plays a crucial role in the design of high energy‐density lithium‐sulfurized polyacrylonitrile (Li‐SPAN) batteries, promising energy storage technology. However, current predominant electrolyte systems face challenges anode dendrite growth and cathode polysulfide loss, which limit cycling stability Li‐SPAN batteries. Here, weakly solvating (WSE) primarily composed diethoxy methane (DEM) is proposed to simultaneously address at both electrodes. At anode, DEM's capability accelerates Li + diffusion desolvation, preventing out‐of‐plane deposition formation caused by concentration gradients surface. More significantly cathode, solvated exhibits stronger Lewis acidity, preferentially stabilizing S 3 2− intermediates via hard acid‐base interaction. These higher‐reduction‐state promote faster subsequent lithiation reactions, reducing loss while improving rate performance enhancements corresponding mechanisms are supported electrochemical spectroscopic characterizations. With this WSE, batteries achieve exceptional (0.087% capacity fade per cycle over 500 cycles 1 C), pouch cell life increases from 9 35 with 90.6% retention. This strategy provides valuable insights for developing high‐performance

Language: Английский

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Constructing a Multifunctional Sandwich-Structured Sulfur Host To Enhance Energy Density and Cycling Life in Lithium–Sulfur Battery

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: June 4, 2025

Language: Английский

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