Developing Cathode Films for Practical All‐Solid‐State Lithium‐Sulfur Batteries

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

Published: July 29, 2024

Abstract The development of all‐solid‐state lithium‐sulfur batteries (ASSLSBs) toward large‐scale electrochemical energy storage is driven by the higher specific energies and lower cost in comparison with state‐of‐the‐art Li‐ion batteries. Yet, insufficient mechanistic understanding quantitative parameters key components sulfur‐based cathode hinders advancement ASSLSB technologies. This review offers a comprehensive analysis electrode parameters, including capacity, voltage, S mass loading content establishing (Wh kg −1 ) density L ASSLSBs. Additionally, this work critically evaluates progress enhancing lithium ion electron percolation mitigating electrochemical‐mechanical degradation cathodes. Last, critical outlook on potential future research directions provided to guide rational design high‐performance cathodes practical

Language: Английский

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Ether‐Modified Nonflammable Phosphate Enabling Anion‐Rich Electrolyte for High‐Voltage Lithium Metal Batteries

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

Published: Nov. 6, 2024

Abstract Phosphate‐based localized high‐concentration electrolytes (LHCE) feature high flame retardant and satisfactory cathodic stability for lithium metal batteries. However, stable cycling of those at ultra‐high upper cut‐off voltages long‐term remains challenging. Herein, an ether‐modified phosphate, diethyl (2‐methoxy ethoxy) methylphosphonate (DMEP), is designed high‐voltage applications. The ether modification enhances the Li + ‐DMEP‐FSI − coordination structure, promoting formation cation‐anion aggregates (AGG) dominated solvation which favors generation LiF‐rich cathode electrolyte interphase layers compared to triethyl phosphate (TEP)‐based LHCE. Consequently, degradation, including transition‐metal dissolution electrode cracking, well‐suppressed. LiNi 0.8 Co 0.1 Mn O 2 (NCM811)||Li full cells using DMEP‐based LHCEs show more than 90.7% capacity retention ultrahigh voltage 4.7 V after 100 cycles. Notably, DMEP‐LHCE exhibits enhanced safety that TEP‐LHCE, suggesting its versatility potential next‐generation

Language: Английский

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Designing Isocyanate‐Containing Elastomeric Electrolytes for Antioxidative Interphases in 4.7 V Solid‐State Lithium Metal Batteries

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

Published: Oct. 9, 2024

Abstract To facilitate the use of solid polymer electrolytes (SPEs) with high‐nickel (Ni) cathodes in high‐voltage lithium (Li) metal batteries (LMBs), it is crucial to address challenges low oxidative stability and formation vulnerable interphases. In this study, isocyanate groups (−N═C═O) are incorporated develop an SPE a bi‐continuous structure, consisting elastomeric plastic crystal phases. This rationally designed exhibits high ionic conductivity (0.9 × 10 −3 S cm −1 at 25 °C), excellent elasticity (elongation break 330%), enhanced (over 4.8 V vs. Li/Li⁺). A full cell, incorporating thin Li foil 40 µm, high‐Ni LiNi 0.8 Co 0.1 Mn O 2 (NCM811) cathode operating 4.7 Li/Li⁺, demonstrates cyclability, retaining 70% its initial capacity after 200 cycles under C‐rate 1C °C. The extended cycling isocyanate‐containing Li/Li⁺ attributed robust compact inorganic‐rich interphases enabled by antioxidative −N−C═O components, as well uniform deposition structured SPE. study suggests that system promising candidate for solid‐state LMBs constructing stable

Language: Английский

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Progresses on advanced electrolytes engineering for high-voltage lithium metal batteries

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 500, P. 157269 - 157269

Published: Nov. 1, 2024

Language: Английский

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Tuning anionic bands and lattice stability by short-range disorder at nanoscale for ultrastable Co-free Li-rich cathode

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 24, 2025

Language: Английский

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Developing Quasi‐Solid‐State Ether‐Based Electrolytes with Trifluorotoluylation Ionic Liquids for High Voltage Lithium Metal Batteries

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

Published: April 25, 2025

Abstract The practical application of quasi‐solid‐state ether‐based electrolytes is hindered by lithium dendrite formation and poor oxidation stability, which reduce the cycle life energy density battery. Here, taking advantage ionic liquids’ high interactions structural flexibility in forming an optimized electrode/electrolyte interface, a pyrrolidinium‐based liquids with trifluorotoluylation cationic segment designed developed. anions induced to form robust inorganic LiF‐rich interphase at cathode, thereby effectively achieving stability suppressing dissolution transition metal ions. In addition, LiF interphases derived from cations increase modulus anode interface suppress growth dendrites. Therefore, Li‐LiFePO 4 , Li‐LiCoO 2 Li‐LiNi 0.8 Co 0.1 Mn O full cells demonstrate remarkable performance improvements current (10 C), wide voltage range 4.5 V, mass loading 11.1 mg cm −2 temperature −20–80 °C. Furthermore, 2.66 Ah‐level pouch cell high‐energy‐density exceeding 356 Wh kg ‒1 excellent cyclic demonstrates potential strategy providing path for batteries.

Language: Английский

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Regulating Amine Substitution in Fluorosulfonyl-Based Flame-Retardant Electrolytes for Energy-Dense Lithium Metal Batteries

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Sulfone-based electrolytes offer unusually high anodic and thermal stability that in principle makes them promising candidates for fabricating energy-dense lithium metal batteries (LMBs). Their uses practical are currently limited by their inability to sustain long-term Li plating/stripping processes due reactivity toward the metal. Here, we report on design synthesis of a unique family fluorosulfonyl group-based (FSO2-) molecules, modified with ethyl (FSE)/N,N-dimethyl (FSNDM)/N,N-diethyl (FSNDE)/N-pyrrolidine (FSNP) end groups create exceptionally stable single-salt single-solvent electrolytes. The flammability, solvation structure, ion transport, deposition kinetics, high-voltage systematically studied. It is shown nonflammable, possess weak characteristics, yet manifest room-temperature ionic conductivities (1.6-6.1 mS cm-1) low solution viscosities. In comparison FSE, FSNDM-, FSNDE-, FSNP-based exhibit an reversible Coulombic efficiency (>99.71% over 800 cycles) typical oxidative at voltages exceeding 4.6 V. Deployed as (20 μm anode 3 g A h-1 electrolyte) high-loading (18.5 mg cm-2) LiNi0.8Co0.1Mn0.1O2 cathodes, 329 cycles have been achieved before 80% capacity retention. Six Ah pouch cells based designed also energy density (496 W h kg-1) 150 most 2.7% volume expansion. Our findings demonstrate through intentional molecular design, sulfone provide robust route nonflammable compatible cathodes.

Language: Английский

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Improving thermal stability and kinetical properties through polymer brushes towards wide-temperature solid-state lithium metal batteries

Composites Part B Engineering, Journal Year: 2025, Volume and Issue: unknown, P. 112328 - 112328

Published: Feb. 1, 2025

Language: Английский

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Fundamentals, Status and Promise of Li‐Rich Layered Oxides for Energy‐Dense Li‐Ion Batteries

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

Published: March 17, 2025

Abstract Li‐ion batteries (LIBs) are the dominant electrochemical energy storage devices in global society, which cathode materials key components. As a requirement for higher energy‐dense LIBs, Li‐rich layered oxides (LLO) cathodes that can provide specific capacity urgently needed. However, LLO still face several significant challenges before bringing these to market. In this Review, fundamental understanding of is described, with focus on physical structure‐electrochemical property relationships. Specifically, various strategies toward reversible anionic redox discussed, highlighting approaches take basic structure battery into account. addition, application all‐solid‐state and consider prospects assessed.

Language: Английский

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Robust and Antioxidative Quasi‐Solid‐State Polymer Electrolytes for Long‐Cycling 4.6 V Lithium Metal Batteries

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

Published: March 30, 2025

Abstract Quasi‐solid‐state polymer electrolytes (QSPEs) have been considered as one of the most promising for high‐safety high‐energy‐density lithium metal batteries (LMBs). However, their inadequate mechanical properties and instability under high voltages pose significant challenges practical applications. Herein, robust antioxidative QSPEs are developed based on a polymer‐brush‐based rigid supporting film (BC‐ g ‐PLiMTFSI‐ b ‐PPFEMA, BC: bacterial cellulose, PLiMTFSI: poly(lithium (3‐methacryloyloxypropylsulfonyl) (trifluoromethylsulfonyl)imide), PPFEMA: poly(2‐(perfluorohexyl)ethyl methacrylate)). The BC nanofibril backbone can produce highly porous structure with outstanding strength. More importantly, PLiMTFSI‐ ‐PPFEMA side‐chains not only obviously increase conversion ratio easily oxidized monomers in QSPEs, but also possess strong interaction unstable electrolyte components. With such solid‐state electrolytes, Li/LiNi 0.8 Mn 0.1 Co O 2 full cell cathode loading (20.3 mg cm −2 ) exhibits specific discharge capacity 200.7 mAh −1 at 0.5 C demonstrates long lifespan 137 cycles retained 170.7 cut‐off voltage 4.5 V. 4.6 V, 147.0 after 187 be Li/LiCoO cells. This work provides feasible development strategy long‐cycling high‐voltage LMBs.

Language: Английский

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