Tailoring Stable PEO‐Based Electrolyte/Electrodes Interfaces via Molecular Coordination Regulating Enables 4.5 V Solid‐State Lithium Metal Batteries

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

Published: Sept. 13, 2024

Abstract Solid‐state lithium metal batteries (SSLMBs) with poly (ethylene oxide) (PEO)‐based electrolytes have increasingly become one of the most promising battery technologies due to high energy density and safety. However, adverse electrode/electrolyte interface compatibility issues hinder further application. Herein, a PEO‐based composite solid electrolyte excellent anode cathode interfacial is designed via coordination modulation strategy induced by difluorobis(oxalato)phosphate (DFBOP). By utilizing this electrolyte, robust inorganic‐rich interphase involving LiF, Li x PO y F z , P─O components in situ generated on (Li) LiNi 0.8 Co 0.1 Mn O 2 (NCM811) surfaces forceful among PEO, bis(trifluoromethanesulphonyl)imide, DFBOP subsequent adjustment front orbital levels. It contributes homogeneous deposition an effective impediment PEO oxidation decomposition at voltage, promoting superior stability. Consequently, Li‐symmetric cells modified can achieve stable cycle over 7000 h 0.2 mA cm −2 . Specially, unique organic–inorganic interpenetration network structure enables 4.5 V Li/NCM811 steadily 100 cycles, discharge capacity 215.4 mAh g −1 initial coulombic efficiency 91.23%. This research has shed light design from perspective regulation construct high‐performance SSLMBs.

Language: Английский

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Understanding and Design of Cathode–Electrolyte Interphase in High‐Voltage Lithium–Metal Batteries

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

Published: June 10, 2024

Abstract The development of lithium–metal batteries (LMBs) has emerged as a mainstream approach for achieving high‐energy‐density energy storage devices. stability electrochemical interfaces plays an essential role in realizing stable and long‐life LMBs. Despite extensive comprehensive research on the lithium anode interface, there is limited focus cathode particularly regarding high‐voltage transition metal oxide materials. In this review, challenges associated with developing materials are first discussed. Characterization techniques understanding composition structure cathode–electrolyte interphase (CEI) then introduced. Subsequently, recent developments electrolyte design interface modification constructing CEI summarized. Finally, perspectives future trends This review can offer valuable guidance designing CEI, pushing forward

Language: Английский

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Ca-based hybrid interfaces inhibit uncontrolled electrolyte decomposition for efficient Ion-Storage

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 489, P. 151116 - 151116

Published: April 8, 2024

Language: Английский

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Rolling strategy for highly efficient preparation of phosphating interface enabled the stable lithium anode

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: 1005, P. 176193 - 176193

Published: Aug. 28, 2024

Language: Английский

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Magnetic Field-Driven Ion Selectivity Boosts LiF-Rich SEI Formation for Enhanced Lithium Metal Battery Performance Across Temperatures

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

Published: March 13, 2025

Lithium metal anodes are considered highly promising electrode materials due to their exceptional theoretical capacity and low reduction potential. However, path large-scale commercialization has been obstructed by significant challenges such as uncontrolled volume expansion, severe side reactions, dendrite formation. To tackle these issues, our study introduces a covalent modification of separators using tannic acid (TA) Co2+, coupled with the application an external magnetic field. This innovative approach promotes adsorption CO32– ions while inhibiting uptake F– on TA-Co/PP separators, leading formation LiF-rich solid electrolyte interface anode surface. Such modifications significantly enhance electrochemical performance lithium batteries. Remarkably, aid field, batteries featuring modified maintained Coulombic efficiency 90% over 650 cycles at 1 mA cm–2. Additionally, under challenging conditions 60 °C 4 cm–2, polarization voltage Li symmetric cells utilizing is just 20 mV. successful demonstration underlines potential method catalyze broader adoption across varied temperature spectra.

Language: Английский

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Non‐Fluorinated Cyclic Ether‐Based Electrolyte with Quasi‐Conjugate Effect for High‐Performance Lithium Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)

Published: Aug. 29, 2024

Fluorinated ether-based electrolytes are commonly employed in lithium metal batteries (LMBs) to attenuate the coordination ability of ether solvents with Li

Language: Английский

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In Situ Self‐Polymerization of Thioctic Acid Enabled Interphase Engineering Towards High‐Performance Lithium–Sulfur Battery

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

Published: Sept. 3, 2024

Abstract Lithium–sulfur (Li–S) batteries possess high theoretical energy density, whereas the shuttle effect of polysulfides and uncontrollable lithium (Li) dendrites seriously reduce reversible capacity cycling lifespan. Constructing an interphase to address issues in both cathode anode simultaneously is significant but still challenging. In this study, a strategy functionalizing commercial polypropylene (PP) separators proposed by situ poly(thioctic acid) (PTA) polymerization. Compared with conventional separator modifications, ring‐opening polymerization methodology initiated heat more facile environment‐friendly without changing nanostructures among porous separators. On side, PTA‐coated (PTA‐PP) blocks through electrostatic interaction. generates fluoride (LiF)‐rich solid electrolyte interface (SEI), identified cryo‐transmission electron microscopy (cryo‐TEM), accelerate Li + diffusion inhibit growth dendrites. Due interphases constructed PTA‐PP separator, Li–S cells exhibit excellent long‐term which retention rate than 76% after 700 cycles at 0.5 C. The elaborate modification may provide insights into high‐performance design promote potentially large‐scale applications batteries.

Language: Английский

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Insertion Type Li₃VO₄ Lithiophilic Sites Boosting Dendrite‐Free Lithium Deposition in Trapping‐and‐leveling Model

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

Published: Feb. 19, 2025

Abstract Lithium (Li) metal batteries offer high energy densities but suffer from uncontrolled lithium deposition, causing serious dendrite growth and volume fluctuation. Tailorable Li nucleation uniform early‐stage plating are essential for homogenous deposition. Herein, insertion type 3 VO 4 is first demonstrated as efficient lithiophilic sites trapping + ions nucleation. By homogenizing the distribution of electric field flux via an ingenious architecture design with nanodots grown on carbon fibers (LVO@CNFs), leveling deposition after also realized. These, together, result in smooth dendrite‐free LVO@CNFs a trapping‐and‐leveling model, giving rise to unprecedented performance (highly stable plating/stripping exceeding 2500 h at 2 mA cm −2 under capacity, high‐capacity retention 82.5% over 500 cycles Li@LVO@CNFs//LiFePO battery). The successful host insertion‐type may pave new way long lifespan batteries.

Language: Английский

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Customized Solvation Structures for Long‐Term Stable Lithium Metal Batteries

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

Published: March 6, 2025

Lithium metal batteries (LMBs) suffer from severe lithium dendrite growth and side reactions in conventional carbonate electrolytes, which are characterized by low coulombic efficiency poor cycling stability, electrolyte engineering is an effective method for increasing the reversibility of anodes. Herein, solubility nitrate (LiNO3), almost insoluble electrolyte, improved adding zinc trifluoroacetate (Zn(TFA)2), a competitive solvation structure constructed, forming anion-enriched Li+ structure, conducive to formation stable SEI effectively inhibits adverse reactions. The anode exhibits uniform deposition extended cycle life, with high over plating/stripping 640 h. Furthermore, Li||LFP full cell upgraded can operate steadily 300 cycles at 1 C, compatibility high-voltage NCM811 cathode also significantly improved. This work provides feasible strategy dependable interfacial chemistry

Language: Английский

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Synergistic Construction of Electrode–Electrolyte Interphases via Electrolyte Cosolvent and Additive Chemistry toward Ultrastable and Fast-Charging Li-Rich Batteries

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

Published: March 11, 2025

Lithium-rich manganese oxide (LRMO) is a promising high-energy-density material for high-voltage lithium-ion batteries, but its performance hindered by interfacial side reactions, transition metal dissolution, and oxygen release. To address these issues, we propose electrolyte strategy that utilizes cosolvent additive synergy to create stable dual interphases at both the cathode anode. Specifically, lithium difluoro(oxalato)borate (LiDFOB) sacrificially decomposes form uniform yet cathode–electrolyte interphase (CEI) layer, while of bis(2,2,2-trifluoroethyl) carbonate (BTFEC) effectively adjusts solvation structure synergistically stabilizes solid–electrolyte (SEI) on anode, ultimately achieving ultrahigh cycle stability fast-charging feasibility. The presence B–F, LiBxOy species derived from LiDFOB exceptionally fast-ion-transfer CEI F-rich robust SEI layer inhibits irregular growth dendrites. Our enables Li||LRMO cells maintain 95% capacity after 200 cycles 4.8 V, with specific 238 mAh g–1 350 3C. Importantly, 5 Ah graphite||LRMO pouch cell achieves high energy density 323 Wh kg–1 80.4% retention 150 cycles, demonstrating practical application potential.

Language: Английский

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