Electrolyte Design Chart Reframed by Intermolecular Interactions for High-Performance Li–Ion Batteries

JACS Au, Journal Year: 2024, Volume and Issue: 4(5), P. 1986 - 1996

Published: May 3, 2024

Developing advanced electrolytes has been regarded as a pivotal strategy for enhancing the electrochemical performance of batteries; however, criteria electrolyte design remain elusive. In this study, we present an chart reframed through intermolecular interactions. By combining systematic nuclear magnetic resonance, Fourier transform infrared measurements, molecular dynamics (MD) simulations, and machine-learning-assisted classifications, establish semiquantitative correlations between components reversibility electrolytes. We propose equivalent increment Li salt resulting from functional cosolvent solvent–solvent interactions effective prediction. The controllable regulation by properties presents varying effects increasing concentrations in different systems. Based on mechanism, demonstrate highly reversible nonflammable phosphate-based graphite||NCM811 full cells. proposed chart, semiquantitatively determined interactions, provides necessary experimental foundation basis future rapid screening prediction using machine-learning methods.

Language: Английский

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Dual‐Anionic Coordination Manipulation Induces Phosphorus and Boron‐Rich Gradient Interphase Towards Stable and Safe Sodium Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 4, 2024

High-voltage sodium metal batteries (SMBs) present a viable pathway towards high-energy-density sodium-based due to the competitive cost advantage and abundant supply of resources. However, they still suffer from severe capacity decay induced by notorious decomposition electrolyte under high voltage unstable cathode/electrolyte interphase (CEI). In addition, reactivity Na flammable electrolytes push SMBs their safety limits. Herein, special dual-anion aggregated

Language: Английский

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Glyme‐based Localized High Concentration Electrolytes Improve the Stability of Na‐ion Battery Materials in Half‐cells

Batteries & Supercaps, Journal Year: 2025, Volume and Issue: unknown

Published: March 24, 2025

Abstract Sodium‐ion batteries (SIBs) have emerged as promising alternatives to lithium‐ion for grid energy storage and automotive applications. However, their widespread adoption necessitates improved cycling stability density, largely dependent on electrode materials electrolytes. This study investigates the compatibility performance of diglyme‐based localized high concentration electrolyte (LHCE/G2) SIB applications, proposing it choice screening in half‐cell configuration. Three layered oxide cathode were tested LHCE/G2 against sodium metal counter electrodes, demonstrating significantly enhanced compared carbonate The electrochemical was confirmed through long‐term plating/stripping profiles. findings suggest that glyme‐based LHCEs offer a approach evaluating high‐voltage cathodes, minimizing electrolyte‐related degradation, enhancing reliability SIBs.

Language: Английский

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Interface Engineering with Multiple Functional Groups Coupling for High-Voltage and Wide-Temperature Sodium Metal Batteries

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 2487 - 2497

Published: April 28, 2025

Language: Английский

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Structural Investigation of Protic Ionic Liquid Electrolytes with Sodium Salt Using Polarizable Force Fields

Journal of Molecular Liquids, Journal Year: 2025, Volume and Issue: unknown, P. 127496 - 127496

Published: April 1, 2025

Language: Английский

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A Fully Flame‐Retardant Electrolyte with Laminated SEI for Exceptionally Safe, Long‐Life, and High‐Voltage Lithium Metal Batteries

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

Published: April 8, 2025

Abstract Designing an electrolyte that exhibits intrinsic nonflammability, superior compatibility with lithium metal anodes, and excellent tolerance to high‐voltage cathodes is a pivotal, yet highly challenging task for the development of high‐energy batteries. Herein, these three desirable features are simultaneously achieved by incorporating fire‐retardant diluent, ethoxy(pentafluoro)cyclotriphosphazene, together trace additive trioxane into triethylphosphate‐based electrolytes. Ethoxy(pentafluoro)cyclotriphosphazene both compete against triethylphosphate coordination Li + , inducing formation unique laminated solid‐electrolyte interphase (SEI) reversible plating/stripping reactions. This SEI outer layer interwoven components trioxane‐derived polymers N/P/F‐rich inorganics deeper region enriched LiF. It shown this trioxane‐triggered essential effectively inhibiting unwanted TEP decomposition at anode, resulting in record‐high Coulombic Efficiency 99.7% Li||Cu cells. The Li||NCM811 full cells can be cycled steadily up 4.8 V, showing outstanding capacity retention 92% @300th cycle. Importantly, designed intrinsically nonflammable, smoke it releases upon heating even extinguish open flames. 1.1 Ah pouch show no signs thermal runaway 250 °C, demonstrating exceptional safety.

Language: Английский

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Chelating Solvent Mediated Solvation Structure Enables High‐Rate Operation of Ah‐Level Li‐Ion Batteries in Nonflammable Phosphate Electrolyte

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

Published: April 25, 2025

Abstract Highly flammable carbonate electrolytes induce significant safety risk for lithium‐ion batteries (LIBs), raising concerns about their suitability large‐scale applications. In contrast, non‐flammable phosphate offer a potential solution, yet the untamed strong interaction of Li + ‐phosphates and inefficient diffusion result in sluggish reaction kinetics, which restricts operation Ah‐level LIBs to rates below 0.2C. Herein, chelating solvent‐mediated ion‐solvent coordinated structure is designed modulate interaction. This innovative approach enables high‐efficiency pseduo‐structrural diffusion, similar that observed high concentration electrolytes, while maintaining standard 1 mol L −1 achieving Li⁺ conductivity. The operating rate graphite|LiFePO 4 cells increased from 0.2C 2C, with Ah 25 retaining 73.9% 71.0% capacity after 1000 600 cycles, respectively. Additionally, maximum temperature during nail penetration significantly reduced 338.9 200 °C. strategy provides promising tuition developing advanced electrolytes.

Language: Английский

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The Solvation Structure of Localized High Concentration Electrolytes

ChemElectroChem, Journal Year: 2024, Volume and Issue: 11(11)

Published: April 4, 2024

Abstract The development of liquid electrolytes receives significant attention within the field battery research. New concepts are emerging, and one these groundbreaking ideas is localized high concentration (LHCEs). fundamental characteristic this type electrolyte related to its solvation structure. However, despite progress made, process relationship towards physicochemical electrochemical properties not yet fully understood. A comprehensive understanding LHCEs their structure requires further dedicated research analysis. This concept review offers a thorough examination design principles governing LHCEs, elucidates methodologies for investigating structures, connects insights interphase chemistry, explores potential applications in future technology.

Language: Английский

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Localized High‐Concentration Sulfone Electrolytes with High‐Voltage Stability and Flame Retardancy for Ni‐Rich Lithium Metal Batteries

Small, Journal Year: 2024, Volume and Issue: unknown

Published: May 28, 2024

Abstract The localized high‐concentration electrolyte (LHCE) propels the advanced high‐voltage battery system. Sulfone‐based LHCE is a transformative direction compatible with high energy density and safety. In this work, application of lithium bis(trifluoromethanesulphonyl)imide bis(fluorosulfonyl)imide (LiFSI) in system constructed from sulfolane 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropyl ether (TTE) investigated. addition diluent causes an increase contact ion pairs ionic aggregates solvation cluster acceptable quantity free solvent molecules. A small amount LiFSI as additive can synergistically decompose TTE on cathode participate construction both electrode interfaces. designed helps Ni‐rich to cycle firmly at voltage 4.5 V. Even mass load lean electrolyte, it keep reversible specific capacity 91.5% after 50 cycles. sulfone‐based exhibits excellent thermal stability far beyond commercial electrolytes. Further exploration in‐situ gelation has led quick conversion liquid gel state, accompanied by preserved stability, which provides for synergistic development

Language: Английский

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Solvation Effect: The Cornerstone of High‐Performance Battery Design for Commercialization‐Driven Sodium Batteries

Small, Journal Year: 2024, Volume and Issue: unknown

Published: June 10, 2024

Abstract Sodium batteries (SBs) emerge as a potential candidate for large‐scale energy storage and have become hot topic in the past few decades. In previous researches on electrolyte, designing electrolytes with solvation theory has been most promising direction is to improve electrochemical performance of through theory. general, four essential factors commercial application SBs, which are cost, low temperature performance, fast charge safety. The solvent structure significant impact applications. But so far, design electrolyte practical sodium not comprehensively summarized. This review first clarifies process Na + strategies adjusting solvation. It worth noting that relationship between interface pointed out. temperature, charging, safety issues systematically importance de‐solvation step charging emphasized help select better specific Finally, new insights solutions related SBs proposed stimulate revolutionary chemistry next generation SBs.

Language: Английский

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