Non-Flammable Electrolyte Mediated by Solvation Chemistry toward High-Voltage Lithium-Ion Batteries

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(4), P. 1604 - 1616

Published: March 19, 2024

The development of nonflammable electrolytes can boost energy density and battery safety, especially for layered metal oxide cathodes operating at high voltage. However, most are designed in a concentration compatibility with graphite electrodes and/or less decomposition. Herein, we introduced solvation structure-mediated model to develop electrolyte based on trimethyl phosphate (TMP) solvent normal concentration. This advancement allows the || lithium cobalt full cell operate 4.5 V, delivering also exhibiting feature. achievement is realized using previously unreported components, including carbonate solvent, ethylene sulfate (DTD) additives, conventional LiPF6 salt. We analyzed molecular behaviors each composition uncovered impact DTD, highlighting its prerequisite conditions effectively weakening Li+-TMP interactions. bottom-up design strategy offers fresh perspective regulating structures formulations.

Language: Английский

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Enabling Ultralow‐Temperature (−70 °C) Lithium‐Ion Batteries: Advanced Electrolytes Utilizing Weak‐Solvation and Low‐Viscosity Nitrile Cosolvent

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(5)

Published: Nov. 3, 2023

Abstract Low‐temperature performance of lithium‐ion batteries (LIBs) has always posed a significant challenge, limiting their wide application in cold environments. In this work, the high‐performance LIBs working under ultralow‐temperature conditions, which is achieved by employing weak‐solvation and low‐viscosity isobutyronitrile as cosolvent to tame affinity between solvents lithium ions, reported. The as‐prepared electrolytes exhibit sufficiently high conductivity (1.152 mS cm −1 ) at −70 °C. enable LiCoO 2 cathode graphite anode achieve Coulombic efficiency >99.9% during long‐term cycling room temperature, respectively 75.8% 100.0% room‐temperature capacities −40 Even //graphite pouch cells can retain 68.7% capacity when discharged °C, present stable 60 This work provides solution for development advanced wide‐temperatures range.

Language: Английский

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Regulating Ion‐Dipole Interactions in Weakly Solvating Electrolyte towards Ultra‐Low Temperature Sodium‐Ion Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 9, 2024

Sodium-ion batteries (SIBs) are recognized as promising energy storage devices. However, they suffer from rapid capacity decay at ultra-low temperatures due to high Na

Language: Английский

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Designing Advanced Electrolytes for High-Safety and Long-Lifetime Sodium-Ion Batteries via Anion–Cation Interaction Modulation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(23), P. 15751 - 15760

Published: June 4, 2024

Safety hazards caused by flammable electrolytes have been major obstacles to the practical application of sodium-ion batteries (SIBs). The adoption nonflammable all-phosphate can effectively improve safety SIBs; however, traditional low-concentration phosphate are not compatible with carbon-based anodes. Herein, we report an anion–cation interaction modulation strategy design superior physicochemical properties. Tris(2,2,2-trifluoroethyl) (TFEP) is introduced as a cosolvent regulate ion–solvent-coordinated (ISC) structure through enhancing interactions, forming stable anion-induced ISC (AI-ISC) structure, even at low salt concentration (1.22 M). Through spectroscopy analyses and theoretical calculations, reveal underlying mechanism responsible for stabilization these electrolytes. Impressively, both hard carbon (HC) anode Na4Fe2.91(PO4)2(P2O7) (NFPP) cathode work well developed designed electrolyte enables Ah-level HC//NFPP pouch cells average Coulombic efficiency (CE) over 99.9% capacity retention 84.5% after 2000 cycles. In addition, operate in wide temperature range (−20 60 °C) successfully pass rigorous testing. This provides new insight into electrochemically compatibility high-safety long-lifetime SIBs.

Language: Английский

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LiNO₃‐Based Electrolytes via Electron‐Donation Modulation for Sustainable Nonaqueous Lithium Rechargeable Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(10)

Published: Jan. 13, 2024

LiPF

Language: Английский

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Molecular modulation strategies for two-dimensional transition metal dichalcogenide-based high-performance electrodes for metal-ion batteries

Chemical Science, Journal Year: 2024, Volume and Issue: 15(7), P. 2323 - 2350

Published: Jan. 1, 2024

Through the purposeful modulation of specific parts or regions TMD molecules, molecular strategies aim to realize effective TMDs' properties from an ‘internal’ perspective.

Language: Английский

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Intrinsic Solubilization of Lithium Nitrate in Ester Electrolyte by Multivalent Low‐Entropy‐Penalty Design for Stable Lithium‐Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(10)

Published: Jan. 8, 2024

LiNO

Language: Английский

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Anchored Weakly‐Solvated Electrolytes for High‐Voltage and Low‐Temperature Lithium‐ion Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: June 14, 2024

Electrolytes endowed with high oxidation/reduction interfacial stability, fast Li-ion desolvation process and decent ionic conductivity over wide temperature region are known critical for low fast-charging performance of energy-dense batteries, yet these characteristics rarely satisfied simultaneously. Here, we report anchored weakly-solvated electrolytes (AWSEs), that designed by extending the chain length polyoxymethylene ether electrolyte solvent, can achieve above merits at moderate salt concentrations. The -O-CH

Language: Английский

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Contact Ion-Pair-Dominated Electrolyte Enabling Inorganic-Rich Solid–Electrolyte Interphase for Long-Cycling Magnesium Metal Anodes

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 552 - 561

Published: Jan. 1, 2025

Mg anodes are hindered by a huge overpotential and limited cycling life, stemming primarily from the unstable interphase between electrolyte. An effective approach lies in establishing an anion-derived, inorganic-rich solid–electrolyte (SEI) that mitigates continuous reduction of Nevertheless, high charge density divalent cations poses significant challenge balancing coordination dissociation anions within Mg2+ solvation sheath. Herein, selecting small-sized OTf–, diglyme solvent, trimethyl phosphate (TMP) as cosolvents with similar donor number (DN) values, electrolyte-dominated Mg2+–OTf– contact ion-pair configuration is achieved, further deriving stable inorganic SEI containing fluoride phosphide components. Among them, TMP can break lattice energy magnesium salts, while OTf– low electron delocalization ensure degree Mg2+, jointly realizing anion chemistry. MgF2 MgS, dominated decomposition at potential 0.6 V (vs Mg/Mg2+), enhance electronic insulation interphase. Consequently, exhibit superior performance over 3200 h polarization (<0.1 V) excellent plating/stripping Coulombic efficiency 1000 cycles 0.1 mA cm–2.

Language: Английский

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Doping in Solvation Structure: Enabling Fluorinated Carbonate Electrolyte for High-Voltage and High-Safety Lithium-Ion Batteries

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(6), P. 2536 - 2544

Published: May 7, 2024

Operating a Ni-rich cathode beyond 4.3 V safely holds promise for boosting the energy density in lithium-ion batteries (LIBs). Methyl 2,2,2-trifluoroethyl carbonate (FEMC) shows oxidative stability and high safety but suffers from degraded LUMO levels once coordinated with Li+ within electrolytes. Here, we utilize propylene (PC) as functional dopant, which deliberately tunes FEMC-dominated solvation chemistry improves by dipole–dipole interaction microsolvating competition. As result, optimized electrolyte demonstrates an expanded electrochemical window (4.7 NCM811), fire resistance, wide liquid range (−60–120 °C), affording 75.6% capacity retention 1.2 Ah NCM811/graphite pouch cells over 1200 cycles. This "doping strategy" is generalized to other electrolytes (e.g., carbonates, fluorinated esters, carboxylic esters) qualifies ameliorated interfacial compatibility, providing insights designing high-safety high-energy LIBs.

Language: Английский

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