Development of PFAS-Free Locally Concentrated Ionic Liquid Electrolytes for High-Energy Lithium and Aluminum Metal Batteries

Accounts of Chemical Research, Год журнала: 2025, Номер unknown

Опубликована: Янв. 26, 2025

ConspectusLithium-ion batteries (LIBs) based on graphite anodes are a widely used state-of-the-art battery technology, but their energy density is approaching theoretical limits, prompting interest in lithium-metal (LMBs) that can achieve higher density. In addition, the limited availability of lithium reserves raises supply concerns; therefore, research postlithium metal underway. A major issue with these anodes, including lithium, dendritic formation and insufficient reversibility, which leads to safety risks due short circuits use flammable electrolytes.Ionic liquid electrolytes (ILEs), composed salts ionic liquids, offer safer alternative nonflammable nature high thermal stability. Moreover, they enable Coulombic efficiency (CE) for (LMAs) allow reversible stripping/plating various post-lithium metals application, e.g., aluminum (AMBs). Despite advantages, ILEs suffer from viscosity, impairs ion transport wettability. To resolve challenges, researchers have developed locally concentrated (LCILEs) by adding low-viscosity nonsolvating cosolvents, hydrofluoroether, ILEs. These cosolvents do not coordinate cationic charge carriers, thereby reducing viscosity improving without compromising compatibility anodes. However, inherent difference molecular organic solvents liquids full charged species, most i.e., less effective respect conventional solvents. hydrofluoroether contains environmentally problematic -CF3 and/or -CF2- groups, per- polyfluoroalkyl substances (PFAS), subject restrictions.In this Account, we provide an overview endeavors our group development PFAS-free LCILEs high-energy LMBs AMBs. First, aromatic cations less/nonfluorinated proposed weaken cation-anion interaction strengthen cation-cosolvent interaction, respectively. This consideration uncovered phase nanosegregation structure effectively reduces promotes Li+ ability nonaromatic highly fluorinated PFAS cosolvents. Then, effect electrolyte components Li+, SEI composition LMA reversibility presented, confirms feasibility reaching CE up 99.7% LCILEs. subsequent discussion cathode compatibility, present addition LiFePO4 cyclability inferior density, nickel-rich layered oxide sulfurized polyacrylonitrile (SPAN) be employed construct different anodic Additionally, feasible application LCILE strategy promote kinetics AMBs relying anode chemistry demonstrated. Lastly, future directions emphasis component optimization, dynamics, electrode/electrolyte interphase provided.

Язык: Английский

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Nonflammable F/N synergistic electrolyte boosting high-voltage Li metal batteries in wide temperature range

Energy storage materials, Год журнала: 2025, Номер unknown, С. 104066 - 104066

Опубликована: Янв. 1, 2025

Язык: Английский

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Regulating Interfacial Wettability for Fast Mass Transfer in Rechargeable Metal-Based Batteries

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Фев. 26, 2025

The interfacial wettability between electrodes and electrolytes could ensure sufficient physical contact fast mass transfer at the gas-solid-liquid, solid-liquid, solid-solid interfaces, which improve reaction kinetics cycle stability of rechargeable metal-based batteries (RMBs). Herein, engineering multiphase interfaces is summarized from electrolyte electrode aspects to promote interface rate durability RMBs, illustrates revolution that taking place in this field thus provides inspiration for future developments RMBs. Specifically, review presents principle macro- microscale summarizes emerging applications concerning effect on Moreover, deep insight into development provided outlook. Therefore, not only insights but also offers strategic guidance modification optimization toward stable electrode-electrolyte

Язык: Английский

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Electrode‐Electrolyte Interface Regulation Enables Large‐Capacity Gel‐State Na Metal Batteries with Appealing Cycling Stability

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 20, 2025

Abstract Gel‐state Na metal batteries (NMBs) are promising candidates for the large‐scale energy storage due to merits of low cost, abundant sodium resources, and high density. However, long‐term lifespan safety NMBs with large capacity limited by unstable electrode‐electrolyte interface. Herein, interfaces regulated mechanically robust GPE coupled artificial NaBr/Na x Sn y layer on anode, enabling symmetric cells a cycling over 2500 h at 0.5 mA cm −2 , along an ultralong cycle life ca. 4700 0.2 under −20 °C. With area 0.9 mAh based 3 V 2 (PO 4 ) SnBr ‐Na|GPE|Na full exhibit retention 96.6% after 1100 cycles, resulting from ionic conductivity (3.7 mS −1 stable inorganic surface. This work provides new insight development capacity.

Язык: Английский

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Indium-MOF as Multifunctional Promoter to Remove Ionic Conductivity and Electrochemical Stability Constraints on Fluoropolymer Electrolytes for All-Solid-State Lithium Metal Battery

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Май 7, 2025

Abstract Fluoropolymers promise all-solid-state lithium metal batteries (ASLMBs) but suffer from two critical challenges. The first is the trade-off between ionic conductivity ( σ ) and anode reactions, closely related to high-content residual solvents. second, usually consciously overlooked, fluoropolymer’s inherent instability against alkaline anodes. Here, we propose indium-based metal–organic frameworks (In-MOFs) as a multifunctional promoter simultaneously address these challenges, using poly(vinylidene fluoride–hexafluoropropylene) (PVH) typical fluoropolymer. In-MOF plays trio: (1) adsorbing converting free solvents into bonded states prevent their side reactions with anodes while retaining advantages on Li + transport; (2) forming inorganic-rich solid electrolyte interphase layers PVH reacting promote uniform deposition without dendrite growth; (3) reducing crystallinity promoting Li-salt dissociation. Therefore, resulting PVH/In-MOF (PVH-IM) showcases excellent electrochemical stability anodes, delivering 5550 h cycling at 0.2 mA cm −2 remarkable cumulative capacity of 1110 mAh . It also exhibits an ultrahigh 1.23 × 10 −3 S −1 25 °C. Moreover, LiFePO 4 |PVH-IM|Li full cells show outstanding rate capability cyclability (80.0% retention after 280 cycles 0.5C), demonstrating high potential for practical ASLMBs.

Язык: Английский

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Regulating the solvation structure of an acetonitrile-based electrolyte for Li/NMC811 batteries cycled at low temperature

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(12), С. 6947 - 6954

Опубликована: Янв. 1, 2024

An acetonitrile-based localized high concentration electrolyte has been developed for low temperature lithium metal batteries. The corresponding Li/NMC811 cell delivers a capacity of 113 mA h g −1 at −40 °C with 85.5% retention.

Язык: Английский

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An Anode-Free Sodium Dual-ion Battery

Energy storage materials, Год журнала: 2024, Номер 70, С. 103480 - 103480

Опубликована: Май 13, 2024

Язык: Английский

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Interphase Engineering via Solvent Molecule Chemistry for Stable Lithium Metal Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Март 27, 2024

Abstract Lithium metal battery has been regarded as promising next‐generation system aiming for higher energy density. However, the lithium anode suffers severe side‐reaction and dendrite issues. Its electrochemical performance is significantly dependant on electrolyte components solvation structure. Herein, a series of fluorinated ethers are synthesized with weak‐solvation ability owing to duple steric effect derived from designed longer carbon chain methine group. The structure rich in AGGs (97.96 %) enables remarkable CE 99.71 % (25 °C) well high 98.56 even at −20 °C. Moreover, lithium‐sulfur exhibits excellent wide temperature range (−20 50 ascribed modified interphase LiF/LiO 2 . Furthermore, pouch cell delivers superior density 344.4 Wh kg −1 maintains 80 capacity retention after cycles. novel solvent design via molecule chemistry provides alternative strategy adjust thus favors high‐energy batteries.

Язык: Английский

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Enhancing the Filler Utilization of Composite Gel Electrolytes via In Situ Solution‐Processable Method for Sustainable Sodium‐Ion Batteries

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 24, 2024

Abstract The composite gel electrolyte (CGE), which combines the advantages of inorganic solid‐state electrolytes and solid polymer electrolytes, is regarded as ultimate candidate for constructing batteries with high safety superior electrode‐electrolyte interface contact. However, ubiquitous agglomeration nanofillers results in low filler utilization, seriously reduces structural uniformity ion transport efficiency, thus restricting development consistent durable batteries. Herein, a solution‐processable method to situ construct CGE utilization introduced. homogeneous metal–organic framework fillers contribute uniform ionic electronic filed distribution, realizing stable interface. Consequently, achieves an ultra‐long lifespan 10 000 cycles capacity retention 80.2%. This work provides guidance high‐performance CGEs electrochemical energy‐storage devices.

Язык: Английский

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Practical Lithium–Sulfur Batteries: Beyond the Conventional Electrolyte Concentration

ACS Energy Letters, Год журнала: 2024, Номер unknown, С. 5576 - 5586

Опубликована: Окт. 26, 2024

Язык: Английский

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