Correlating the Solvating Power of Solvents with the Strength of Ion‐Dipole Interaction in Electrolytes of Lithium‐ion Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(47)

Опубликована: Окт. 9, 2023

The solvation structure of Li+ plays a significant role in determining the physicochemical properties electrolytes. However, to date, there is still no clear definition solvating power different electrolyte solvents, and even solvents that preferentially participate remain controversial. In this study, we comprehensively discuss process ions using both experimental characterizations theoretical calculations. Our findings reveal dependent on strength -solvent (ion-dipole) interaction. Additionally, uncover anions tend enter sheath most systems through -anion (ion-ion) interaction, which weakened by shielding effect solvents. competition between interactions ultimately determines final structures. This insight into fundamental understanding provides inspiration for design multifunctional mixed-solvent electrolytes advanced batteries.

Язык: Английский

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Cyclopentylmethyl Ether, a Non‐Fluorinated, Weakly Solvating and Wide Temperature Solvent for High‐Performance Lithium Metal Battery

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(21)

Опубликована: Март 23, 2023

Abstract While recent work demonstrates the advantages of weakly solvating solvents in enhancing cyclability LMBs, both new designs and design strategies for high performance solvent, especially physicochemical properties, are still lacking. Here, we propose a molecular to tune power properties non‐fluorinated ether solvent. The resulting cyclopentylmethyl (CPME) have weak wide liquid‐phase temperature range. By optimizing salt concentration, CE is further promoted 99.4 %. Besides, improved electrochemical Li−S battery CPME‐based electrolytes obtained at −20 °C. Li||LFP (17.6 mg cm −2 ) with developed electrolyte maintains >90 % original capacity over 400 cycles. Our concept solvent molecule provides promising pathway window high‐energy‐density LMBs.

Язык: Английский

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Fundamentals of Electrolyte Design for Wide‐Temperature Lithium Metal Batteries

Advanced Energy Materials, Год журнала: 2023, Номер 13(37)

Опубликована: Авг. 3, 2023

Abstract Lithium metal‐based batteries (LMBs) have garnered significant attention due to their exceptional energy density and lightweight characteristics. However, the electrochemical performance of LMBs often falls short, particularly in extreme temperature conditions. To address these challenges, development electrolytes capable withstanding wide ranges has emerged as a highly promising strategy for enhancing operational capabilities LMB across diverse weather This comprehensive review aims explore degradation mechanisms wide‐temperature electrolytes, establishing fundamental understanding failure that impede at harsh temperatures. Essential properties required are elucidated, latest advancements electrolyte technologies tailored specifically all‐climate operations comprehensively discussed. Particular emphasis is placed on unique role solvation structure interfacial offers valuable insights proposes directions practical implementation LMBs, contributing significantly existing knowledge base while concurrently paving way developing robust rigors environments.

Язык: Английский

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Active Diluent‐Anion Synergy Strategy Regulating Nonflammable Electrolytes for High‐Efficiency Li Metal Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(7)

Опубликована: Янв. 3, 2024

Abstract High‐energy Li metal batteries (LMBs) consisting of anodes and high‐voltage cathodes are promising candidates the next generation energy‐storage systems owing to their ultrahigh energy density. However, it is still challenging develop nonflammable electrolytes with superior anode cathode compatibility for LMBs. Here, we propose an active diluent‐anion synergy strategy achieve outstanding by using 1,2‐difluorobenzene (DFB) high activity yielding LiF as diluent regulate dimethylacetamide (DMAC)‐based localized concentration electrolyte (LHCE‐DFB). DFB bis(fluorosulfonyl)imide (FSI − ) anion cooperate construct robust LiF‐rich solid interphase (SEI) (CEI), which effectively stabilize DMAC from intrinsic reactions enhance interfacial stability LiNi 0.8 Co 0.1 Mn O 2 (NCM811) cathodes. LHCE‐DFB enables Coulombic efficiency (98.7 %), dendrite‐free, extremely stable long‐term cycling in || Cu cells cells. The fabricated NCM811 display remarkably enhanced excellent rate capability. This work provides a designing high‐energy batteries.

Язык: Английский

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Solvating lithium and tethering aluminium using di-coordination-strength anions for low-temperature lithium metal batteries

Energy & Environmental Science, Год журнала: 2024, Номер 17(12), С. 4036 - 4043

Опубликована: Янв. 1, 2024

Di-coordination-strength anions can simultaneously solvate lithium and tether aluminium in low-temperature metal batteries: the weakly coordinated anion exerts high ionic transport kinetics while strongly stabilizes surface.

Язык: Английский

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Weakly Coordinating Diluent Modulated Solvation Chemistry for High‐Performance Sodium Metal Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(21)

Опубликована: Март 16, 2024

Diluents have been extensively employed to overcome the disadvantages of high viscosity and sluggish kinetics high-concentration electrolytes, but generally do not change pristine solvation structure. Herein, a weakly coordinating diluent, hexafluoroisopropyl methyl ether (HFME), is applied regulate coordination Na

Язык: Английский

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Advanced Ether‐Based Electrolytes for Lithium‐ion Batteries

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Июль 14, 2024

Abstract Lithium‐ion batteries (LIBs) have emerged as vital elements of energy storage systems permeating every facet modern living, particularly in portable electronic devices and electric vehicles. However, with the sustained economic social development, new‐generation LIBs high density, wide operating temperature range, fast charge, safety are eagerly expected, while conventional ethylene carbonate (EC)‐based electrolytes fail to satisfy corresponding requirements. Comparatively, ether‐based electrolyte fascinating properties recently been revived fields, many advanced exciting performances under developed. This review provides an extensive overview latest breakthroughs concerning applied intercalation cathodes. To systematically outline progression electrolytes, this is categorized from perspective anodes follows: i) graphite anode‐based LIBs; ii) silicon iii) lithium metal LIBs.

Язык: Английский

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A Lithiophilic–Lithiophobic Gradient Solid Electrolyte Interface Toward a Highly Stable Solid‐State Polymer Lithium Metal Batteries

Advanced Functional Materials, Год журнала: 2024, Номер 34(27)

Опубликована: Март 7, 2024

Abstract The functional lithiophilic−lithiophobic gradient solid electrolyte interphase (SEI) between Li‐metal anode and solid‐state polymer electrolytes may be effective in addressing the long‐standing issue of side reactions Li‐dendrite growth during repeated deposition or dissolution polymer‐based high‐energy‐density batteries. Herein, a reliable lithiophilic–lithiophobic SEI (G‐SEI) LiAg‐LiF/Li 3 N is situ formed by AgTFSI, used as an additive for polyethylene oxide‐based (PEO‐Ag). upper layer consists lithiophobic LiF/Li N‐rich layer, wherein LiF possesses high interfacial energy, while Li enables fast + diffusion, which synergistically facilitates uniform . Lithiophilic Li–Ag alloy can effectively reduce nucleation overpotential promote more planar lithium. Furthermore, such G‐SEI mechanical modulus, mitigating penetration dendrites through thereby preventing continuous degradation PEO‐based electrolyte. As result, over three times improvement lifespan | PEO‐Ag LFP cell achieved, demonstrating 81.4% capacity retention rate after 500 cycles at 1C, compared to PEO with common SEI. Thus, developments lithiophilic‐lithiophobic provide substantial path toward high‐performance lithium

Язык: Английский

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Understanding the Inorganic‐Rich Feature of Anion‐Derived Solid Electrolyte Interphase

Advanced Energy Materials, Год журнала: 2024, Номер 14(21)

Опубликована: Март 10, 2024

Abstract Anion‐derived solid‐electrolyte interphase (SEI) has received growing attention owing to its appealing properties like fast ion transport and excellent passivation effect. However, a sophisticated understanding of anion‐derived SEI is lacking. To common wisdom, features an inorganic‐rich composition. Herein, it reveal that the freshly formed consists polymer‐rich outer layer inorganic inner layer. Then, organic components dissolve during discharge process, while species with low solubility are retained in empty husk. The accumulation husks cycling forms reacted lithium (Li) layer, which much higher content than newly SEI. Therefore, acknowledged “anion‐derived SEI” actually refers Li instead This work provides fruitful insights on compositional

Язык: Английский

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An Inorganic‐Dominate Molecular Diluent Enables Safe Localized High Concentration Electrolyte for High‐Voltage Lithium‐Metal Batteries

Advanced Functional Materials, Год журнала: 2022, Номер 33(6)

Опубликована: Ноя. 28, 2022

Abstract The development of high‐voltage Lithium‐metal batteries (LMBs) is hindered by suitable electrolytes that are simultaneously compatible with both cathodes and Li anodes. Herein, a novel localized high‐concentration electrolyte ethoxy(pentafluoro)cyclotriphosphazene (PFPN) as nonflammable diluent developed. inorganic‐dominate improves the safety organic electrolyte, helps to construct robust passivation interphases on electrodes. Specifically, PFPN accelerates complete reduction anions, leading stable anion‐derived interphase layer anode. Meanwhile, anions co‐participate in formation cathode‐electrolyte interphase, suppressing side reactions structural damage Ni‐rich cathodes. As result, PFPN‐based prolongs cycling life LMBs based LiNi 0.6 Co 0.2 Mn (NCM622) 0.8 0.1 (NCM811) Specially, 25‐µm‐thick paired NCM622 N/P ratio 1.3 (4.4 V) exhibits excellent capacity retention above 90% after 200 cycles. This study highlights important role tailoring electrode/electrolyte provides new strategy for designing high‐safety toward LMBs.

Язык: Английский

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