A Tetrahydropyran‐Based Weakly Solvating Electrolyte for Low‐Temperature and High‐Voltage Lithium Metal Batteries DOI Open Access

Zezhuo Li,

Yaqi Liao, Haijin Ji

et al.

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

Published: Dec. 17, 2024

Abstract Ether‐based electrolytes show great potential in low‐temperature lithium metal batteries (LMBs) for their low viscosity and decent reduction stability. However, conventional ethers with multidentate chelate sites suffer from oxidation stability high desolvation energy barrier due to the strong coordination between oxygen Li + . Herein, cyclic tetrahydropyran (THP) a unidentate site is designed as solvent, fluoroethylene carbonate (FEC) nitrate (LiNO 3 ) serve additives LMBs. The strain effect endow THP weak affinity ions, which accelerates process induces anion‐derived electrode/electrolyte interface at temperature. formed inorganic‐rich further improves expedites interfacial ion transportation. As result, assembled Li‐LiNi 0.8 Mn 0.1 Co O 2 (NMC811) cell stably cycles 87% capacity retention after 100 −40 °C 4.5 V. 2.7 Ah Li‐NMC811 pouch an density of 403 Wh kg −1 delivers 53% room‐temperature −50 °C. This work reveals that regulating solvents can well optimize realize

Language: Английский

Nonflammable Phosphate‐Based Electrolyte for Safe and Stable Potassium Batteries Enabled by Optimized Solvation Effect DOI

Dianwei Zhang,

Hongwei Fu,

Xuemei Ma

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(29)

Published: May 6, 2024

Abstract Current potassium‐ion batteries (PIBs) are limited in safety and lifetime owing to the lack of suitable electrolyte solutions. To address these issues, herein, we report an innovative non‐flammable design strategy that leverages optimal moderate solvation phosphate‐based solvent which strikes a balance between capability salt dissociation ability, leading superior electrochemical performance. The formulated simultaneously exhibits advantages low concentration (only 0.6 M), viscosity, high ionic conductivity, oxidative stability, safety. Our also promotes formation self‐limiting inorganic‐rich interphases at anode surface, alongside robust cathode‐electrolyte interphase on iron‐based Prussian blue analogues, mitigating electrode/electrolyte side reactions preventing Fe dissolution. Notably, PIBs employing our exhibit exceptional durability, with 80 % capacity retention after 2,000 cycles high‐voltage 4.2 V coin cell. Impressively, larger scale pouch cell, it maintains over 81 its initial 1,400 1 C‐rate average Coulombic efficiency 99.6 %. This work represents significant advancement toward realization safe, sustainable, high‐performance PIBs.

Language: Английский

Citations

34
Advanced Ether‐Based Electrolytes for Lithium‐ion Batteries DOI
Shizhu Wang, Jian‐Yu Shi, Zhenhui Liu

et al.

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

Published: July 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.

Language: Английский

Citations

19
Designing Current Collectors to Stabilize Li Metal Anodes DOI Creative Commons

Zhimeng Hao,

Yong Lü, Gaojing Yang

et al.

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

Published: Jan. 5, 2025

Rechargeable batteries employing Li metal anodes have gained increasing attention due to their high energy density. Nevertheless, low stability and reversibility of severely impeded practical applications. Designing current collectors (CCs) with reasonable structure composition is an efficient approach stabilizing the anodes. However, in-depth comprehensive understanding about design principles modification strategies CCs for realizing stable still lacking. Herein, a critical review focusing on rational summarized. First, requirements in are elucidated clarify objectives CCs. Then, including lithiophilic site modification, 3D architecture construction, protective layer crystalline plane engineering, as well corresponding highlighted. On this basis, recent progress development discussed. Finally, future directions suggested focus developing operando monitoring technology, designing cells under conditions close commercial This will spur more insightful researches toward advanced CCs, promote commercialization.

Language: Английский

Citations

3
Nonflammable Phosphate‐Based Electrolyte for Safe and Stable Potassium Batteries Enabled by Optimized Solvation Effect DOI

Dianwei Zhang,

Hongwei Fu,

Xuemei Ma

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(29)

Published: May 6, 2024

Abstract Current potassium‐ion batteries (PIBs) are limited in safety and lifetime owing to the lack of suitable electrolyte solutions. To address these issues, herein, we report an innovative non‐flammable design strategy that leverages optimal moderate solvation phosphate‐based solvent which strikes a balance between capability salt dissociation ability, leading superior electrochemical performance. The formulated simultaneously exhibits advantages low concentration (only 0.6 M), viscosity, high ionic conductivity, oxidative stability, safety. Our also promotes formation self‐limiting inorganic‐rich interphases at anode surface, alongside robust cathode‐electrolyte interphase on iron‐based Prussian blue analogues, mitigating electrode/electrolyte side reactions preventing Fe dissolution. Notably, PIBs employing our exhibit exceptional durability, with 80 % capacity retention after 2,000 cycles high‐voltage 4.2 V coin cell. Impressively, larger scale pouch cell, it maintains over 81 its initial 1,400 1 C‐rate average Coulombic efficiency 99.6 %. This work represents significant advancement toward realization safe, sustainable, high‐performance PIBs.

Language: Английский

Citations

12
Progresses on advanced electrolytes engineering for high-voltage lithium metal batteries DOI
S.H. Dai,

Wenqiang Fang,

Tianxiang Wang

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 500, P. 157269 - 157269

Published: Nov. 1, 2024

Language: Английский

Citations

4
Fast Charging Lithium Metal Battery Based on Lewis Acid/Base Dual-Site Solid Electrolyte Interphase DOI

Minjian Li,

Lianzhan Huang,

Boyong Wu

et al.

Energy storage materials, Journal Year: 2025, Volume and Issue: unknown, P. 104069 - 104069

Published: Jan. 1, 2025

Language: Английский

Citations

0
Effects of Li+ Solvation Structures on Aluminum Corrosion in Ether‐Based Electrolyte Solutions with Lithium Bis(Fluorosulfonyl)imide (LiFSI) DOI Open Access
Taegyu Jang,

Seon Yeong Cho,

Jaegeol Kim

et al.

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

Published: Feb. 16, 2025

Abstract Lithium bis(fluorosulfonyl)imide (LiFSI) is widely used in lithium‐metal batteries to form a stable lithium fluoride (LiF)‐based solid electrolyte interphase (SEI). However, the FSI⁻ itself fails create protective passivation layer on aluminum (Al) current collectors, leading Al 3 ⁺ dissolution and severe corrosion. While fluorinated ether solvents have shown promise mitigating corrosion, mechanisms remain unclear. Here, role of cation solvations ion pairing structures corrosion mitigation. 2,2,3,3‐tetrafluoro‐1,4‐dimethoxybutane (FDMB), 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropyl (TTE)/1,2‐dimethoxyethane (DME) mixture, non‐fluorinated ethers are evaluated 1 m LiFSI. FDMB promoted formation AlF₃ while preventing under extreme conditions (e.g., 4.5 V vs Li/Li⁺, 60 °C). Electrochemical DFT analyses showed that underwent favorable defluorination coordination with both Li⁺ arose from oxidizing surface. Meanwhile, aggregated pairs between Li + inhibited generation soluble 3+ species coordinated FSI − . Modifying alkyl chains further enhanced anti‐corrosive effects by reducing solubility species. In contrast, DME/TTE exhibited more similar tetraethylene glycol dimethyl (TEGDME), due less limited solvation TTE.

Language: Английский

Citations

0
Unveiling the Formation and Electrochemical Properties of Nano‐Clusters in Lithium Battery Electrolyte Induced by Nitrate Ion DOI Creative Commons

Jingwei Zhang,

Jia Li, Yawen Li

et al.

Energy & environment materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

LiNO 3 is known to significantly enhance the reversibility of lithium metal batteries; however, modification solvation structures in various solvents and its further impact on interface have not been fully revealed. Herein, we systematically studied evolution with increasing concentration both carbonate ether electrolytes. The results from molecular dynamics simulations unveil that Li + structure less affected electrolytes, while there a significant decrease solvent molecules coordination, larger average size emerges as increases. Notably, formation large ion aggregates several nanometers (nano‐clusters), observed ether‐based electrolytes at conventional (1 m ) higher ratio, which proved by infrared spectroscopy small‐angle X‐ray scattering experiments. nano‐clusters abundant anions are endowed narrow energy gap orbitals, contributing an inorganic rich electrode/electrolyte interphase enhances stripping/plating Coulombic efficiency up 99.71%. discovery elucidates underlying mechanism linking ions/solvent aggregation states interfacial stability advanced battery systems.

Language: Английский

Citations

0
A molecular review on weakly solvating electrolytes for lithium batteries DOI

Yao‐Peng Chen,

Xiang Chen, Nan Yao

et al.

Materials Today, Journal Year: 2025, Volume and Issue: unknown

Published: March 1, 2025

Language: Английский

Citations

0
Regulating Amine Substitution in Fluorosulfonyl-Based Flame-Retardant Electrolytes for Energy-Dense Lithium Metal Batteries DOI

Lan‐Qing Wu,

Zhe Li, Huamei Li

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Sulfone-based electrolytes offer unusually high anodic and thermal stability that in principle makes them promising candidates for fabricating energy-dense lithium metal batteries (LMBs). Their uses practical are currently limited by their inability to sustain long-term Li plating/stripping processes due reactivity toward the metal. Here, we report on design synthesis of a unique family fluorosulfonyl group-based (FSO2-) molecules, modified with ethyl (FSE)/N,N-dimethyl (FSNDM)/N,N-diethyl (FSNDE)/N-pyrrolidine (FSNP) end groups create exceptionally stable single-salt single-solvent electrolytes. The flammability, solvation structure, ion transport, deposition kinetics, high-voltage systematically studied. It is shown nonflammable, possess weak characteristics, yet manifest room-temperature ionic conductivities (1.6-6.1 mS cm-1) low solution viscosities. In comparison FSE, FSNDM-, FSNDE-, FSNP-based exhibit an reversible Coulombic efficiency (>99.71% over 800 cycles) typical oxidative at voltages exceeding 4.6 V. Deployed as (20 μm anode 3 g A h-1 electrolyte) high-loading (18.5 mg cm-2) LiNi0.8Co0.1Mn0.1O2 cathodes, 329 cycles have been achieved before 80% capacity retention. Six Ah pouch cells based designed also energy density (496 W h kg-1) 150 most 2.7% volume expansion. Our findings demonstrate through intentional molecular design, sulfone provide robust route nonflammable compatible cathodes.

Language: Английский

Citations

0