Achieving High‐Performance Lithium–Sulfur Batteries by Modulating Li+ Desolvation Barrier with Liquid Crystal Polymers DOI
Xiang Miao, Chenxi Song, Weisheng Hu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(29)

Published: April 25, 2024

Abstract Lithium–sulfur (Li–S) batteries offer high theoretical capacity but are hindered by poor rate capability and cycling stability due to sluggish Li 2 S precipitation kinetics. Here a sulfonate‐group‐rich liquid crystal polymer (poly‐2,2′‐disulfonyl‐4,4′‐benzidine terephthalamide, PBDT) is designed fabricated accelerate promoting the desolvation of + from electrolyte. PBDT‐modified separators employed assemble Li–S batteries, which deliver remarkable (761 mAh g −1 at 4 C) (500 cycles with an average decay 0.088% per cycle 0.5 C). A PBDT‐based pouch cell even delivers exceptional ≈1400 areal ≈11 cm −2 under lean‐electrolyte high‐sulfur‐loading condition, demonstrating promise for practical applications. Results Raman spectra, molecular dynamic (MD) density functional theory (DFT) calculations reveal that abundant anionic sulfonate groups PBDT aid in attenuating ‐solvent interactions lowering energy barrier. Plus, polysulfide adsorption/catalysis also excluded via electrostatic repulsion. This work elucidates critical impact on provides new design direction advanced batteries.

Language: Английский

Green Ether Electrolytes for Sustainable High‐voltage Potassium Ion Batteries DOI

Xuemei Ma,

Hongwei Fu, Jingyi Shen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Oct. 17, 2023

Ether-based electrolytes are promising for secondary batteries due to their good compatibility with alkali metal anodes and high ionic conductivity. However, they suffer from poor oxidative stability toxicity, leading severe electrolyte decomposition at voltage biosafety/environmental concerns when leakage occurs. Here, we report a green ether solvent through rational design of carbon-chain regulation elicit steric hindrance, such structure significantly reducing the solvent's biotoxicity tuning solvation electrolytes. Notably, our is versatile, an anion-dominated favored, facilitating stable interphase formation on both anode cathode in potassium-ion batteries. Remarkably, ether-based demonstrates excellent K graphite 4.2 V high-voltage (200 cycles average Coulombic efficiency 99.64 %). This work points path toward molecular practical other rechargeable

Language: Английский

Citations

84
Weakly solvating electrolytes for next-generation lithium batteries: design principles and recent advances DOI Creative Commons
Zhijie Wang, Biao Zhang

Energy Materials and Devices, Journal Year: 2023, Volume and Issue: 1(1), P. 9370003 - 9370003

Published: Sept. 1, 2023

Lithium batteries play a dominant role in the power source market of electric vehicles and portable electronic devices. The electrolyte is critical to determining performance lithium batteries. Conventional electrolytes cannot meet ever-growing demands fast-charging, wide-temperature operation, safety properties Despite great success (localized) high-concentration electrolytes, they still suffer from disadvantages like low ionic conductivity high cost. emerging weakly solvating also known as low-solvating offer another solution these challenges have attracted intensive research interests recent years. This contribution reviews working mechanisms, design principles, advances developing electrolytes. A summary perspective about future directions this field provided. insights will benefit both academic industrial communities designing safe high-performance next-generation Li

Language: Английский

Citations

71
Unique Tridentate Coordination Tailored Solvation Sheath Toward Highly Stable Lithium Metal Batteries DOI

Junru Wu,

Ziyao Gao,

Yao Tian

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(38)

Published: June 7, 2023

Electrolyte optimization by solvent molecule design is recognized as an effective approach for stabilizing lithium (Li) metal batteries. However, the coordination pattern of Li ions (Li+ ) with molecules sparsely considered. Here, electrolyte strategy reported based on bi/tridentate chelation Li+ and to tune solvation structure. As a proof concept, novel multi-oxygen sites demonstrated facilitate formation anion-aggregated shell, enhancing interfacial stability de-solvation kinetics. result, as-developed exhibits ultra-stable cycling over 1400 h in symmetric cells 50 µm-thin foils. When paired high-loading LiFePO4 , full maintain 92% capacity 500 cycles deliver improved electrochemical performances wide temperature range from -10 60 °C. Furthermore, concept validated pouch cell (570 mAh), achieving retention 99.5% after 100 cycles. This brand-new insight engineering provides guidelines practical high-performance

Language: Английский

Citations

53
Non-Flammable Electrolyte Mediated by Solvation Chemistry toward High-Voltage Lithium-Ion Batteries DOI
Haoran Cheng, Zheng Ma, Pushpendra Kumar

et al.

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

Citations

53
More is better: high-entropy electrolyte design in rechargeable batteries DOI
Xin Zhao, Zhiqiang Fu, Xiang Zhang

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(7), P. 2406 - 2430

Published: Jan. 1, 2024

This review conducts a comprehensive survey of the high-entropy effect on key properties electrolytes. The applications electrolytes in various rechargeable batteries are presented to address their critical drawbacks.

Language: Английский

Citations

48
Co-Intercalation-Free Ether-Based Weakly Solvating Electrolytes Enable Fast-Charging and Wide-Temperature Lithium-Ion Batteries DOI
Zhicheng Wang, Ran Han, Dan Huang

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(18), P. 18103 - 18113

Published: Sept. 7, 2023

Ether-based electrolytes are competitive choices to meet the growing requirements for fast-charging and low-temperature lithium-ion batteries (LIBs) due low viscosity melting point of ether solvents. Unfortunately, graphite (Gr) electrode is incompatible with commonly used solvents their irreversible co-intercalation into Gr interlayers. Here, we propose cyclopentyl methyl (CPME) as a co-intercalation-free solvent, which contains cyclopentane group large steric hindrance obtain weakly solvating power Li+ wide liquid-phase temperature range (-140 +106 °C). A electrolyte (WSE) based on CPME fluoroethylene carbonate (FEC) cosolvents can simultaneously achieve fast desolvation ability high ionic conductivity, also induces LiF-rich solid interphase (SEI) anode. Therefore, Gr/Li half-cell this WSE deliver outstanding rate capability, stable cycling performance, specific capacity (319 mAh g-1) at an ultralow -60 °C. Furthermore, practical LiFePO4 (loading ≈25 mg cm-2)/Gr ≈12 cm-2) pouch cell reveals capability long-term performance above 1000 cycles Coulombic efficiency (≈99.9%) achieves impressive application potential

Language: Английский

Citations

47
Building Stable Anodes for High‐Rate Na‐Metal Batteries DOI
X.D. Wang, Jingyu Lu,

Yehui Wu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 5, 2024

Due to low cost and high energy density, sodium metal batteries (SMBs) have attracted growing interest, with great potential power future electric vehicles (EVs) mobile electronics, which require rapid charge/discharge capability. However, the development of high-rate SMBs has been impeded by sluggish Na

Language: Английский

Citations

41
A Low‐Cost, Fluorine‐Free Localized Highly Concentrated Electrolyte Toward Ultra‐High Loading Lithium Metal Batteries DOI
Feng Hai,

Yikun Yi,

Zichun Xiao

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(17)

Published: Feb. 21, 2024

Abstract Localized highly concentrated electrolytes have revitalized the advancement of secondary batteries. However, fluorinated diluents typically drawbacks high toxicity, serious environmental pollution, challenging synthesis, and cost. This work develops a low‐cost, eco‐friendly localized electrolyte by utilizing benzene as diluent, simultaneously achieving reversible lithium‐metal anodes long‐term stable cycling single crystal LiNi 0.8 Co 0.1 Mn O 2 (SC811) cathode. The unique conjugated structure absence electron‐withdrawing groups provide decent redox stability inertness, which enables it to modulate solvation structure. PhH‐LHCE supports SC811‐Li cells with cathode loading 9 mg cm −2 87.3% capacity retention after 450 cycles. Cells consisting ultra‐high Ni83 (≈31 ) ultra‐thin Li (50 µm) anode achieve 70 cycles lean condition. can be generalized promising electrochemical energy storage systems such sodium potassium metal batteries solve cost pollution problems in large‐scale production process.

Language: Английский

Citations

25
Intermolecular Interaction Mediated Potassium Ion Intercalation Chemistry in Ether‐Based Electrolyte for Potassium‐Ion Batteries DOI

Hongliang Xie,

Honghong Liang,

Pushpendra Kumar

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(28)

Published: June 4, 2024

Abstract Electrolyte design is indeed a highly effective strategy to improve battery performance. However, identifying the intermolecular interaction in electrolyte solvation structure rarely reported potassium‐ion batteries. Herein, it discovered that solvent‐solvent can be formed when introducing cyclopentylmethyl ether (CPME) solvent into commonly used 1,2‐dimethoxyethane (DME)‐based electrolytes. Such not only analyzed by 2D 1 H‐ H correlation spectroscopy for first time but also found weaken K + ‐DME significantly, consequently enabling reversible (de‐)intercalation within graphite. By employing this without using any fluorine‐based solvent, new fluorine‐free and low‐concentration ether‐based designed, which compatible with graphite facilitates of high‐energy‐density safe potassium ion sulfur A novel molecular interfacial model further presented analyze behaviors ‐solvent‐anion complexes on electrode surface are affected interactions, elucidating reasons behind superior compatibility performance at scale. This work sheds some light critical role solvent–solvent interactions batteries provides valuable insights engineering enhancing electrolytes

Language: Английский

Citations

22
Solvating lithium and tethering aluminium using di-coordination-strength anions for low-temperature lithium metal batteries DOI

Jinxiu Chen,

Jinhao Zhang, Xiao-Zhong Fan

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(12), P. 4036 - 4043

Published: Jan. 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.

Language: Английский

Citations

19