Electrolyte Engineering via Fluorinated Siloxane Solvent for Achieving High-Performance Lithium-Metal Batteries

ACS Nano, Journal Year: 2024, Volume and Issue: 18(24), P. 15802 - 15814

Published: June 4, 2024

Advanced solvent is of important significance to develop an excellent electrolyte that simultaneously maintains a high ionic conductivity, wide electrochemical window, and good compatibility with electrodes for high-performance lithium-metal batteries (LMBs). To realize stable electrode/electrolyte interface uniform lithium (Li) deposition process, optimal fluorinated siloxane (3,3,3-trifluoropropyltrimethoxysilane, TFTMS) proposed as cosolvent 1,2-dimethoxyethane (DME) highly antioxidative fluoroethylene carbonate (FEC) formulate Li-metal electrolyte. The TFTMS-based presents oxidization stability, Li+ transfer number, contributing the accelerated reaction kinetics, homogeneous Li behavior, interfacial chemistry. Therefore, stripping/plating reversibility (∼99%) cycling (1400 h) are achieved in electrolyte, giving rise performance practical full cells. Moreover, industrial 4 Ah NCM811|Gr pouch cell demonstrated display similar commercial 120 cycles at 1 C. This work offers approach toward LMBs through rational design solvent.

Language: Английский

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A Weakly Solvating Ether Electrolyte Enables Fast-Charging and Wide-Temperature Lithium-Ion Pouch Cells

ACS Nano, Journal Year: 2024, Volume and Issue: 18(31), P. 20762 - 20771

Published: July 27, 2024

Graphite-based lithium-ion batteries have succeeded greatly in the electric vehicle market. However, they suffer from performance deterioration, especially at fast charging and low temperatures. Traditional electrolytes based on carbonated esters sluggish desolvation kinetics, recognized as rate-determining step. Here, a weakly solvating ether electrolyte with tetrahydropyran (THP) solvent is designed to enable reversible (Li+) intercalation graphite anode. Unlike traditional ether-based which easily cointercalate into layers, THP-based shows ability can match well In addition, weak interconnection between Li+ THP allows more anions come shell of Li+, inducing an inorganic-rich interface thus suppressing side reactions. As result, lithium iron phosphate/graphite pouch cell (3 Ah) capacity retention 80.3% after 500 cycles 2 C charging, much higher than that ester system (7.6% 200 cycles). At 4 discharging increased 2.29 Ah 2.96 THP. Furthermore, work normally over wide working temperatures (-20 60 °C). Our design provides some understanding

Language: Английский

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Achieving Ultra‐Thin Solid Electrolyte Interphase for High‐Performance Lithium Metal Anodes via Chloride‐Assisted Electrochemical Corrosion

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

Published: April 26, 2025

Abstract The thickness and composition of the solid electrolyte interphase (SEI) on lithium (Li) metal are critical factors influencing dendrite growth. This study introduces a novel selection strategy based electrochemical corrosion principles. By employing LiCl LiNO 3 simultaneously, itself has high donor number, low desolvation energy, Li⁺ transference number conductivity, moderate stability window. In addition, it dynamically reduces SEI reactivates dead Li, forming ≈100 nm enriched with LiF Li 2 O anode, which ensures stable cycling symmetric cells for 2000 h at current density 5 mA cm⁻ . Consequently, using LiFePO 4 (LFP) as cathode ‐LiCl‐added exhibit excellent performance 1600 cycles 680 g⁻ 1 Even thin (5 µm)|LFP cell retains 95% capacity after 70 170 universality feasibility this design also validated in diverse battery chemistries such anode‐free Cu|LFP, Li|LiNi 0.8 Mn 0.1 Co (NMC811), Li|S cells, well pouch high‐loading LFP NMC811 cathodes, showcasing promising batteries.

Language: Английский

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Anionic Aggregates Induced Interphase Chemistry Regulation toward Wide‐Temperature Silicon‐Based Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(40)

Published: July 22, 2024

Abstract Silicon nanoparticles (SiNPs) show great promise as high‐capacity anodes owing to their ability mitigate mechanical failure. However, the substantial surface area of SiNPs triggers interfacial side reactions and solid electrolyte interphase (SEI) permeation during volume fluctuations. The slow kinetics at low temperatures degradation SEI high further hinder practical application in real‐world environments. Here, these challenges are addressed by manipulating solvation structure through molecular space hindrance. enables anions aggregate outer Helmholtz layer under an electric field, leading rapid desolvation capabilities formation anion‐derived SEI. resulting double‐layer SEI, where inorganic nano‐clusters uniformly dispersed amorphous structure, completely encapsulates particles first cycle. ultra‐high modulus this can withstand stress accumulation, preventing penetration repeated expansion contraction. As a result, SiNPs‐based batteries demonstrate exceptional electrochemical performance across wide temperature range from −20 60 °C. Moreover, assembled 80 mAh SiNPs/LiFePO 4 pouch cells maintain cycling retention 85.6% after 150 cycles, marking significant step forward silicon‐based batteries.

Language: Английский

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Interfacial Chemistry Design for Hybrid Lithium‐Ion/Metal Batteries Under Extreme Conditions

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(29)

Published: May 2, 2024

Abstract The storage behavior of Li ions in the anode limits energy density full cell. Storing entirely as sacrifices while storing metal shortens cycle life. hybrid maximizes both and lifespan through good candidate interface engineering. In this work, is tailored carbon film (CF) a Li‐ion/metal to reduce consumption at low N/P ratios. A series weakly solvating electrolytes are screened enhance intercalation ability CF inducing highly reversible plating/stripping. Among them, 1 m LiFSI‐THF‐0.5 wt.%LiNO 3 electrolyte achieves interfacial barrier, allowing not only have highest capacity 236.5 mAh g −1 , but also exhibit excellent cycling stability high Coulombic efficiency, even fast charging temperature. NCM811||CF cell with ratio 0.5 delivers 527.3 25 °C, 381.5 −20 achieving densities 312.6 223.7 Wh kg respectively. 100 pouch can be cycled stably over 500 cycles, retention 83.0%.

Language: Английский

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Rational Molecular Engineering via Electron Reconfiguration toward Robust Dual-Electrode/Electrolyte Interphases for High-Performance Lithium Metal Batteries

ACS Nano, Journal Year: 2024, Volume and Issue: 18(22), P. 14764 - 14778

Published: May 22, 2024

High-energy-density lithium-metal batteries (LMBs) coupling anodes and high-voltage cathodes are hindered by unstable electrode/electrolyte interphases (EEIs), which calls for the rational design of efficient additives. Herein, we analyze effect electron structure on coordination ability energy levels additive, from aspects intramolecular cloud density delocalization, to reveal its mechanism solvation structure, redox stability, as-formed EEI chemistry, electrochemical performances. Furthermore, propose an reconfiguration strategy molecular engineering additives, taking sorbide nitrate (SN) additive as example. The lone pair electron-rich group enables strong interaction with Li ion regulate delocalization yields further positive synergistic effects. electron-withdrawing moiety decreases ether-based backbone, improving overall oxidation stability cathode compatibility, anchoring it a reliable cathode/electrolyte interface (CEI) framework integrity. In turn, electron-donating bicyclic-ring-ether backbone breaks inherent resonance nitrate, facilitating reducibility form N-contained inorganic Li2O-rich solid electrolyte (SEI) uniform deposition. Optimized physicochemical properties interfacial biaffinity enable significantly improved performance. High rate (10 C), low temperature (-25 °C), long-term (2700 h) achieved, 4.5 Ah level Li||NCM811 multilayer pouch cell under harsh conditions is realized high (462 W h/kg). proof concept this work highlights that ingenious based regulation represents energetic modulate interphase providing realistic reference innovations practical LMBs.

Language: Английский

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Enhancing stable LiF-rich interface formation of polyester based electrolyte using fluoroethylene carbonate for quasi-solid state lithium metal batteries

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 67, P. 608 - 617

Published: April 23, 2024

Language: Английский

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The Ether’s Chain Length Effect in Electrolyte for Hard carbon towards Efficient Sodium Storage at Low Temperature

Nano Energy, Journal Year: 2024, Volume and Issue: 132, P. 110362 - 110362

Published: Oct. 12, 2024

Language: Английский

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Unlocking the potential of Mg-ion batteries: Cu2C MXene anode with ultrahigh storage and energy density with rapid Mg diffusion

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 498, P. 155368 - 155368

Published: Aug. 31, 2024

Language: Английский

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Electrolyte Design Enables Stable and Energy‐dense Potassium‐ion Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 10, 2024

Abstract Free from strategically important elements such as lithium, nickel, cobalt, and copper, potassium‐ion batteries (PIBs) are heralded promising low‐cost sustainable electrochemical energy storage systems that complement the existing lithium‐ion (LIBs). However, reported performance of PIBs is still suboptimal, especially under practically relevant battery manufacturing conditions. The primary challenge stems lack electrolytes capable concurrently supporting both low‐voltage anode high‐voltage cathode with satisfactory Coulombic efficiency (CE) cycling stability. Herein, we report a electrolyte facilitates commercially mature graphite (>3 mAh cm −2 ) to achieve an initial CE 91.14 % (with average around 99.94 %), fast redox kinetics, negligible capacity fading for hundreds cycles. Meanwhile, also demonstrates good compatibility 4.4 V ( vs . K + /K) 2 Mn[Fe(CN) 6 ] (KMF) cathode. Consequently, KMF||graphite full‐cell without precycling treatment electrodes can provide discharge voltage 3.61 specific 316.5 Wh kg −1 −(KMF+graphite), comparable LiFePO 4 ||graphite LIBs, maintain 71.01 retention after 2000

Language: Английский

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