Multi‐Effect Ionic Liquid Additives Achieve High Cycle Stability Lithium‐Sulfur Batteries by Constructing an Electrostatic Shielding Layer and Eliminating ‘Dead Sulfur’

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

Published: March 7, 2025

Abstract Lithium‐sulfur (Li‐S) batteries are considered the most promising alternative for energy storage, however, their practical applications still limited by lithium dendrites growth, slow polysulfides (LiPSs) conversion kinetics, shuttle effect, and deposition of “dead sulfur” at Li anode surface. Herein, a novel ionic liquid tetrabutylammonium triiodide (TBAI 3 ) is adopted as multi‐effect electrolyte additive to solve low coulombic efficiency short life issues Li‐S batteries. A series in situ characterization technologies, theoretical calculations, potentiostatic 2 S experiments, different kinds symmetric asymmetric cells conducted reveal multifunctional electrochemical work mechanism. It found that TBA + cations can coordinate with solvent molecules, reduce desolvation barrier, accelerate transport kinetics; they also form dynamic electrostatic shielding layer protrusions induce uniform deposition. The I − /I redox pairs continuously eliminate transforming deposits into soluble LiPSs release active substances during cycling, while reduzate be electrochemically rejuvenated when charged 2.89 V. Therefore, TBAI additives exhibit ultra‐long cycle performance 503 mAh g −1 C after 1000 cycles an average 99.99%.

Language: Английский

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Revealing the Coordination and Mediation Mechanism of Arylboronic Acids Toward Energy‐Dense Li‐S Batteries

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

Published: March 27, 2025

Lithium-sulfur (Li─S) batteries offer a promising avenue for the next generation of energy-dense batteries. However, it is quite challenging to realize practical Li─S under limited electrolytes and high sulfur loading, which may exacerbate problems interface deterioration low utilization. Herein, coordination mediation chemistry arylboronic acids that enable long-term-cycling proposed. The between NO3 - breaks resonance configuration thermodynamically promotes its reduction on anode, contributing mechanically robust interface. lithium arylborate polysulfides distorts S─S/Li─S bonds, alters rate-determining step from Li2S4→Li2S2 Li2S6→Li2S4, homogeneously accelerates redox kinetics. using 3,5-bis(trifluoromethyl)phenylboronic acid (BPBA) show excellent cycling stability (1000 cycles with capacity decay rate 0.033% per cycle) energy density 422 Wh kg-1 aggressive chemical environments (high loading 17.4 mg cm-2 lean electrolyte operation 3.6 mL gS -1). basic mechanism can be extended other different configurations compositions, thus broadening application prospect in engineering

Language: Английский

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Optimization of Zinc and Aluminum Hydroxyquinolines for Applications as Semiconductors in Molecular Electronics

Molecules, Journal Year: 2025, Volume and Issue: 30(9), P. 1896 - 1896

Published: April 24, 2025

This work explores the dispersed heterojunction of tris-(8-hydroxyquinoline) aluminum (AlQ3) and 8-hydroxyquinoline zinc (ZnQ2) with tetracyanoquinodimethane (TCNQ) 2,6-diaminoanthraquinone (DAAq). Thin films these organic semiconductors were deposited analyzed, their structures calculated B3PW91/6-31G** method. The optimized structure for AlQ3-TCNQ, AlQ3-DAAq, is achieved by means three hydrogen bonds, whereas ZnQ2-DAAq, two interactions are predicted. These recalculated including GD3 dispersion term. A stable ordering was also AlQ3-TCNQ-GD3, AlQ3-DAAq-GD3, ZnQ2-DAAq-GD3 four contacts former latter, respectively. Infrared (IR) UV-visible spectroscopy confirmed theoretical predictions, in addition to obtaining optical band gap films. values ranged between 1.62 2.97 eV (theoretical) 2.46 2.87 (experimental). Additional parameters electrical behavior obtained, which indicates potential be used as semiconductors. All showed transmittance above 76%, broadens range applications electrodes, transparent transistors, or photovoltaic cells. Devices fabricated using materials displayed ohmic behavior, peak current 2 × 10−3 6 A.

Language: Английский

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Tuning the Solvation Structure of a Weakly Solvating Cyclic Ether Electrolyte for Wide‐Temperature Cycling of Lithium‐Sulfurized Polyacrylonitrile Batteries

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

Published: Oct. 21, 2024

Abstract Sulfurized polyacrylonitrile (SPAN) cathodes in high energy‐density Li‐metal batteries have garnered widespread interest owing to their good cycling stability and moderately capacities. However, application is hindered by the low prevalence of advanced electrolytes that can simultaneously mitigate polysulfide generation at cathode stabilize anode. Here, a weakly solvating electrolyte presented, employing single solvent tetrahydropyran (THP). The solvation structure effectively tuned adjusting salt concentration both anode SPAN cathode. This approach enables stable with loadings (≈5 mg cm −2 ) lean contents µL −1 across wide temperature range: 0 °C, room temperature, 50 °C. A pouch cell loading electrolyte‐to‐SPAN (E/SPAN) ratio 3 shows 79.1% capacity retention after 40 cycles. Additionally, THP be employed localized high‐concentration (LHCE) systems reduce diluent‐to‐solvent for greater LHCE viability. study demonstrates potential solvents Li‐SPAN batteries, offering pathway practical application.

Language: Английский

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Long-life Graphite – Lithium Sulfide Full Cells Enabled through a Solvent Co-intercalation-free Electrolyte Design

Materials Horizons, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 19, 2024

Graphite (Gr) is the predominant anode material for current lithium-ion technologies. The Gr could offer a practical pathway development of lithium-sulfur (Li-S) batteries due to its superior stability and safety compared Li-metal. However, anodes are not compatible with conventional dilute ether-based electrolytes typically used in Li-S systems. Here, an optimized ether electrolyte presented, utilizing 1 M lithium bis(trifluoromethanesulfonyl)-imide (LiTFSI) 1,3-dioxolane (DOL)/1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropylether (TTE). Without altering salt concentration, this regulates solvation structure promotes formation robust solid-electrolyte interphase (SEI) layer, leading significant improvement cyclability anodes. Meanwhile, DOL/TTE maintains adequate kinetics sulfur cathode, enabling pairing without any cathode modification. cell delivers reversible discharge capacity 515 mA h g

Language: Английский

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Synergistic Regulation of Bidirectional Conversion of LiPSs and Li₂S Using Anthraquinone as a Redox Mediator

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 20, 2024

Lithium–sulfur (Li–S) batteries are strong contenders as energy storage options in the next-generation, primarily because of their potential for delivering high densities. Nonetheless, widespread commercialization faces several obstacles, including sluggish sulfur redox kinetics, insulating properties Li2S discharge product, and significant reaction barriers. In this work, anthraquinone (AQ) was introduced a mediator incorporated onto Co-doped carbon materials through π–π interactions. The results showed that synergistic effect between AQ Co atoms facilitated bidirectional conversion lithium polysulfides (LiPSs) Li2S. During charging, lowered barrier oxidation thereby enhanced reversibility reactions. Density functional theory (DFT) calculations AQ-Li2Sx exhibits lower lowest unoccupied molecular orbital (LUMO) higher highest occupied (HOMO). Experimental demonstrated an impressive initial specific capacity 1290 mAh g–1 achieved by fabricated S@AQ/Co–N–C electrode at 0.1 C. After 600 cycles 1 C, it retained 64% exhibited minimal 0.06% decay rate per cycle.

Language: Английский

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