Stabilizing Residual Monomers within In Situ Polymerized Electrolytes for High-Voltage Lithium Metal Batteries DOI
Zhenzhong Sun, Jinlin Yang, Yao Wu

et al.

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

Published: May 16, 2025

Poly(1,3-dioxolane) (PDOL)-based electrolyte has gained wide attention due to its high compatibility with the lithium metal anode, intimate contact electrodes, and ionic conductivity. However, application in high-voltage batteries is limited because residual DOL monomers are prone oxidation at voltage. Here, we report that LiDFOB-initiated situ polymerization stabilizes these monomers, thus overcoming oxidation-related limitations of PDOL-based electrolytes. This approach promotes formation a thermodynamically stable Li+-DOL-DFOB- solvation structure DOL-PDOL clusters, reducing oxidative decomposition extending electrochemical stability window up 5.0 V vs Li+/Li. It also enhances conductivity (4.39 mS cm-1), facilitates uniform, F-rich cathode-electrolyte interphase. Electrochemical tests computational simulations reveal reduced Li+-PDOL interactions designed PDOL promote higher mobility stability. Consequently, Li||LiCoO2 cells using exhibit remarkable cycling performance, maintaining 80% capacity retention over 760 cycles cut-off voltage 4.35 V. These findings establish as transformative for batteries.

Language: Английский

In Situ Polymerized Polyfluorinated Crosslinked Polyether Electrolytes for High‐Voltage Lithium Metal Batteries DOI Creative Commons
Shimei Li, Hu Hong,

Xinru Yang

et al.

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

Published: May 2, 2025

Abstract In situ polymerized polyether electrolytes are promising for solid‐state Li metal batteries due to their high ionic conductivity and excellent interfacial contact. However, practical application is hindered by dendrite formation, degradation, limited oxidative stability. Herein, we propose an in polyfluorinated crosslinked electrolyte (PDOL‐OFHDBO), synthesized copolymerizing 1,3‐dioxolane (DOL) with 2,2′‐(2,2,3,3,4,4,5,5‐octafluorohexane‐1,6‐diyl)bis(oxirane) (OFHDBO) as a crosslinker. The electron‐withdrawing groups endow PDOL‐OFHDBO enhanced stability compatibility, while reducing the solvation power of polymer matrix promote anion‐derived inorganic‐rich solid interphase uniform deposition. Consequently, exhibits wide electrochemical window (>5.6 V) enables long‐term stable plating/stripping over 1100 h. Furthermore, Li||LiNi 0.8 Co 0.1 Mn O 2 (NCM811) full cells utilizing demonstrate outstanding cycling high‐loading cathodes (≈3.8 mAh cm −2 ) thin anodes (50 µm), achieving capacity retention 95.5% 89.1% 100 cycles at cut‐off voltages 4.3 4.5 V, respectively. Remarkably, Ah‐level Li||NCM811 pouch deliver impressive specific energy 401.8 Wh kg −1 , highlighting potential batteries.

Language: Английский

Citations

0
Stabilizing Residual Monomers within In Situ Polymerized Electrolytes for High-Voltage Lithium Metal Batteries DOI
Zhenzhong Sun, Jinlin Yang, Yao Wu

et al.

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

Published: May 16, 2025

Poly(1,3-dioxolane) (PDOL)-based electrolyte has gained wide attention due to its high compatibility with the lithium metal anode, intimate contact electrodes, and ionic conductivity. However, application in high-voltage batteries is limited because residual DOL monomers are prone oxidation at voltage. Here, we report that LiDFOB-initiated situ polymerization stabilizes these monomers, thus overcoming oxidation-related limitations of PDOL-based electrolytes. This approach promotes formation a thermodynamically stable Li+-DOL-DFOB- solvation structure DOL-PDOL clusters, reducing oxidative decomposition extending electrochemical stability window up 5.0 V vs Li+/Li. It also enhances conductivity (4.39 mS cm-1), facilitates uniform, F-rich cathode-electrolyte interphase. Electrochemical tests computational simulations reveal reduced Li+-PDOL interactions designed PDOL promote higher mobility stability. Consequently, Li||LiCoO2 cells using exhibit remarkable cycling performance, maintaining 80% capacity retention over 760 cycles cut-off voltage 4.35 V. These findings establish as transformative for batteries.

Language: Английский

Citations

0