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

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Май 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.

Язык: Английский

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

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Май 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.

Язык: Английский

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