Anion-modulated Ion Conductor with Chain Conformational Transformation for stabilizing Interfacial Phase of High-Voltage Lithium Metal Batteries

Chao Wang, Xiaoxue Zhao, Dabing Li, Chong Yan, Qiang Zhang*, Li Zhen Fan*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

11 Citations (Scopus)

Abstract

In solid-state lithium metal batteries (SSLMBs), the inhomogeneous electrolyte-electrode interphase layer aggravates the interfacial stability, leading to discontinuous interfacial ion/charge transport and continuous degradation of the electrolyte. Herein, we constructed an anion-modulated ionic conductor (AMIC) that enables in situ construction of electrolyte/electrode interphases for high-voltage SSLMBs by exploiting conformational transitions under multiple interactions between polymer and lithium salt anions. Anions modulate the decomposition behavior of supramolecular poly (vinylene carbonate) (PVC) at the electrode interface by changing the spatial conformation of the polymer chains, which further enhances ion transport and stabilizes the interfacial morphology. In addition, the AMIC weakens the “Li+-solvation” and increases Li+ vehicle sites, thereby enhancing the lithium-ion transport number (tLi+=~0.67). Consequently, Li || LiNi0.8Co0.1Mn0.1O2 cell maintains about 85 % capacity retention and Coulombic efficiency >99.8 % in 200 cycles at a charge cut-off voltage of 4.5 V. This study provides a new understanding of lithium salt anions regulating polymer chain segment behavior in the solid-state polymer electrolyte (SPE) and highlights the importance of the ion environment in the construction of interfacial phases and ionic conduction.

Original languageEnglish
Article numbere202317856
JournalAngewandte Chemie - International Edition
Volume63
Issue number19
DOIs
Publication statusPublished - 6 May 2024
Externally publishedYes

Keywords

  • Interface Phase
  • Interfacial Chemistry
  • Solid Polymer Electrolyte
  • Solid-State Lithium Metal Batteries

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