MOFs-induced robust interphase enriched in Li2O boosting Li plating/stripping coulombic efficiency of lithium metal anode in commercial carbonate electrolyte

Ke Wang, Ji Qian*, Yi Chen, Tianyang Yu, Man Zhang, Xinhui Pan, Renjie Chen

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Lithium metal anodes face challenges of dendritic growth and unstable solid electrolyte interface (SEI) in carbonate electrolytes, leading to low Coulombic efficiency (CE<80%) and rapid capacity decay. Herein, we present a facile separator modification strategy utilizing functional Metal-organic framework (MOF) to catalyze the Li₂O-dominated SEI formation. The amine-functionalized MOF nanoparticles preferentially induce inorganic-rich SEI formation, yielding a mechanically robust interface with Li₂O crystallization and Young's modulus of 3.69 GPa, superior to that of conventional PP. Additionally, the porous structure of MOF nanoparticles endows the resulting separators with excellent electrolyte wettability and homogenizes ion transport. The functional separator with these synergistic effects reduces the decomposition of the electrolyte and facilitate the dense and uniform deposition of Li metal. As a result, exceptional Li plating/stripping stability is achieved in commercial carbonate electrolytes, delivering an average CE of 99.12% over 250 cycles at 1 mA cm−2/1 mAh cm−2 in Li/Cu cells. By implementing this functional separator, the Li/LiFePO4 full cells deliver a superior cycling lifespan that renders a high specific capacity of 130 mAh g−1 over 500 cycles at 1C with 90.9% capacity retention. This electrolyte-separator interfacial engineering strategy addresses critical challenges of Li metal anodes in carbonate electrolyte while demonstrating scalable potential for practical high-energy batteries.

Original languageEnglish
Article number164928
JournalChemical Engineering Journal
Volume519
DOIs
Publication statusPublished - 1 Sept 2025

Keywords

  • Carbonate electrolyte
  • Coulombic efficiency
  • Lithium metal anode
  • Li₂O-rich solid electrolyte interphase
  • MOFs

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