Highly stable interface formation in onsite coagulation dual-salt gel electrolyte for lithium-metal batteries

Yu Hsing Lin, Ramesh Subramani, Yu Ting Huang, Yuh Lang Lee, Jeng Shiung Jan, Chi Cheng Chiu, Sheng Shu Hou, Hsisheng Teng

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12 Citations (Scopus)


The formation of Li dendrites in Li-metal batteries (LMBs) may lead to a short circuit, causing a fire or an explosion, and consume Li through dead-Li formation and solid-electrolyte interphase (SEI) thickening. Instead of using an artificial SEI, we use a gel polymer electrolyte (GPE) comprising poly(vinylidene fluoride-co-hexafluoro propylene) (PVDF-co-HFP) and poly(2-hydroxyethyl methacrylate) (PHEMA), dual lithium salts, and carbonate solvents to stabilize the SEI and suppress dendrite formation. When incorporated with a separator, the GPE exhibits higher ionic conductivity than liquid electrolytes and has a high Li+-transference number of 0.64. Without adding LiNO3, this GPE allows uniform Li plating/stripping on both Cu- and Li-metal anodes at high currents owing to robust SEI formation and negligible dendrite growth. Full-cell LMBs containing this GPE can deliver high capacities at high discharge rates and present high cycling stability. The high-polarity PVDF-co-HFP facilitates counter-ion dissociation to increase conductivity and tethers an anion to reduce the space-charge region and thus hinder Li-dendrite growth. Moreover, PHEMA closely contacts the metal anodes, which helps suppress solvent reduction and SEI thickening. This GPE is synthesized as a liquid, which coagulates onsite during LMB assembly. This study presents a strategy to advance metal anode technology for realizing LMBs.

Original languageEnglish
Pages (from-to)5675-5684
Number of pages10
JournalJournal of Materials Chemistry A
Issue number9
Publication statusPublished - 2021 Mar 7

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • Renewable Energy, Sustainability and the Environment
  • General Materials Science


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