In Situ High-performance Gel Polymer Electrolyte with Dual-reactive Cross-linking for Lithium Metal Batteries

Abstract

Lithium metal batteries have been considered as one of the most promising next-generation power-support devices due to their high specific energy and output voltage. However, the uncontrollable side-reaction and lithium dendrite growth lead to the limited serving life and hinder the practical application of lithium metal batteries. Here, a tri-monomer copolymerized gel polymer electrolyte (TGPE) with a cross-linked reticulation structure was prepared by introducing a cross-linker (polyurethane group) into the acrylate-based in situ polymerization system. The soft segment of polyurethane in TGPE enables the far migration of lithium ions, and the -NH forms hydrogen bonds in the hard segment to build a stable cross-linked framework. This system hinders anion migration and leads to a high Li⁺ migration number ({\mathrm{t}}_{{\mathrm{L}\mathrm{i}}^{+}}= 0.65), which achieves uniform lithium deposition and effectively inhibits lithium dendrite growth. As a result, the assembled symmetric cell shows robust reversibility over 5500 h at a current density of 1 mA cm^-2. The LFP¦¦TGPE¦¦Li cell has a capacity retention of 89.8% after cycling 800 times at a rate of 1C. In summary, in situ polymerization of TGPE electrolytes is expected to be a candidate material for high-energy-density lithium metal batteries.

Keywords

gel polymer electrolytes / hydrogen bonds / in situ polymerization / lithium metal batteries / polyurethane

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2022 The Authors. Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.