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Regulating the solvation structure of lithium ion for smooth Li metal deposition in quasi‐solid‐state batteries

Von Wiley-VCH zur Verfügung gestellt

In-situ polymerized gel electrolytes (GPE) are the promising next generation of electrolytes for high-energy batteries, integrating the multiple advantages of liquid and all solid state electrolytes. Herein, we synthesized GPE with Poly(ethylene glycol) acrylate (PEGDA) in order to understand how GPE efficiently inhibits lithium dendrite formation and growth. The effects of PEGDA on the lithium ion solvated structure are investigated using density functional theory (DFT) and ab-initio molecular dynamics (AIMD), which are also supported by the Raman result. The GPE electrolytes with the optimal PEGDA concentration exhibit the high transference numbers (tLi+ = 0.72) and ionic conductivity (σ = 3.24 mS cm −1). The lithium symmetric battery using GPE achieves a stable cycle with 1200h in comparison to 320h in liquid electrolytes (LE), possibly owing to the high content of LiF (17.9%) in the Solid Electrolyte Interphase (SEI) film of the GPE cell. The observed facile concentration/electric field gradient also accounts for high super cyclic performance through the finite element method (FEM). Besides, a LiCoO2|GPE|Li cell demonstrates superior capacity retention of 87.09% for 200 cycles, promising guidelines for the design of high specific energy lithium batteries.

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