摘要
The formation of lithium dendrites and the safety hazards arising from flammable liquid electrolytes have seriously hindered the development of high-energy-density lithium metal batteries.Herein,an emerging amide-based electrolyte is proposed,containing LiTFSI and butyrolactam in different molar ratios.1,1,2,2-Tetrafluoroethyl-2,2,3,3-tetrafluoropropylether and fluoroethylene carbonate are introduced into the amide-based electrolyte as counter solvent and additives.The well-designed amide-based electrolyte possesses nonflammability,high ionic conductivity,high thermal stability and electrochemical stability(>4.7 V).Besides,an inorganic/organic-rich solid electrolyte interphase with an abundance of LiF,Li3N and Li-N-C is in situ formed,leading to spherical lithium deposition.The formation mechanism and solvation chemistry of amide-based electrolyte are further inves-tigated by molecular dynamics simulations and density functional theory.When applied in Li metal batteries with LiFePO4 and LiMn2O4 cathode,the amide-based electrolyte can enable stable cycling performance at room temperature and 60℃.This study provides a new insight into the development of amide-based electrolytes for lithium metal batteries.
基金
supported by the National Natural Science Foundation of China(21905069,52002094)
the Shenzhen Science and Technology Innovation Committee(JCYJ20180507183907224,KQTD20170809110344233)
the Economic,Trade and Information Commission of Shenzhen Municipality through the Graphene Manufacture Innovation Center(201901161514)
the Guangdong Province Covid-19 Pandemic Control Research Fund(2020KZDZX1220)
the School Research Startup Expenses of Harbin Institute of Technology(Shenzhen)(DD29100027).