The formation of lithium dendrites and the safety hazards arising from flammable liquid electrolytes have seri-ously 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 elec-trolyte as counter solvent and additives. The well-designed amide-based electrolyte possesses nonflammability, high ionic conductiv-ity, 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.

Wanbao Wu;Yiyang Bo;Deping Li;Yihong Liang;Jichuan Zhang;Miaomiao Cao;Ruitian Guo;Zhenye Zhu;Lijie Ci;Mingyu Li;Jiaheng Zhang

Sauvage Laboratory for Smart Materials,Harbin Institute of Technology(Shenzhen),Shenzhen 518055,People's Republic of China;Research Centre of Printed Flexible Electronics,School of Materials Science and Engineering,Harbin Institute of Technology(Shenzhen),Shenzhen 518055,People's Republic of China;School of Materials Science and Engineering,Harbin Institute of Technology(Shenzhen),Shenzhen 518055,People's Republic of China;Department of Chemistry,University of Idaho,Moscow,ID 83844?2343,USA

纳微快报（英文）

[1]Wanbao Wu;Yiyang Bo;Deping Li;Yihong Liang;Jichuan Zhang;Miaomiao Cao;Ruitian Guo;Zhenye Zhu;Lijie Ci;Mingyu Li;Jiaheng Zhang-.Safe and Stable Lithium Metal Batteries Enabled by an Amide?Based Electrolyte)[J].纳微快报（英文）,2022(03):120-133

butyrolactam,Tetrafluoroethyl,tetrafluoropropylether

Safe,Stable,Lithium,Metal,Batteries,Enabled,by,Amide,Based,Electrolyte,formation,lithium,dendrites,safety,hazards,arising,from,flammable,liquid,electrolytes,have,seri,ously,hindered,development,high,energy,density,metal,batteries,Herein,emerging,amide,proposed,containing,LiTFSI,different,molar,ratios,fluoroethylene,carbonate,are,introduced,into,counter,solvent,additives,well,designed,possesses,nonflammability,ionic,conductiv,thermal,stability,electrochemical,Besides,inorganic,rich,solid,interphase,abundance,Li3N,situ,formed,leading,spherical,deposition,mechanism,solvation,chemistry,further,inves,tigated,molecular,dynamics,simulations,functional,theory,When,applied,LiFePO4,LiMn2O4,cathode,can,enable,stable,cycling,performance,room,temperature,This,study,provides,new,insight

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