期刊
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
卷 168, 期 11, 页码 -出版社
ELECTROCHEMICAL SOC INC
DOI: 10.1149/1945-7111/ac30ad
关键词
nitrogen doping; lithium lanthanum titanate; solid-state electrolyte; lithium battery; composite electrolyte; nanofiber
资金
- Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) [DE-EE0007806]
- National Energy Research Scientific Computing Center at DOE Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]
- National Science Foundation [ACI-1548562, CTS190069]
The study focused on improving the ionic conductivity of LLTO by nitrogen doping and successfully preparing a solid-state composite electrolyte. The electrochemical performance tests demonstrated that the nitrogen-doped composite electrolyte exhibited good ionic conductivity and cycling stability at room temperature.
Currently cation doping is common for improving ionic conductivity of metal oxide-based lithium-ion conductors. In this work, anions (nitrogen ions) have been doped to perovskite Li3xLa2/3 - xTiO3 (LLTO) nanofibers by heat treatment in the ammonia-containing atmosphere, and substituted for oxygen anions partially in the perovskite structure. Density-functional theory (DFT) calculation results reveal that nitrogen doping weakens the bonding of Li ions on the A sites in perovskite ABO(3) structure and allows for larger lattice distortion, reducing the activation energy for Li-ion hopping in both the forward and backward jumping directions. Experimental results have also confirmed that nitrogen doping has improved ionic conductivity of LLTO. Nitrogen-doped LLTO nanofibers have been incorporated with a poly (vinylidene fluoride)-co-hexafluoropropylene (PVDF-HFP) polymer to form a solid-state composite electrolyte, which exhibits ionic conductivity of 3.8 x 10(-4) S center dot cm(-1) at room temperature and an electrochemical stability window of up to 4.9 V vs Li divide Li+. The all-solid-state Li metal divide composite electrolyte divide LiFePO4 lithium batteries, which employ nitrogen-doped LLTO nanofibers, show better rate capability and cycling stability at room temperature than the counterparts with pristine LLTO nanofibers.
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