Nitrogen-Doped Lithium Lanthanum Titanate Nanofiber-Polymer Composite Electrolytes for All-Solid-State Lithium Batteries

Yang, Hui; Tay, Kieran; Xu, Yaobin; Rajbanshi, Biplab; Kasani, Sujan; Bright, Joeseph; Boryczka, Jennifer; Wang, Chongmin; Bai, Peng; Wu, Nianqiang

doi:10.1149/1945-7111/ac30ad

Title: Nitrogen-Doped Lithium Lanthanum Titanate Nanofiber-Polymer Composite Electrolytes for All-Solid-State Lithium Batteries

Journal Article · Mon Nov 08 00:00:00 EST 2021 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ac30ad· OSTI ID:1829510

Yang, Hui;

; Xu, Yaobin; Rajbanshi, Biplab; Kasani, Sujan; Bright, Joeseph; Boryczka, Jennifer; Wang, Chongmin; Bai, Peng;

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 Li_3xLa_{2/3 – x}TiO₃ (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 ABO₃ 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 × 10^–4 S·cm^–1 at room temperature and an electrochemical stability window of up to 4.9 V vs Li|Li⁺. The all-solid-state Li metal|composite electrolyte|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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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-76RL01830; AC02-05CH11231

OSTI ID:: 1829510

Alternate ID(s):: OSTI ID: 1826383; OSTI ID: 1833357

Report Number(s):: PNNL-SA-162349

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Vol. 168 Journal Issue: 11; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
nitrogen doping
lithium lanthanum titanate
solid-state electrolyte
lithium battery
composite electrolyte
nanofiber

Title: Nitrogen-Doped Lithium Lanthanum Titanate Nanofiber-Polymer Composite Electrolytes for All-Solid-State Lithium Batteries

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