Nanostructured ligament and fiber Al–doped Li7La3Zr2O12 scaffolds to mediate cathode-electrolyte interface chemistry

Georgios Polizos; Jaswinder Sharma; Charl J. Jafta; Nitin Muralidharan; Gabriel M. Veith; Jong K. Keum; Alexander Kukay; Ritu Sahore; David L. Wood

doi:10.1016/j.jpowsour.2021.230551

Nanostructured ligament and fiber Al–doped Li₇La₃Zr₂O₁₂ scaffolds to mediate cathode-electrolyte interface chemistry

Georgios Polizos, Jaswinder Sharma, Charl J. Jafta, Nitin Muralidharan, Gabriel M. Veith, Jong K. Keum, Alexander Kukay, Ritu Sahore, David L. Wood

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

Scaffold structures of electrospun aluminum–substituted lithium lanthanum zirconate Li₇La₃Zr₂O₁₂ (Al-LLZO) were synthesized and used as an additive in a LiNi_0.6Mn_0.2Co_0.2O₂ composite cathode. The scaffolds were crystalized in the cubic phase after calcination at 700 °C. The Al-LLZO scaffold morphology was dependent on the precursor formulation (aqueous and dimethylformamide. The aqueous precursors resulted in scaffolds of densely coalesced ligaments, whereas the dimethylformamide precursors resulted in high–aspect ratio nanofiber scaffolds. The long-term cycling stability and rate performance of the cells were found to depend on the Al-LLZO scaffold morphology. The uniformly dispersed Al-LLZO fibers resulted in a more stable cathode electrolyte interface formation through the reduced decomposition of the LiPF₆ salt during cycling, resulting in a better high-rate and long-term cycling performance.

Original language	English
Article number	230551
Journal	Journal of Power Sources
Volume	513
DOIs	https://doi.org/10.1016/j.jpowsour.2021.230551
State	Published - Nov 30 2021

Funding

This research at Oak Ridge National Laboratory, managed by UT Battelle LLC, for the US Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy Advanced Manufacturing Office (Program Manager: Brian Valentine). The SEM and XRD characterization were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. XPS measurements were supported by the DOE Office of Basic Energy Sciences, Division of Materials Science and Engineering (G.M.V.). N.M. was supported by Laboratory Directed Research and Development Program at Oak Ridge National Laboratory. This research at Oak Ridge National Laboratory , managed by UT Battelle LLC, for the US Department of Energy ( DOE ) under contract DE-AC05-00OR22725, was sponsored by the Office of Energy Efficiency and Renewable Energy Advanced Manufacturing Office (Program Manager: Brian Valentine). The SEM and XRD characterization were conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. XPS measurements were supported by the DOE Office of Basic Energy Sciences , Division of Materials Science and Engineering (G.M.V.). N.M. was supported by Laboratory Directed Research and Development Program at Oak Ridge National Laboratory . Notice: This manuscript has been authored by UT-Battelle LLC under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

Cathode-electrolyte interface
Composite cathodes
Cubic phase
Electrospinning
LLZO scaffolds

Access to Document

10.1016/j.jpowsour.2021.230551

Cite this

@article{4375636d36734945aee36dcf7e3d5f61,

title = "Nanostructured ligament and fiber Al–doped Li7La3Zr2O12 scaffolds to mediate cathode-electrolyte interface chemistry",

abstract = "Scaffold structures of electrospun aluminum–substituted lithium lanthanum zirconate Li7La3Zr2O12 (Al-LLZO) were synthesized and used as an additive in a LiNi0.6Mn0.2Co0.2O2 composite cathode. The scaffolds were crystalized in the cubic phase after calcination at 700 °C. The Al-LLZO scaffold morphology was dependent on the precursor formulation (aqueous and dimethylformamide. The aqueous precursors resulted in scaffolds of densely coalesced ligaments, whereas the dimethylformamide precursors resulted in high–aspect ratio nanofiber scaffolds. The long-term cycling stability and rate performance of the cells were found to depend on the Al-LLZO scaffold morphology. The uniformly dispersed Al-LLZO fibers resulted in a more stable cathode electrolyte interface formation through the reduced decomposition of the LiPF6 salt during cycling, resulting in a better high-rate and long-term cycling performance.",

keywords = "Cathode-electrolyte interface, Composite cathodes, Cubic phase, Electrospinning, LLZO scaffolds",

author = "Georgios Polizos and Jaswinder Sharma and Jafta, {Charl J.} and Nitin Muralidharan and Veith, {Gabriel M.} and Keum, {Jong K.} and Alexander Kukay and Ritu Sahore and Wood, {David L.}",

note = "Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

year = "2021",

month = nov,

day = "30",

doi = "10.1016/j.jpowsour.2021.230551",

language = "English",

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journal = "Journal of Power Sources",

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T1 - Nanostructured ligament and fiber Al–doped Li7La3Zr2O12 scaffolds to mediate cathode-electrolyte interface chemistry

AU - Polizos, Georgios

AU - Sharma, Jaswinder

AU - Jafta, Charl J.

AU - Muralidharan, Nitin

AU - Veith, Gabriel M.

AU - Keum, Jong K.

AU - Kukay, Alexander

AU - Sahore, Ritu

AU - Wood, David L.

PY - 2021/11/30

Y1 - 2021/11/30

N2 - Scaffold structures of electrospun aluminum–substituted lithium lanthanum zirconate Li7La3Zr2O12 (Al-LLZO) were synthesized and used as an additive in a LiNi0.6Mn0.2Co0.2O2 composite cathode. The scaffolds were crystalized in the cubic phase after calcination at 700 °C. The Al-LLZO scaffold morphology was dependent on the precursor formulation (aqueous and dimethylformamide. The aqueous precursors resulted in scaffolds of densely coalesced ligaments, whereas the dimethylformamide precursors resulted in high–aspect ratio nanofiber scaffolds. The long-term cycling stability and rate performance of the cells were found to depend on the Al-LLZO scaffold morphology. The uniformly dispersed Al-LLZO fibers resulted in a more stable cathode electrolyte interface formation through the reduced decomposition of the LiPF6 salt during cycling, resulting in a better high-rate and long-term cycling performance.

AB - Scaffold structures of electrospun aluminum–substituted lithium lanthanum zirconate Li7La3Zr2O12 (Al-LLZO) were synthesized and used as an additive in a LiNi0.6Mn0.2Co0.2O2 composite cathode. The scaffolds were crystalized in the cubic phase after calcination at 700 °C. The Al-LLZO scaffold morphology was dependent on the precursor formulation (aqueous and dimethylformamide. The aqueous precursors resulted in scaffolds of densely coalesced ligaments, whereas the dimethylformamide precursors resulted in high–aspect ratio nanofiber scaffolds. The long-term cycling stability and rate performance of the cells were found to depend on the Al-LLZO scaffold morphology. The uniformly dispersed Al-LLZO fibers resulted in a more stable cathode electrolyte interface formation through the reduced decomposition of the LiPF6 salt during cycling, resulting in a better high-rate and long-term cycling performance.

KW - Cathode-electrolyte interface

KW - Composite cathodes

KW - Cubic phase

KW - Electrospinning

KW - LLZO scaffolds

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