Two-layer cathode architecture for high-energy density and high-power density solid state batteries

Georgios Polizos, Sergiy Kalnaus, Xi Chelsea Chen, Marm Dixit, Mahalingam Balasubramanian, Jaswinder Sharma, Runming Tao, Jianlin Li

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

Solid state batteries with high-energy density and high-power density require the development of thick and energy dense cathodes. Structured cathode electrodes with a double-layer configuration were enabled using a freeze tape casting technique. A bottom dense layer was utilized to enhance the energy density whereas a top porous layer with vertically aligned walls was utilized to enhance the power density. The porous structure of the power layer was achieved by ice templating this layer on top of the densified energy layer of the cathode. This configuration was found to better utilize the active material of the cathodes and was optimized using numerical simulation and computer modeling. Cells with Li metal anode and LiNi0.6Mn0.2Co0.2O2 (NMC622) at approximately 5 and 20 mg/cm2 were cycled at 70 °C at different C-rates. Poly(ethylene oxide) (PEO) with lithium bis-trifluoromethanesulfonimide (LiTFSI) was used for the catholyte and the solid-state electrolyte. The structured cathodes exhibited more than double capacity values as well as better Coulombic efficiency compared to non-structured (single-layer) thick cathodes. Synchrotron X-ray tomography and scanning electron microscopy were used to characterize the microstructure of the cathodes.

Original languageEnglish
Article number101704
JournalMaterials Today Chemistry
Volume33
DOIs
StatePublished - Oct 2023

Funding

This research at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725 , was sponsored by Laboratory Directed Research and Development Program at ORNL. This research used resources of the Advanced Photon Source; a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-21AC02-06CH11357. The authors would like to thank Pavel Shevchenko and Francesco de Carlo for their help with the tomography experiments. Caitlin Duggan is acknowledged for preparation of metallographic cross-sections of the cathode. 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).This research at Oak Ridge National Laboratory (ORNL), managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by Laboratory Directed Research and Development Program at ORNL. This research used resources of the Advanced Photon Source; a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-21AC02-06CH11357. The authors would like to thank Pavel Shevchenko and Francesco de Carlo for their help with the tomography experiments. Caitlin Duggan is acknowledged for preparation of metallographic cross-sections of the cathode. 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

  • Freeze tape cast cathode
  • Solid state batteries
  • Structured cathode

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