A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte

Max J. Palmer; Sergiy Kalnaus; Marm B. Dixit; Andrew S. Westover; Kelsey B. Hatzell; Nancy J. Dudney; X. Chelsea Chen

doi:10.1016/j.ensm.2019.12.031

A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte

Max J. Palmer, Sergiy Kalnaus, Marm B. Dixit, Andrew S. Westover, Kelsey B. Hatzell, Nancy J. Dudney, X. Chelsea Chen

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

76 Scopus citations

Abstract

In this work we introduce an approach to fabricate a solid composite electrolyte film that is thin, ionically conductive, and mechanically robust with good potential for manufacturability, in the application of lithium metal batteries. First a doped-lithium aluminum titanium phosphate ceramic thin film with thickness of ~25 μm is formed by aqueous spray coating, a scalable process. The film is partially sintered to form a three-dimensionally interconnected structure with a dense backbone. It is then backfilled with a crosslinkable poly(ethylene oxide) (PEO)-based polymer electrolyte. The composite has very high ceramic loading of 77 wt% (61 vol%) and an ionic conductivity of 3.5 × 10^-5 S/cm at 20 °C with an activation energy of 0.43 eV. The main ion transport pathway is through the ceramic network, predicted by modelling and verified by experiments. Owing to the interconnected structure of the ceramic, the composite electrolyte exhibits much improved mechanical strength.

Original language	English
Pages (from-to)	242-249
Number of pages	8
Journal	Energy Storage Materials
Volume	26
DOIs	https://doi.org/10.1016/j.ensm.2019.12.031
State	Published - Apr 2020

Funding

This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy 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 was sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office's Advanced Battery Materials Research Program (Tien Duong, Program Manager). The Oak Ridge National Laboratory's Directed Research and Development Program (LDRD) provided partial support. Oak Ridge National Laboratory is managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE), under contract DE-AC05-00OR22725. KBH and MD were supported by the National Science Foundation under grant No. 1847029 and the ECS Toyota Fellowship. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. We thank our ORNL colleagues Dr. Tomonori Saito and Michelle Lehmann for their help with the polymer electrolytes and Dr. Christopher Nelson for help with the preparation of X-ray tomography samples. This research was sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s Advanced Battery Materials Research Program (Tien Duong, Program Manager). The Oak Ridge National Laboratory’s Directed Research and Development Program (LDRD) provided partial support. Oak Ridge National Laboratory is managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) , under contract DE-AC05-00OR22725 . KBH and MD were supported by the National Science Foundation under grant No. 1847029 and the ECS Toyota Fellowship. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357 . We thank our ORNL colleagues Dr. Tomonori Saito and Michelle Lehmann for their help with the polymer electrolytes and Dr. Christopher Nelson for help with the preparation of X-ray tomography samples. Appendix A

Funders	Funder number
Advanced Photon Source
DOE Office of Science
DOE Public Access Plan
Oak Ridge National Laboratory
Oak Ridge National Laboratory
Office of Science User Facility operated
United States Government
National Science Foundation
U.S. Department of Energy
Directorate for Engineering	1847029
Battelle	DE-AC05-00OR22725
Office of Science
Office of Energy Efficiency and Renewable Energy
Argonne National Laboratory	DE-AC02-06CH11357
Laboratory Directed Research and Development
Electrochemical Society

Keywords

Composite electrolyte
Ionic conductivity
Lithium battery
Solid state electrolyte
Spray coating

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.ensm.2019.12.031

Cite this

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title = "A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte",

abstract = "In this work we introduce an approach to fabricate a solid composite electrolyte film that is thin, ionically conductive, and mechanically robust with good potential for manufacturability, in the application of lithium metal batteries. First a doped-lithium aluminum titanium phosphate ceramic thin film with thickness of ~25 μm is formed by aqueous spray coating, a scalable process. The film is partially sintered to form a three-dimensionally interconnected structure with a dense backbone. It is then backfilled with a crosslinkable poly(ethylene oxide) (PEO)-based polymer electrolyte. The composite has very high ceramic loading of 77 wt% (61 vol%) and an ionic conductivity of 3.5 × 10-5 S/cm at 20 °C with an activation energy of 0.43 eV. The main ion transport pathway is through the ceramic network, predicted by modelling and verified by experiments. Owing to the interconnected structure of the ceramic, the composite electrolyte exhibits much improved mechanical strength.",

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AU - Palmer, Max J.

AU - Kalnaus, Sergiy

AU - Dixit, Marm B.

AU - Westover, Andrew S.

AU - Hatzell, Kelsey B.

AU - Dudney, Nancy J.

AU - Chen, X. Chelsea

PY - 2020/4

Y1 - 2020/4

N2 - In this work we introduce an approach to fabricate a solid composite electrolyte film that is thin, ionically conductive, and mechanically robust with good potential for manufacturability, in the application of lithium metal batteries. First a doped-lithium aluminum titanium phosphate ceramic thin film with thickness of ~25 μm is formed by aqueous spray coating, a scalable process. The film is partially sintered to form a three-dimensionally interconnected structure with a dense backbone. It is then backfilled with a crosslinkable poly(ethylene oxide) (PEO)-based polymer electrolyte. The composite has very high ceramic loading of 77 wt% (61 vol%) and an ionic conductivity of 3.5 × 10-5 S/cm at 20 °C with an activation energy of 0.43 eV. The main ion transport pathway is through the ceramic network, predicted by modelling and verified by experiments. Owing to the interconnected structure of the ceramic, the composite electrolyte exhibits much improved mechanical strength.

AB - In this work we introduce an approach to fabricate a solid composite electrolyte film that is thin, ionically conductive, and mechanically robust with good potential for manufacturability, in the application of lithium metal batteries. First a doped-lithium aluminum titanium phosphate ceramic thin film with thickness of ~25 μm is formed by aqueous spray coating, a scalable process. The film is partially sintered to form a three-dimensionally interconnected structure with a dense backbone. It is then backfilled with a crosslinkable poly(ethylene oxide) (PEO)-based polymer electrolyte. The composite has very high ceramic loading of 77 wt% (61 vol%) and an ionic conductivity of 3.5 × 10-5 S/cm at 20 °C with an activation energy of 0.43 eV. The main ion transport pathway is through the ceramic network, predicted by modelling and verified by experiments. Owing to the interconnected structure of the ceramic, the composite electrolyte exhibits much improved mechanical strength.

KW - Composite electrolyte

KW - Ionic conductivity

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JF - Energy Storage Materials

ER -

A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte

Abstract

Funding

Keywords

UN SDGs

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