Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li 2 S‐P 2 S 5 (LPS) Solid Electrolyte for Solid‐State Li Metal Batteries
Abstract
Abstract A combination of high ionic conductivity and facile processing suggest that sulfide‐based materials are promising solid electrolytes that have the potential to enable Li metal batteries. Although the Li 2 S‐P 2 S 5 (LPS) family of compounds exhibit desirable characteristics, it is known that Li metal preferentially propagates through microstructural defects, such as particle boundaries and/or pores. Herein, it is demonstrated that a near theoretical density (98% relative density) LPS 75‐25 glassy electrolyte exhibiting high ionic conductivity can be achieved by optimizing the molding pressure and temperature. The optimal molding pressure reduces porosity and particle boundaries while preserving the preferred amorphous structure. Moreover, molecular rearrangements and favorable Li coordination environments for conduction are attained. Consequently, the Young's Modulus approximately doubles (30 GPa) and the ionic conductivity increases by a factor of five (1.1 mS cm −1 ) compared to conventional room temperature molding conditions. It is believed that this study can provide mechanistic insight into processing‐structure‐property relationships that can be used as a guide to tune microstructural defects/properties that have been identified to have an effect on the maximum charging current that a solid electrolyte can withstand during cycling without short‐circuiting.
- Authors:
-
[1];
[4];
[5]
- Department of Materials Science and Engineering University of Michigan Ann Arbor MI 48109 USA
- Department of Mechanical Engineering University of Michigan Ann Arbor MI 48109 USA
- Spallation Neutron Source Oak Ridge National Laboratory Oak Ridge TN 37831 USA
- Department of Materials Science and Engineering University of Michigan Ann Arbor MI 48109 USA, Department of Mechanical Engineering University of Michigan Ann Arbor MI 48109 USA
- Department of Materials Science and Engineering University of Michigan Ann Arbor MI 48109 USA, Department of Mechanical Engineering University of Michigan Ann Arbor MI 48109 USA, University of Michigan Ann Arbor MI 48109 USA
- Publication Date:
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1607941
- Resource Type:
- Publisher's Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Name: Advanced Energy Materials Journal Volume: 10 Journal Issue: 19; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley Blackwell (John Wiley & Sons)
- Country of Publication:
- Germany
- Language:
- English
Citation Formats
Garcia‐Mendez, Regina, Smith, Jeffrey G., Neuefeind, Joerg C., Siegel, Donald J., and Sakamoto, Jeff. Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li 2 S‐P 2 S 5 (LPS) Solid Electrolyte for Solid‐State Li Metal Batteries. Germany: N. p., 2020.
Web. doi:10.1002/aenm.202000335.
Garcia‐Mendez, Regina, Smith, Jeffrey G., Neuefeind, Joerg C., Siegel, Donald J., & Sakamoto, Jeff. Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li 2 S‐P 2 S 5 (LPS) Solid Electrolyte for Solid‐State Li Metal Batteries. Germany. https://doi.org/10.1002/aenm.202000335
Garcia‐Mendez, Regina, Smith, Jeffrey G., Neuefeind, Joerg C., Siegel, Donald J., and Sakamoto, Jeff. Wed .
"Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li 2 S‐P 2 S 5 (LPS) Solid Electrolyte for Solid‐State Li Metal Batteries". Germany. https://doi.org/10.1002/aenm.202000335.
@article{osti_1607941,
title = {Correlating Macro and Atomic Structure with Elastic Properties and Ionic Transport of Glassy Li 2 S‐P 2 S 5 (LPS) Solid Electrolyte for Solid‐State Li Metal Batteries},
author = {Garcia‐Mendez, Regina and Smith, Jeffrey G. and Neuefeind, Joerg C. and Siegel, Donald J. and Sakamoto, Jeff},
abstractNote = {Abstract A combination of high ionic conductivity and facile processing suggest that sulfide‐based materials are promising solid electrolytes that have the potential to enable Li metal batteries. Although the Li 2 S‐P 2 S 5 (LPS) family of compounds exhibit desirable characteristics, it is known that Li metal preferentially propagates through microstructural defects, such as particle boundaries and/or pores. Herein, it is demonstrated that a near theoretical density (98% relative density) LPS 75‐25 glassy electrolyte exhibiting high ionic conductivity can be achieved by optimizing the molding pressure and temperature. The optimal molding pressure reduces porosity and particle boundaries while preserving the preferred amorphous structure. Moreover, molecular rearrangements and favorable Li coordination environments for conduction are attained. Consequently, the Young's Modulus approximately doubles (30 GPa) and the ionic conductivity increases by a factor of five (1.1 mS cm −1 ) compared to conventional room temperature molding conditions. It is believed that this study can provide mechanistic insight into processing‐structure‐property relationships that can be used as a guide to tune microstructural defects/properties that have been identified to have an effect on the maximum charging current that a solid electrolyte can withstand during cycling without short‐circuiting.},
doi = {10.1002/aenm.202000335},
journal = {Advanced Energy Materials},
number = 19,
volume = 10,
place = {Germany},
year = {Wed Apr 01 00:00:00 EDT 2020},
month = {Wed Apr 01 00:00:00 EDT 2020}
}
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