Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte
Abstract
Several active areas of research in novel energy storage technologies, including three-dimensional solid state batteries and passivation coatings for reactive battery electrode components, require conformal solid state electrolytes. We describe an atomic layer deposition (ALD) process for a member of the lithium phosphorus oxynitride (LiPON) family, which is employed as a thin film lithium-conducting solid electrolyte. The reaction between lithium tert-butoxide (LiOtBu) and diethyl phosphoramidate (DEPA) produces conformal, ionically conductive thin films with a stoichiometry close to Li2PO2N between 250 and 300°C. The P/N ratio of the films is always 1, indicative of a particular polymorph of LiPON which closely resembles a polyphosphazene. Films grown at 300°C have an ionic conductivity of (6.51 ± 0.36)×10-7 S/cm at 35°C, and are functionally electrochemically stable in the window from 0 to 5.3V vs. Li/Li+. We demonstrate the viability of the ALD-grown electrolyte by integrating it into full solid state batteries, including thin film devices using LiCoO2 as the cathode and Si as the anode operating at up to 1 mA/cm2. The high quality of the ALD growth process allows pinhole-free deposition even on rough crystalline surfaces, and we demonstrate the fabrication and operation of thin film batteries with the thinnest (<40nm) solidmore »
- Authors:
-
- Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering
- Sandia National Lab. (SNL-CA), Livermore, CA (United States)
- Johns Hopkins Univ., Laurel, MD (United States). Applied Physics Lab., Dept. of Research and Exploratory Development
- American Society for Engineering Education, Washington, DC (United States)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-CA), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1360797
- Report Number(s):
- SAND-2017-2069J
Journal ID: ISSN 0897-4756; 651195
- Grant/Contract Number:
- AC04-94AL85000; SC0001160
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 8; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Atomic layer deposition; solid state battery; solid state electrolyte; LiPON; thin film; energy storage; flexible
Citation Formats
Pearse, Alexander J., Schmitt, Thomas E., Fuller, Elliot J., El-Gabaly, Farid, Lin, Chuan-Fu, Gerasopoulos, Konstantinos, Kozen, Alexander C., Talin, A. Alec, Rubloff, Gary, and Gregorczyk, Keith E.. Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b00805.
Pearse, Alexander J., Schmitt, Thomas E., Fuller, Elliot J., El-Gabaly, Farid, Lin, Chuan-Fu, Gerasopoulos, Konstantinos, Kozen, Alexander C., Talin, A. Alec, Rubloff, Gary, & Gregorczyk, Keith E.. Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte. United States. https://doi.org/10.1021/acs.chemmater.7b00805
Pearse, Alexander J., Schmitt, Thomas E., Fuller, Elliot J., El-Gabaly, Farid, Lin, Chuan-Fu, Gerasopoulos, Konstantinos, Kozen, Alexander C., Talin, A. Alec, Rubloff, Gary, and Gregorczyk, Keith E.. Mon .
"Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte". United States. https://doi.org/10.1021/acs.chemmater.7b00805. https://www.osti.gov/servlets/purl/1360797.
@article{osti_1360797,
title = {Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte},
author = {Pearse, Alexander J. and Schmitt, Thomas E. and Fuller, Elliot J. and El-Gabaly, Farid and Lin, Chuan-Fu and Gerasopoulos, Konstantinos and Kozen, Alexander C. and Talin, A. Alec and Rubloff, Gary and Gregorczyk, Keith E.},
abstractNote = {Several active areas of research in novel energy storage technologies, including three-dimensional solid state batteries and passivation coatings for reactive battery electrode components, require conformal solid state electrolytes. We describe an atomic layer deposition (ALD) process for a member of the lithium phosphorus oxynitride (LiPON) family, which is employed as a thin film lithium-conducting solid electrolyte. The reaction between lithium tert-butoxide (LiOtBu) and diethyl phosphoramidate (DEPA) produces conformal, ionically conductive thin films with a stoichiometry close to Li2PO2N between 250 and 300°C. The P/N ratio of the films is always 1, indicative of a particular polymorph of LiPON which closely resembles a polyphosphazene. Films grown at 300°C have an ionic conductivity of (6.51 ± 0.36)×10-7 S/cm at 35°C, and are functionally electrochemically stable in the window from 0 to 5.3V vs. Li/Li+. We demonstrate the viability of the ALD-grown electrolyte by integrating it into full solid state batteries, including thin film devices using LiCoO2 as the cathode and Si as the anode operating at up to 1 mA/cm2. The high quality of the ALD growth process allows pinhole-free deposition even on rough crystalline surfaces, and we demonstrate the fabrication and operation of thin film batteries with the thinnest (<40nm) solid state electrolytes yet reported. Finally, we show an additional application of the moderate-temperature ALD process by demonstrating a flexible solid state battery fabricated on a polymer substrate.},
doi = {10.1021/acs.chemmater.7b00805},
journal = {Chemistry of Materials},
number = 8,
volume = 29,
place = {United States},
year = {Mon Apr 10 00:00:00 EDT 2017},
month = {Mon Apr 10 00:00:00 EDT 2017}
}
Web of Science
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