Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte

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.

doi:10.1021/acs.chemmater.7b00805

Title: Nanoscale Solid State Batteries Enabled by Thermal Atomic Layer Deposition of a Lithium Polyphosphazene Solid State Electrolyte

Journal Article · Mon Apr 10 00:00:00 EDT 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b00805· OSTI ID:1360797

^[1]; Schmitt, Thomas E. ^[1]; Fuller, Elliot J. ^[2]; El-Gabaly, Farid ^[2]; Lin, Chuan-Fu ^[1]; Gerasopoulos, Konstantinos ^[3]; Kozen, Alexander C. ^[4];

^[2]; Rubloff, Gary ^[1]; Gregorczyk, Keith E. ^[1]

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)

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 (LiO^tBu) 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.

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Research Organization:: Sandia National Lab. (SNL-CA), Livermore, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; SC0001160

OSTI ID:: 1360797

Report Number(s):: SAND-2017-2069J; 651195

Journal Information:: Chemistry of Materials, Vol. 29, Issue 8; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 104 works

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