Journal
CHEMISTRY OF MATERIALS
Volume 29, Issue 8, Pages 3740-3753Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.7b00805
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Funding
- Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center (EFRC) - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DESC0001160]
- Independent Research and Development - Research & Exploratory Development Department (REDD) of the Johns Hopkins University Applied Physics Laboratory (JHU/APL)
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
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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 atypical 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 ((LiOBu)-Bu-t) and diethyl phosphoramidate (DEPA) produces conformal, ionically conductive thin films with a stoichiometry close to Li2PO2N between 250 and 300 degrees C. Unusually, the P/N ratio of the films is always 1, indicative of a particular polymorph of LiPON that closely resembles a polyphosphazene. Films grown at 300 degrees C have an ionic conductivity of (6.51 +/- 0.36) x 10(-7) S/cm at 35 degrees C and are functionally electrochemically stable in the window from 0 to 5.3 V versus 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/cm(2). The high quality of the ALD growth process allows pinhole-free deposition even on rough crystalline surfaces, and we demonstrate the successful fabrication and operation of thin film batteries with ultrathin (<100 nm) solid state electrolytes. 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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