Abstract
Many technologies including high-energy solid-state batteries rely on high quality solid-solid interfaces. Solid-solid interfaces are particularly difficult to study as their nature requires the interface to be buried. In this work we demonstrate the use of a combination of neutron reflectometry and in situ electrochemistry to measure the interface between Li metal and the solid electrolyte LiPON across an 8 cm2 area. Neutron reflectometry measurements confirm the interphase to be less than 7 nm thick. The neutron reflectometry data further emphasize that the interphase that forms is a chemical gradient consisting of a Li-rich layer that gradually decreases in Li content until it blends into pure LiPON. Experimental confirmation that we can make ideal solid-solid interphases less than 10 nm thick will help facilitate the adoption of high efficiency next generation solid state batteries. Further this combination of complementary techniques provides a more general methodology for studying buried solid-solid interfaces across applications.
| Original language | English |
|---|---|
| Pages (from-to) | 1985-1991 |
| Number of pages | 7 |
| Journal | ACS Energy Letters |
| Volume | 8 |
| Issue number | 4 |
| DOIs | |
| State | Published - Apr 14 2023 |
Funding
This work was funded by the Department of Energy’s Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s US-German Cooperation on Energy Storage: Lithium-Solid-Electrolyte Interfaces program. A portion of this research used resources at the SNS, a Department of Energy (DOE) Office of Science User Facility operated by ORNL. Neutron reflectometry measurements were carried out on the Liquids Reflectometer at the SNS, which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, DOE. The authors would like to acknowledge, Tien Duong, the program manager for this funding, as well as Nancy Dudney, and Wyatt Tenhaeff for insight and early attempts to perform the measurement which provided valuable insights. The authors would also like to acknowledge Candice Halbert, who helped facilitate the neutron reflectometry measurements. This work was funded by the Department of Energy’s Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s US-German Cooperation on Energy Storage: Lithium-Solid-Electrolyte Interfaces program. A portion of this research used resources at the SNS, a Department of Energy (DOE) Office of Science User Facility operated by ORNL. Neutron reflectometry measurements were carried out on the Liquids Reflectometer at the SNS, which is sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, DOE. This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05–00OR22725 with the US Department of Energy (DOE). The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US government purposes. DOE 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 ). Acknowledgments
| Funders | Funder number |
|---|---|
| Candice Halbert | |
| Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office | |
| Scientific User Facilities Division | |
| Wyatt Tenhaeff | |
| U.S. Department of Energy | |
| Office of Science | |
| Basic Energy Sciences | |
| Oak Ridge National Laboratory |
