Abstract
Interfaces are the key to next-generation high-energy batteries including solid-state Li metal batteries. In solid-state batteries, the buried nature of solid-solid electrolyte-electrode interfaces makes studying them difficult. Neutrons have significant potential to non-destructively probe these buried solid-solid interfaces. This work presents a comparative study using both neutron depth profiling (NDP) and neutron reflectometry (NR) to study a model lithium metal-lithium phosphorus oxynitride (LiPON) solid electrolyte system. In the NDP data, no distinct interphase is observed at the interface. NR shows a difference between electrodeposited, and vapor deposited LiPON-Li interfaces but finds both are gradient interphases that are less than 30 nm thick. Additional simulations of the LiPON-Li2O-Li system demonstrate that NDP has an excellent resolution in the 50 nm-1 μm regime while NR has an ideal resolution from 0.1-200 nm with different sample requirements. Together NDP and NR can provide a complementary understanding of interfaces between Li metal and solid electrolytes across relevant length scales.
| Original language | English |
|---|---|
| Journal | Journal of Materials Chemistry A |
| DOIs | |
| State | Accepted/In press - 2025 |
Funding
The 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. R. G. and N. P were funded by the Federal Ministry of Education and Research (BMBF) under grant number 03XP0509C. Funding for the NDP portion of the work was also supported by the Ministry of Education, Youth and Sports (MŠMT) of the Czech Republic within the project CZ.02.01.01/00/22_008/0004591. The authors would like to thanks Mathieu Doucet for significant contributions in performing the neutron reflectometry experiments and for performing the additional simulations of artificial interface layers for the NR data presented in Fig. 5. The authors would like to acknowledge, Tien Duong, the US program manager for this funding. The authors would also like to acknowledge Candace Halbert, who helped facilitate the Neutron Reflectometry measurements and Ethan Self and Shomaz Ul Haq for help in editing the manuscript. A portion of this research used resources at Spallation Neutron Source an OE Office of Science User Facility operated by the Oak Ridge National Laboratory. The beam time was allocated to the Liquid Reflectometer (LR) on proposal number IPTS-24417. Neutron Depth Profiling measurements were performed at the Nuclear Physics Institute (NPI) in Řež, Czech Republic within the CANAM (Center of Accelerators and Nuclear Analytical Methods) infrastructure at the LVR15 research reactor. 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 ).
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