Abstract
This study investigates the impact of the ceramic particle size on the bulk and interfacial ion transport properties of composite polymer electrolytes. The ceramic particles used for this study are micrometer-sized commercial lithium lanthanum titanate (LLTO) powders and LLTO nanorods (NR) prepared in the laboratory. The polymer matrices are vinylene carbonate (VEC) based single-ion-conducting (SIC) and dual-ion-conducting (DIC) polymer electrolytes. Our results reveal that the addition of LLTO NR results in improved ion transport, while the addition of commercial LLTO is ineffective or even detrimental. We ascribe these results to the formation of an interfacial polymer layer around the LLTO particles with enhanced Li+ mobility and estimate the thickness of the interfacial layer to be ∼5 nm. The high surface-to-volume ratio of the LLTO NR leads to the percolation of the interfacial region at a relatively low ceramic loading of 30 wt %. This study highlights the importance of achieving percolation of the interface region (as opposed to the particles themselves) within the composite electrolyte when the interfacial layer is the enhancement mechanism.
| Original language | English |
|---|---|
| Pages (from-to) | 7489-7498 |
| Number of pages | 10 |
| Journal | Macromolecules |
| Volume | 57 |
| Issue number | 15 |
| DOIs | |
| State | Published - Aug 13 2024 |
Funding
This work was supported as part of the Fast and Cooperative Ion Transport in Polymer-Based Materials (FaCT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences at Oak Ridge National Laboratory. The research reported here made use of the shared facilities of the Materials Research Science and Engineering Center (MRSEC) at UC Santa Barbara: NSF DMR-2308708. The UC Santa Barbara MRSEC is a member of the Materials Research Facilities Network( www.mrfn.com ). A.B. acknowledges Dr. Oscar Nordness for assisting in NMR experiments and fruitful scientific discussions. The TEM and part of the BDS experiments were conducted at the Center for Nanophase Materials Sciences, a US Department of Energy Office of Science User Facility operated at Oak Ridge National Laboratory.