Abstract
In a three-dimensional interconnected polymer/ceramic composite electrolyte (3D composite), both the polymer and ceramic electrolyte phases are individually connected with a polymer-rich surface layer to provide conformal contact with the electrodes. This work investigates how the transference number of the polymer phase affects the electrochemical properties of the 3D composite. Here, we fabricate a 3D composite using a “single-ion” conducting polymer electrolyte (PE), Li1+x+yAlxTi2-xSiyP3-yO12 (LICGC) ceramic, and compare its electrochemical properties with the neat polymer, and with a 3D composite made with a dual-ion-conducting PE (we reported previously). Our results reveal that changing the polymer phase from a dual-ion-conducting PE to a single-ion-conducting PE results in a 9-fold increase in the limiting current density, although the interfacial impedance between the polymer and LICGC ceramic remains high (and contributes significantly to the total impedance of the 3D composite). The limiting current density of the 3D composite is dictated by the PE and minimally affected by the ceramic scaffold. The ceramic scaffold, however, helps to ease the concentration gradient buildup within the PE and moderately improves the overall transference number. The LICGC scaffold does not provide any additional Li dendrite resistance due to its high reactivity with Li.
Original language | English |
---|---|
Journal | ACS Applied Energy Materials |
DOIs | |
State | Accepted/In press - 2024 |
Funding
This research at Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy under Contract DE-AC05-00OR22725, was primarily sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Offices Advanced Battery Materials Research Program (Tien Duong and Simon Thompson, Program Managers). We also acknowledge Ercan Cakmak for his help with X-ray computed tomography (XCT) measurements.
Keywords
- ceramic electrolyte
- composite electrolyte
- polymer/ceramic interface
- single-ion conducting polymer
- solid-state battery