Abstract
Single-ion conducting polymer electrolytes present a possible route for achieving high energy density next-generation batteries due to their flexible nature and high cation transport number. The trifluoromethanesulfonimide (TFSI) functional group represents one of the most efficient tethered anions for Li-ion conductivity. However, the covalent attachment of TFSI groups into polymer electrolytes has been challenging and costly due to its synthetic difficulty and limited commercial availability of building blocks. Here, we present a new polymer electrolyte synthesized by the Michael addition reaction between poly(allylamine) (PAA) and a vinyl TFSI anion under mild reaction conditions. The resulting PAATFSI exhibits a lower glass transition temperature and several orders of magnitude higher Li-ion conductivity than similar TFSI-based single-ion conducting homopolymers in the dry state. Moreover, PAATFSI exhibits excellent Li-ion conductivity (2.7 × 10-4 S/cm at 30 °C) with the addition of a plasticizer (60 wt % of carbonate solvent), which enables stable lithium-metal battery performance. This study demonstrates a facile route for the synthesis of new single-ion conducting polymer electrolytes that opens a library of possibilities to enable the realization of polymer-based batteries.
| Original language | English |
|---|---|
| Pages (from-to) | 4708-4714 |
| Number of pages | 7 |
| Journal | Macromolecules |
| Volume | 58 |
| Issue number | 9 |
| DOIs | |
| State | Published - May 13 2025 |
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. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy 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 ).