Abstract
This study advances the development of flexible, sheet-type sulfide solid-state electrolytes (SSEs) for use in all-solid-state batteries, emphasizing the important and previously insufficiently investigated role of polymer binder entanglement. The molecular weight of polymer binders is pivotal in crafting robust, freestanding SSE films. Our research uncovers a dual impact: higher molecular weight binders bolster the structural integrity of SSE films but elevate grain boundary resistance and diminish critical current density, whereas lower molecular weight poly(isobutylene) films, despite their more uniform distribution, lack the essential strain hardening or strength for sustained active material contact. Crucially, full cells employing higher molecular weight binders demonstrate improved discharge capacity retention, contrasting sharply with the notable capacity degradation in lower molecular weight cells. Our findings not only deepen the comprehension of binder influences in solid-state batteries but also chart a course for refining all-solid-state battery technologies, a key stride for the future of energy storage solutions.
| Original language | English |
|---|---|
| Pages (from-to) | 2677-2684 |
| Number of pages | 8 |
| Journal | ACS Energy Letters |
| Volume | 9 |
| Issue number | 6 |
| DOIs | |
| State | Published - Jun 14 2024 |
Funding
This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program, managed by Simon Thompson and Tien Duong. E.W. acknowledges the support from the Advanced Materials and Manufacturing Technologies Office (AMMTO) of the EERE through its summer internship program. SEM and AFM research was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This work has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. We thank Drs. Ethan Self, Teerth Brahmbhatt, and Frank Delnick for their fruitful discussions. We are also in debted to Dr. Andrew Westover for his support on thin Li anode.