Abstract
Silicon (Si) is the most naturally abundant element possessing 10-fold greater theoretical capacity compared to that of graphite-based anodes. The practicality of implementing Si anodes is, however, limited by the unstable solid/electrolyte interphase (SEI) and anode fracturing during continuous lithiation/delithiation. We demonstrate that glyme-based electrolytes (GlyEls) ensure a conformal SEI on Si and keep the Si "fracture-free". Benchmarking against the optimal, commonly used carbonate electrolyte with the fluoroethylene carbonate additive, the Si anode cycled in a GlyEl exhibits a reduced early parasitic current (by 62.5%) and interfacial resistance (by 72.8%), while cell capacity retention is promoted by >7% over the course of 110 cycles. A mechanistic investigation by X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy indicates GlyEl enriches Si SEI with elastic polyether but diminishes its carbonate species. Glyme-based electrolytes proved to be viable in stabilizing the SEI on Si for future high energy density lithium-ion batteries.
| Original language | English |
|---|---|
| Pages (from-to) | 1684-1693 |
| Number of pages | 10 |
| Journal | ACS Energy Letters |
| Volume | 6 |
| Issue number | 5 |
| DOIs | |
| State | Published - May 14 2021 |
Funding
This work is supported by the U.S. Department of Energy (DOE) Vehicle Technologies Office under the Silicon Electrolyte Interface Stabilization (SEISta) Consortium directed by Brian Cunningham and managed by Anthony Burrell. The manuscript has been authored by UT-Battelle LLC under Contract DE-AC05-00OR22725 with DOE. The electrodes in this article were fabricated at Argonne’s Cell Analysis, Modeling and Prototyping (CAMP) Facility. The authors thank Drs. Sheng Dai, Andrew Jansen, Bryant Polzin, and Fulya Dogan Key for experiment support. The U.S. government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of the manuscript, or allow other to do so, for U.S. 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 ).
