Abstract
Lithium thiophosphates represent a promising class of solid Li+ conductors for all-solid-state batteries. Scalable solvent-mediated synthesis routes for several Li-P-S ternary compounds have been reported, but little is known regarding the reaction mechanism of such pathways. This work demonstrates that solvent-mediated synthesis of lithium thiophosphate solid electrolytes from mixtures of Li2S and P2S5 proceeds through a highly soluble P2S62-intermediate. This intermediate exhibits virtually the same Raman spectra in several solvents including acetonitrile, methyl acetate, ethyl acetate, ethyl propionate, dimethoxyethane, tetraethylene glycol dimethyl ether, and tetrahydrofuran. Based on this universal intermediate, a general reaction mechanism is proposed for the solvent-mediated synthesis of several lithium thiophosphates including (LiPS3)n, Li2P2S6, Li7P3S11, and Li3PS4.
| Original language | English |
|---|---|
| Pages (from-to) | 27396-27402 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry C |
| Volume | 124 |
| Issue number | 50 |
| DOIs | |
| State | Published - Dec 17 2020 |
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 supported by Asst. Secretary, Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide 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 ).