Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping
Abstract
Quasi-binary thiophosphate-based solid electrolytes (SEs) are attracting substantial interest for lithium batteries due to their outstanding room temperature ionic conductivities. This work describes reactions occurring at the solid electrolyte (SE)/Au interface during Li deposition and stripping for two exemplary SE materials: β-Li3PS4 (β-LPS) and Li10GeP2S12 (LGPS). We used in situ Raman spectroscopy, along with X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) to evaluate potential-dependent changes in the chemistry of these materials at active electrode interfaces. For β-LPS, a partially reversible conversion of PS43– to P2S64– was found along with the formation of Li2S during Li deposition and stripping. In contrast, LGPS exhibited only irreversible changes at potentials below 0.7 V vs Li+/Li. The different behaviors likely relate to differences in the structures of the two SE materials and the availability of easily bridged anion components in close proximity. In conclusion, the work shows that SE integrity at interfaces can be altered by applied potential and illustrates important speciations for the interfacial structures that mediate their electrochemical activities.
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1388302
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 29; Journal Issue: 7; Related Information: CEES partners with Argonne National Laboratory (lead); University of Illinois, Urbana-Champaign; Northwest University; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; energy storage (including batteries and capacitors); charge transport; materials and chemistry by design; synthesis (novel materials)
Citation Formats
Sang, Lingzi, Haasch, Richard T., Gewirth, Andrew A., and Nuzzo, Ralph G. Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping. United States: N. p., 2017.
Web. doi:10.1021/acs.chemmater.7b00034.
Sang, Lingzi, Haasch, Richard T., Gewirth, Andrew A., & Nuzzo, Ralph G. Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping. United States. https://doi.org/10.1021/acs.chemmater.7b00034
Sang, Lingzi, Haasch, Richard T., Gewirth, Andrew A., and Nuzzo, Ralph G. Tue .
"Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping". United States. https://doi.org/10.1021/acs.chemmater.7b00034. https://www.osti.gov/servlets/purl/1388302.
@article{osti_1388302,
title = {Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping},
author = {Sang, Lingzi and Haasch, Richard T. and Gewirth, Andrew A. and Nuzzo, Ralph G.},
abstractNote = {Quasi-binary thiophosphate-based solid electrolytes (SEs) are attracting substantial interest for lithium batteries due to their outstanding room temperature ionic conductivities. This work describes reactions occurring at the solid electrolyte (SE)/Au interface during Li deposition and stripping for two exemplary SE materials: β-Li3PS4 (β-LPS) and Li10GeP2S12 (LGPS). We used in situ Raman spectroscopy, along with X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) to evaluate potential-dependent changes in the chemistry of these materials at active electrode interfaces. For β-LPS, a partially reversible conversion of PS43– to P2S64– was found along with the formation of Li2S during Li deposition and stripping. In contrast, LGPS exhibited only irreversible changes at potentials below 0.7 V vs Li+/Li. The different behaviors likely relate to differences in the structures of the two SE materials and the availability of easily bridged anion components in close proximity. In conclusion, the work shows that SE integrity at interfaces can be altered by applied potential and illustrates important speciations for the interfacial structures that mediate their electrochemical activities.},
doi = {10.1021/acs.chemmater.7b00034},
journal = {Chemistry of Materials},
number = 7,
volume = 29,
place = {United States},
year = {Tue Mar 14 00:00:00 EDT 2017},
month = {Tue Mar 14 00:00:00 EDT 2017}
}
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