Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping

Sang, Lingzi; Haasch, Richard T.; Gewirth, Andrew A.; Nuzzo, Ralph G.

doi:10.1021/acs.chemmater.7b00034

Title: Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping

Journal Article · 14 March 2017 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.7b00034 · OSTI ID:1388302

Sang, Lingzi ^[1];

^[1];

^[1]; Nuzzo, Ralph G. ^[1]

Univ. of Illinois at Urbana−Champaign, Urbana, IL (United States)

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 PS₄^3– to P₂S₆^4– 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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1388302

Journal Information:: Chemistry of Materials, Vol. 29, Issue 7; Related Information: CEES partners with Argonne National Laboratory (lead); University of Illinois, Urbana-Champaign; Northwest University; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping

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