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Cited by 719

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Elucidating Reversible Electrochemical Redox of Li6PS5Cl Solid Electrolyte

Open access
Tan, Darren H. S., Wu, Erik A., Nguyen, Han, Chen, Zheng, Marple, Maxwell A. T., Doux, Jean-Marie, Wang, Xuefeng, Yang, Hedi, Banerjee, Abhik, Meng, Ying Shirley·2019·ACS Energy Letters

Abstract

Sulfide-based solid electrolytes are promising candidates for all solid-state batteries (ASSBs) due to their high ionic conductivity and ease of processability. However, their narrow electrochemical stability window causes undesirable electrolyte decomposition. Existing literature on Li-ion ASSBs report an irreversible nature of such decompositions, while Li–S ASSBs show evidence of some reversibility. Here, we explain these observations by investigating the redox mechanism of argyrodite Li 6 PS 5 Cl at various chemical potentials. We found that Li–In | Li 6 PS 5 Cl | Li 6 PS 5 Cl–C half-cells can be cycled reversibly, delivering capacities of 965 mAh g –1 for the electrolyte itself. During charging, Li 6 PS 5 Cl forms oxidized products of sulfur (S) and phosphorus pentasulfide (P 2 S 5 ), while during discharge, these products are first reduced to a Li 3 PS 4 intermediate before forming lithium sulfide (Li 2 S) and lithium phosphide (Li 3 P). Finally, we quantified the relative contributions of the products toward cell impedance and proposed a strategy to reduce electrolyte decomposition and increase cell Coulombic efficiency.

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Metadata

Authors
Tan, D. H. S., Wu, E. A., Nguyen, H., Chen, Z., Marple, M. A. T., Doux, J.-M., Wang, X., Yang, H., Banerjee, A., & Meng, Y. S.
Venue
ACS Energy Letters
Published
2019-08-20
Volume
4
Issue
10
Pages
2418-2427
ISSN
2380-8195 (ISSN-L)
OpenAlex
W2969387578
Cited by
719
References
27
FWCI
13.75
Type
journal article
Language
en
Open access
green

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CoChat. (2026). Citation check: Elucidating Reversible Electrochemical Redox of Li6PS5Cl Solid Electrolyte. https://app.cochat.ai/papers/10.1021/acsenergylett.9b01693
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Tan, D. H. S., Wu, E. A., Nguyen, H., Chen, Z., Marple, M. A. T., Doux, J.-M., Wang, X., Yang, H., Banerjee, A., & Meng, Y. S. (2019). Elucidating Reversible Electrochemical Redox of Li6PS5Cl Solid Electrolyte. ACS Energy Letters. https://doi.org/10.1021/acsenergylett.9b01693

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