Peeking across Grain Boundaries in a Solid-State Ionic Conductor

Swapna Ganapathy, Chuang Yu, Ernst R.H. Van Eck, Marnix Wagemaker

Research output: Contribution to journalArticleScientificpeer-review

26 Citations (Scopus)
110 Downloads (Pure)

Abstract

The development of high-performance all-solid-state batteries relies on charge transport in solid electrolytes, where transport across grain boundaries often limits their bulk conductivity. The argyrodite Li 6 PS 5 X (X = Cl, Br) solid electrolyte has a high conductivity; however, macroscopic diffusion in this material involves complex jump processes, which leads to an underestimation of the activation energy. Using a comprehensive frequency- and temperature-dependent analysis of the spin-lattice relaxation rates, a complete estimation of Li self-diffusion is demonstrated. Another experimental challenge is quantifying the impact of grain boundaries on the total bulk conductivity. Li 6 PS 5 Cl and Li 6 PS 5 Br have identical crystalline structures, but with 6 Li MAS NMR, their resonance peaks have different chemical shifts. Exploiting this with two-dimensional 6 Li- 6 Li exchange NMR on a mixture of Li 6 PS 5 Br and Li 6 PS 5 Cl, we observe Li exchange between particles of these two materials across grain boundaries, allowing direct and unambiguous quantification of this often limiting process in solid-state electrolytes.

Original languageEnglish
Pages (from-to)1092-1097
JournalACS Energy Letters
Volume4
Issue number5
DOIs
Publication statusPublished - 2019

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