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Issue 40, 2017
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Revealing the relation between the structure, Li-ion conductivity and solid-state battery performance of the argyrodite Li6PS5Br solid electrolyte

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Abstract

Based on its high Li-ion conductivity, argyrodite Li6PS5Br is a promising solid electrolyte for all-solid-state batteries. However, more understanding is required on the relation between the solid electrolyte conductivity and the solid-state battery performance with the argyrodite structure, crystallinity and particle size that depend on the synthesis conditions. In the present study, this relationship is investigated using neutron and X-ray diffraction to determine the detailed structure and impedance as well as 7Li solid state NMR spectroscopy to study the Li-ion kinetics. It is found that depending on the synthesis conditions the distribution of the Br dopant over the crystallographic sites in Li6PS5Br is inhomogeneous, and that this may be responsible for a larger mobile Li-ion fraction in the interfacial regions in the annealed argyrodite materials. Comparing the bulk and interfacial properties of the differently prepared Li6PS5Br materials, it is proposed that optimal solid-state battery performance requires a different particle size for the solid electrolyte only region and the solid electrolyte in the cathode mixture. In the electrolyte region, the grain boundary resistance is minimized by annealing the argyrodite Li6PS5Br resulting in relatively large crystallites. In the cathode mixture however, additional particle size reduction of the Li6PS5Br is required to provide abundant Li6PS5Br–Li2S interfaces that reduce the resistance of this rate limiting step in Li-ion transport. Thereby the results give insight into how to improve solid-state battery performance by controlling the solid electrolyte structure.

Graphical abstract: Revealing the relation between the structure, Li-ion conductivity and solid-state battery performance of the argyrodite Li6PS5Br solid electrolyte

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Publication details

The article was received on 09 Jun 2017, accepted on 11 Sep 2017 and first published on 14 Sep 2017


Article type: Paper
DOI: 10.1039/C7TA05031C
Citation: J. Mater. Chem. A, 2017,5, 21178-21188
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    Revealing the relation between the structure, Li-ion conductivity and solid-state battery performance of the argyrodite Li6PS5Br solid electrolyte

    C. Yu, S. Ganapathy, E. R. H. van Eck, L. van Eijck, S. Basak, Y. Liu, L. Zhang, Henny W. Zandbergen and M. Wagemaker, J. Mater. Chem. A, 2017, 5, 21178
    DOI: 10.1039/C7TA05031C

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