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Tailoring Li6PS5Br ionic conductivity and understanding of its role in cathode mixtures for high performance all-solid-state Li–S batteries

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Abstract

The ultrafast ionic conductivity of Li6PS5Br, which is higher than 1 mS cm−1 at room temperature, makes it an attractive candidate electrolyte for the all-solid-state Li–S battery. A simple synthesis route with an easy scale up process is critical for practical applications. In this work, the highest room temperature ionic conductivity (2.58 × 10−3 S cm−1) of Li6PS5Br is obtained by an optimal annealing temperature in a simple solid-state reaction method. Neutron diffraction and XRD show that the origin of the highest ionic conductivity is due to the higher purity, smaller mean lithium ion jumps and the optimal Br ordering over 4a and 4c sites. All-solid-state Li–S batteries using a S–C composite cathode in combination with the optimized Li6PS5Br electrolyte and Li–In anode show high (dis)charge capacities. Different cycling modes (charge–discharge and discharge–charge) reveal that the capacity of the S–C–Li6PS5Br/Li6PS5Br/Li–In battery arises from both the active S–C composite and the Li6PS5Br in the cathode mixture. The contribution of the latter is verified from all-solid-state batteries using Li6PS5Br and its analogues as active materials. Ex situ XRD and electrochemical performance results show that the contribution of capacity from Li6PS5Br in the cathode mixture may be associated with the decomposition product Li2S, while the Li6PS5Br in the bulk solid electrolyte layer is stable during cycling.

Graphical abstract: Tailoring Li6PS5Br ionic conductivity and understanding of its role in cathode mixtures for high performance all-solid-state Li–S batteries

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Publication details

The article was received on 25 Feb 2019, accepted on 26 Mar 2019 and first published on 05 Apr 2019


Article type: Paper
DOI: 10.1039/C9TA02126D
Citation: J. Mater. Chem. A, 2019, Advance Article

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    Tailoring Li6PS5Br ionic conductivity and understanding of its role in cathode mixtures for high performance all-solid-state Li–S batteries

    C. Yu, J. Hageman, S. Ganapathy, L. van Eijck, L. Zhang, K. R. Adair, X. Sun and M. Wagemaker, J. Mater. Chem. A, 2019, Advance Article , DOI: 10.1039/C9TA02126D

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