ISIS Neutron and Muon Source Data Journal

Elucidating the structure and ion transport mechanism in lithium halospinels and high-entropy lithium metal chlorides solid electrolytes

Abstract: Lithium metal chloride solid electrolytes are regarded as promising candidate for applying in all-solid-state batteries as they show good ionic conductivities of > 1 mS cm-1 at room temperature and good electrochemical compatibility with 4V class cathode materials. In this project, we developed Zr4+, Al3+, Fe3+ and Mg2+ doped Li2±xSc1-xMxCl4 halospinel with ionic conductivities up to 1.8 mS cm-1. However, the conductivity of Al3+, Fe3+, Mg2+ doped halospinel is < 1 mS cm-1 and lower than computational prediction. We ascribe the reason not only to the different sizes of lattice framework from different sizes of metal dopant, but to a different lithium distribution over the 8a, 16c, 16d and 48f sites. We propose high resolution neutron powder diffraction to elucidate the halospinel structure and especially lithium sublattice at room temperature and 10K. The low temperature data will reduce thermal diffuse scattering and give insights on the origin of high energy 48f site occupancy. We also developped high entropy Li2.05MCl6 (M=Zr, Mg, Ca, Y, Sc, Ho) crystallizing in orthorhombic crystal system, different from the parent structure trigonal Li2ZrCl6, with a 4-fold ionic conductivity boost to 1.6 mS cm-1. All data will be used for Rietveld refinement analysis and combined with negative fourier density map to find all lithium locations, the results will help us elucidating the structure and ion transport mechanism in lithium metal chloride materials.

Public release date: 30 April 2027

Principal Investigator: Professor Linda Nazar
Experimenter: Mr Issei Otani
Local Contact: Dr Dominic Fortes
Experimenter: Mr Yubo Wang
Experimenter: Dr Zhuo Yu

DOI: 10.5286/ISIS.E.RB2467004-1

Parent DOI: 10.5286/ISIS.E.RB2467004

ISIS Experiment Number: RB2467004

Part Number: 1

Date of Experiment: 18 March 2024

Publisher: STFC ISIS Neutron and Muon Source

Data format: RAW/Nexus
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Data Citation

The recommended format for citing this dataset in a research publication is as:
[author], [date], [title], [publisher], [doi]

For Example:
Professor Linda Nazar et al; (2024): Elucidating the structure and ion transport mechanism in lithium halospinels and high-entropy lithium metal chlorides solid electrolytes, STFC ISIS Neutron and Muon Source, https://doi.org/10.5286/ISIS.E.RB2467004-1

Data is released under the CC-BY-4.0 license.