| Autor: |
Szczuka C; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.; Institute of Energy and Climate Research (IEK-9), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany.; Institute of Physical Chemistry, RWTH Aachen University, 52056 Aachen, Germany., Karasulu B; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.; Department of Chemistry, University of Warwick, Gibbet Hill Road, Coventry CV4 7AL, U.K., Groh MF; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K., Sayed FN; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.; The Faraday Institution, Quad One, Harwell Campus, Didcot OX11 0RA, U.K., Sherman TJ; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K., Bocarsly JD; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.; The Faraday Institution, Quad One, Harwell Campus, Didcot OX11 0RA, U.K., Vema S; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.; The Faraday Institution, Quad One, Harwell Campus, Didcot OX11 0RA, U.K., Menkin S; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.; The Faraday Institution, Quad One, Harwell Campus, Didcot OX11 0RA, U.K., Emge SP; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K., Morris AJ; School of Metallurgy and Materials, University of Birmingham, Birmingham B15 2TT, U.K., Grey CP; Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K. |
| Abstrakt: |
All-solid-state batteries based on non-combustible solid electrolytes are promising candidates for safe energy storage systems. In addition, they offer the opportunity to utilize metallic lithium as an anode. However, it has proven to be a challenge to design an electrolyte that combines high ionic conductivity and processability with thermodynamic stability toward lithium. Herein, we report a new highly conducting solid solution that offers a route to overcome these challenges. The Li-P-S ternary was first explored via a combination of high-throughput crystal structure predictions and solid-state synthesis (via ball milling) of the most promising compositions, specifically, phases within the Li 3 P-Li 2 S tie line. We systematically characterized the structural properties and Li-ion mobility of the resulting materials by X-ray and neutron diffraction, solid-state nuclear magnetic resonance spectroscopy (relaxometry), and electrochemical impedance spectroscopy. A Li 3 P-Li 2 S metastable solid solution was identified, with the phases adopting the fluorite (Li 2 S) structure with P substituting for S and the extra Li + ions occupying the octahedral voids and contributing to the ionic transport. The analysis of the experimental data is supported by extensive quantum-chemical calculations of both structural stability, diffusivity, and activation barriers for Li + transport. The new solid electrolytes show Li-ion conductivities in the range of established materials, while their composition guarantees thermodynamic stability toward lithium metal anodes. |
