%0 Journal Article
%A Szczuka, Conrad
%A Karasulu, Bora
%A Groh, Matthias F.
%A Sayed, Farheen N.
%A Sherman, Timothy J.
%A Bocarsly, Joshua D.
%A Vema, Sundeep
%A Menkin, Svetlana
%A Emge, Steffen P.
%A Morris, Andrew J.
%A Grey, Clare P.
%T Forced Disorder in the Solid Solution Li3P–Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes
%J Journal of the American Chemical Society
%V 144
%N 36
%@ 0002-7863
%C Washington, DC
%I American Chemical Society
%M FZJ-2022-03450
%P 16350 - 16365
%D 2022
%X 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 Li3P–Li2S 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 Li3P–Li2S metastable solid solution was identified, with the phases adopting the fluorite (Li2S) 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%$ 36040461
%U <Go to ISI:>//WOS:000850684900001
%R 10.1021/jacs.2c01913
%U https://juser.fz-juelich.de/record/909829