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000909829 0247_ $$2doi$$a10.1021/jacs.2c01913
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000909829 0247_ $$2ISSN$$a1943-2984
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000909829 1001_ $$0P:(DE-Juel1)179011$$aSzczuka, Conrad$$b0
000909829 245__ $$aForced Disorder in the Solid Solution Li3P–Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes
000909829 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2022
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000909829 520__ $$aAll-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.
000909829 536__ $$0G:(DE-HGF)POF4-1223$$a1223 - Batteries in Application (POF4-122)$$cPOF4-122$$fPOF IV$$x0
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000909829 7001_ $$00000-0001-8129-8010$$aKarasulu, Bora$$b1
000909829 7001_ $$00000-0002-7436-7177$$aGroh, Matthias F.$$b2
000909829 7001_ $$00000-0002-5700-5959$$aSayed, Farheen N.$$b3
000909829 7001_ $$00000-0002-3613-2043$$aSherman, Timothy J.$$b4
000909829 7001_ $$00000-0002-7523-152X$$aBocarsly, Joshua D.$$b5
000909829 7001_ $$00000-0002-9894-5293$$aVema, Sundeep$$b6
000909829 7001_ $$00000-0003-3612-4542$$aMenkin, Svetlana$$b7
000909829 7001_ $$00000-0001-8613-9465$$aEmge, Steffen P.$$b8
000909829 7001_ $$00000-0001-7453-5698$$aMorris, Andrew J.$$b9
000909829 7001_ $$00000-0001-5572-192X$$aGrey, Clare P.$$b10$$eCorresponding author
000909829 773__ $$0PERI:(DE-600)1472210-0$$a10.1021/jacs.2c01913$$gVol. 144, no. 36, p. 16350 - 16365$$n36$$p16350 - 16365$$tJournal of the American Chemical Society$$v144$$x0002-7863$$y2022
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