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Szczuka, Conrad [Verfasser:in]; Karasulu, Bora [Verfasser:in]; Grey, Clare P. [Verfasser:in]; Groh, Matthias F. [Verfasser:in]; Sayed, Farheen N. [Verfasser:in]; Sherman, Timothy J. [Verfasser:in]; Bocarsly, Joshua D. [Verfasser:in]; Vema, Sundeep [Verfasser:in]; Menkin, Svetlana [Verfasser:in]; Emge, Steffen P. [Verfasser:in]; Morris, Andrew J. [Verfasser:in]

Forced Disorder in the Solid Solution Li3P–Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes

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  • Medientyp: E-Artikel
  • Titel: Forced Disorder in the Solid Solution Li3P–Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes
  • Beteiligte: Szczuka, Conrad [Verfasser:in]; Karasulu, Bora [Verfasser:in]; Grey, Clare P. [Verfasser:in]; Groh, Matthias F. [Verfasser:in]; Sayed, Farheen N. [Verfasser:in]; Sherman, Timothy J. [Verfasser:in]; Bocarsly, Joshua D. [Verfasser:in]; Vema, Sundeep [Verfasser:in]; Menkin, Svetlana [Verfasser:in]; Emge, Steffen P. [Verfasser:in]; Morris, Andrew J. [Verfasser:in]
  • Erschienen: American Chemical Society, 2022
  • Erschienen in: Journal of the American Chemical Society 144(36), 16350 - 16365 (2022). doi:10.1021/jacs.2c01913
  • Sprache: Englisch
  • DOI: https://doi.org/10.1021/jacs.2c01913
  • ISSN: 1943-2984; 1520-5126; 0002-7863
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  • Beschreibung: 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.
  • Zugangsstatus: Freier Zugang