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

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

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  • Media type: E-Article
  • Title: Forced Disorder in the Solid Solution Li3P–Li2S: A New Class of Fully Reduced Solid Electrolytes for Lithium Metal Anodes
  • Contributor: Szczuka, Conrad [Author]; Karasulu, Bora [Author]; Grey, Clare P. [Author]; Groh, Matthias F. [Author]; Sayed, Farheen N. [Author]; Sherman, Timothy J. [Author]; Bocarsly, Joshua D. [Author]; Vema, Sundeep [Author]; Menkin, Svetlana [Author]; Emge, Steffen P. [Author]; Morris, Andrew J. [Author]
  • Published: American Chemical Society, 2022
  • Published in: Journal of the American Chemical Society 144(36), 16350 - 16365 (2022). doi:10.1021/jacs.2c01913
  • Language: English
  • DOI: https://doi.org/10.1021/jacs.2c01913
  • ISSN: 1943-2984; 1520-5126; 0002-7863
  • Origination:
  • Footnote: Diese Datenquelle enthält auch Bestandsnachweise, die nicht zu einem Volltext führen.
  • Description: 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.
  • Access State: Open Access