Toluene Tolerated Li<sub>9.88</sub>GeP<sub>1.96</sub>Sb<sub>0.04</sub>S<sub>11.88</sub>Cl<sub>0.12</sub> Solid Electrolyte toward Ultrathin Membranes for All-Solid-State Lithium Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 36535024.
- Also identified by DOI 10.1021/acs.nanolett.2c04140.
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Abstract
Sulfide solid electrolyte membranes employed in all-solid-state lithium batteries generally show high thickness and poor chemical stability, which limit the cell-level energy density and cycle life. In this work, Li<sub>9.88</sub>GeP<sub>1.96</sub>Sb<sub>0.04</sub>S<sub>11.88</sub>Cl<sub>0.12</sub> solid electrolyte is synthesized with Sb, Cl partial substitution of P, S, possessing excellent toluene tolerance and stability to lithium. The formed SbS<sub>4</sub><sup>3-</sup> group in Li<sub>9.88</sub>GeP<sub>1.96</sub>Sb<sub>0.04</sub>S<sub>11.88</sub>Cl<sub>0.12</sub> exhibits low adsorption energy and reactivity for toluene molecules, confirmed by first-principles density functional theory calculation. Using toluene as the solvent, ultrathin Li<sub>9.88</sub>GeP<sub>1.96</sub>Sb<sub>0.04</sub>S<sub>11.88</sub>Cl<sub>0.12</sub> membranes with adjustable thicknesses can be well prepared by the wet coating method, and an 8 μm thick membrane exhibits an ionic conductivity of 1.9 mS cm<sup>-1</sup> with ultrahigh ionic conductance of 1860 mS and ultralow areal resistance of 0.68 Ω cm<sup>-2</sup> at 25 °C. The obtained LiCoO<sub>2</sub>|Li<sub>9.88</sub>GeP<sub>1.96</sub>Sb<sub>0.04</sub>S<sub>11.88</sub>Cl<sub>0.12</sub> membrane|Li all-solid-state lithium battery shows an initial reversible capacity of 125.6 mAh g<sup>-1</sup> with a capacity retention of 86.3% after 250 cycles at 0.1 C under 60 °C.