A cost-effective, ionically conductive and compressible oxychloride solid-state electrolyte for stable all-solid-state lithium-based batteries.

Hu, Lv; Wang, Jinzhu; Wang, Kai; Gu, Zhenqi; Xi, Zhiwei; Li, Hui; Chen, Fang; Wang, Youxi et al. · Nat Commun · 2023

basic_science · Level V

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Abstract

To enable the development of all-solid-state batteries, an inorganic solid-state electrolyte should demonstrate high ionic conductivity (i.e., > 1 mS cm<sup>-1</sup> at 25 °C), compressibility (e.g., > 90% density under 250-350 MPa), and cost-effectiveness (e.g., < $50/kg). Here we report the development and preparation of Li<sub>1.75</sub>ZrCl<sub>4.75</sub>O<sub>0.5</sub> oxychloride solid-state electrolyte that demonstrates an ionic conductivity of 2.42 mS cm<sup>-1</sup> at 25 °C, a compressibility enabling 94.2% density under 300 MPa and an estimated raw materials cost of $11.60/kg. As proof of concept, the Li<sub>1.75</sub>ZrCl<sub>4.75</sub>O<sub>0.5</sub> is tested in combination with a LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub>-based positive electrode and a Li<sub>6</sub>PS<sub>5</sub>Cl-coated Li-In negative electrode in lab-scale cell configuration. This all-solid-state cell delivers a discharge capacity retention of 70.34% (final discharge capacity of 70.2 mAh g<sup>-1</sup>) after 2082 cycles at 1 A g<sup>-1</sup>, 25 °C and 1.5 tons of stacking pressure.