Wet-Milling Synthesis of Superionic Lithium Argyrodite Electrolytes with Different Concentrations of Lithium Vacancy

Liping Wu; Zhichao Zhang; Gaozhan Liu; Wei Weng; Zhihua Zhang; Xiayin Yao

doi:10.1021/acsami.1c13031

Wet-Milling Synthesis of Superionic Lithium Argyrodite Electrolytes with Different Concentrations of Lithium Vacancy

ACS Appl Mater Interfaces. 2021 Oct 6;13(39):46644-46649. doi: 10.1021/acsami.1c13031. Epub 2021 Sep 22.

Authors

Liping Wu^{1

2}, Zhichao Zhang¹, Gaozhan Liu^{1

2}, Wei Weng^{1

2}, Zhihua Zhang¹, Xiayin Yao^{1

2}

Affiliations

¹ Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, P. R. China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, P. R. China.

PMID: 34549943
DOI: 10.1021/acsami.1c13031

Abstract

The ionic conductivities of argyrodite electrolytes are significantly affected by the concentrations of lithium vacancy. Herein, a facile and rapid synthesis route is proposed to systematically investigate Li_6-xPS_5-xCl_1+x (0 ≤ x ≤ 0.8) with different lithium vacancies by adjusting ratios of S/Cl. The highest ionic conductivity of the wet-milling synthesized Li_5.4PS_4.4Cl_1.6 is 6.18 mS cm^-1, which is attributed to higher lithium vacancy concentration and lower electrostatic interaction for ion migration. The Li/Li_5.4PS_4.4Cl_1.6/Li symmetric cell cycles stably for 2000 h at 0.1 mA cm^-2, showing excellent dendrite suppression capability. Moreover, the initial discharge capacity of LiCoO₂/Li_5.4PS_4.4Cl_1.6/Li all-solid-state battery is 126.0 mAh g^-1 at 0.1C and the capacity retention is 83% after 50 cycles. The wet-milling method provides the possibility for rapid exploration and preparation of other argyrodite electrolytes in the future.

Keywords: Li5.4PS4.4Cl1.6; all-solid-state lithium batteries; conductivity; lithium vacancy; wet-milling.