Protective Nanosheet Coatings for Thiophosphate-Based All-Solid-State Batteries

Superionic sulfide solid electrolytes (SEs) are of considerable interest for application in solid-state batteries, but suffer from limited stability. When in combination with state-of-the-art cathode active materials (CAMs), severe degradation at the CAM/SE interface occurs during electrochemical cycling. To improve upon the interfacial stability, inert coatings can be applied to the CAM particles, with the goal of preventing direct contact to the SE. In this study, different methods of depositing coatings, including hexagonal boron nitride, tungsten sulfide and exfoliated ((CH3(CH2)3)4N)4Nb6O17, in the form of nanosheets onto the free surface of a Ni-rich LiNixCoyMnzO2 (NCM) CAM are examined and compared with one another. While dry coating is shown to produce relatively uniform coatings (good surface coverage), the secondary particle morphology of the NCM makes ball milling as a mechanical deposition method less attractive. In contrast, deposition from dispersions in organic solvents yields protective coatings with a lower degree of surface coverage. The different materials are electrochemically tested in liquid- and solid-electrolyte-based lithium-ion batteries. A stabilizing effect from nanosheet coating is only observed for the cells with lithium thiophosphate SE. Various materials in the form of nanosheets are examined with regards to their use as protective coatings in liquid- and solid-electrolyte-based lithium-ion batteries. WS2 and LixNbOy nanosheets are found to have a positive effect on the cycling performance of thiophosphate-based solid-state batteries. image