Visualizing Lithium Ion Transport in Solid‐State Li–S Batteries Using ⁶Li Contrast Enhanced Neutron Imaging

Abstract The elucidation of lithium ion transport pathways through a solid electrolyte separator is a vital step toward development of reliable, functional all‐solid‐state batteries. Here, advantage has been taken of the significantly higher neutron attenuation coefficient of one of the most abundant stable isotopes of lithium, ⁶Li, with respect to that of naturally occurring lithium isotope mixture, to perform neutron imaging on a purpose built all‐solid‐state lithium–sulfur battery. Increasing the ⁶Li content in the anode while using natural lithium in the solid electrolyte separator and the cathode enhances the contrast such that it is possible to differentiate, during the initial discharge, between the mobile lithium ions diffusing through the cell from the anode and those that are initially located in the solid electrolyte. The sensitivity of neutrons to the different lithium isotopes means that operando neutron radiography allows demonstration of the lithium ion diffusion through the cell while in situ neutron tomography has permitted presentation, in three dimensions, of the distribution of the trapped lithium ions inside the cell in charged and discharged states.