<i>In Situ</i> Probing Potassium-Ion Intercalation-Induced Amorphization in Crystalline Iron Phosphate Cathode Materials.

Abstract

Na-ion and K-ion batteries are promising alternatives for large-scale energy storage due to their abundance and low cost. Intercalation of these large ions could cause irreversible structural deformation and partial to complete amorphization in the crystalline electrodes. A lack of understanding of the dynamic changes in the amorphous nanostructure during battery operation is the bottleneck for further developments. Here, we report the utilization of in-<i>operando</i> digital image correlation and XRD techniques to probe dynamic changes in the amorphous phase of iron phosphate during potassium ion intercalation. In-<i>operando</i> XRD demonstrates amorphization in the electrode's nanostructure during the first charge and discharge cycle. Additionally, <i>ex situ</i> HR-TEM further confirms the amorphization after potassium-ion intercalation. An <i>in situ</i> strain analysis detects reversible deformations associated with redox reactions in the amorphous phases. Our approach offers new insights into the mechanism of ion intercalation in the amorphous nanostructure which are highly potent for the development of next-generation batteries.