First 18650-format Na-ion cells aging investigation: A degradation mechanism study

Several Hard carbon||Na3V2(PO4)2F3 full-cells in 18650-format are assembled to demonstrate the possible use of SIBs in stationary applications. The cell aging process is investigated in two different conditions: (i) continuous cycling at different current rates, and (ii) storage at different states-of-charge at various temperatures. The obtained results reveal that the cell degradation depends strongly on the temperature, current rates applied in cycling conditions, or state-of-charge of the storage test. Under cycling conditions, the continuous sodiation/desodiation may induce significant mechanical deformation, leading to the detachment of active materials from the current collector. Furthermore, the post-mortem analysis shows that reaction rate and aging process are not homogeneous along the electrode roll. The XRD analysis shows that Na3V2(PO4)2F3 structure is robust; nevertheless, the material cannot recover the initial Na+ content as the cycling progresses, which is the main cause for capacity loss in the positive electrode. The solid-electrolyte interphase present on the hard carbon surface was characterised using XPS. The hard carbon electrode cannot be detected during this study, evidencing the formation of a relatively thick (>5 nm) passivating layer composed of carbonate salts and NaF, which are the main products of electrolyte decomposition.