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O3-type layered NaNi 0.5 Ti 0.5 O 2 , which has been reported previously as a promising cathode material for Na-ion batteries, has been characterized using comprehensive operando echniques combined with electrochemical and magnetization measurements. Operando Synchrotron diffraction revealed a reversible O3-P3 transformation during charge and discharge without any intermediate phases, which stands in contrast to NaNiO 2 and NaNi 0.5 Mn 0.5 O 2 . Operando X-ray absorption studies showed that the electrochemical process in the potential window of 1.5-4.2 V vs Na + /Na is sustained exclusively by Ni oxidation and reduction while Ti remains inactive. These findings are further supported by ex situ magnetization measurements, yielding a lower paramagnetic moment in the charged state in agreement with Ni oxidation. On the basis of these insights, we elaborate on the beneficial stabilizing effect of Ti. However, a strong C-rate dependence for NaNi 0.5 Ti 0.5 O 2 and NaNi 0.5 Mn 0.5 O 2 during cycling known from the literature points at a rather high influence of the original structure stacking and the associated Na migration paths.

acs applied materials and interfaces

Operando Studies on the NaNi0.5Ti0.5O2 Cathode for Na-Ion Batteries: Elucidating Titanium as a Structure Stabilizer