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|Title:||The unique structural evolution of the O3-phase Na2/3Fe2/3Mn1/3O2 during high rate charge/discharge: a sodium-centred perspective|
|Publisher:||John Wiley & Sons, Inc|
|Citation:||Sharma, N., Gonzalo, E., Pramudita, J. C., Han, M. H., Brand, H. E. A., Hart, J. N., Pang, W. K., Guo, Z. P. & Rojo, T. (2015). The unique structural evolution of the O3‐phase Na2/3Fe2/3Mn1/3O2 during high rate charge/discharge: a sodium‐centred perspective. Advanced Functional Materials, 25(31), 4994-5005. doi:10.1002/adfm.201501655|
|Abstract:||The development of new insertion electrodes in sodium-ion batteries requires an in-depth understanding of the relationship between electrochemical performance and the structural evolution during cycling. To date in situ synchrotron X-ray and neutron diffraction methods appear to be the only probes of in situ electrode evolution at high rates, a critical condition for battery development. Here, the structural evolution of the recently synthesized O3-phase of Na2/3Fe2/3Mn1/3O2 is reported under relatively high current rates. The evolution of the phases, their lattice parameters, and phase fractions, and the sodium content in the crystal structure as a function of the charge/discharge process are shown. It is found that the O3-phase persists throughout the charge/discharge cycle but undergoes a series of two-phase and solid-solution transitions subtly modifying the sodium content and atomic positions but keeping the overall space-group symmetry (structural motif). In addition, for the first time, evidence of a structurally characterized region is shown that undergoes two-phase and solid-solution phase transitions simultaneously. The Mn/Fe-O bond lengths, c lattice parameter evolution, and the distance between the Mn/FeO6 layers are shown to concertedly change in a favorable manner for Na+ insertion/extraction. The exceptional electrochemical performance of this electrode can be related in part to the electrode maintaining the O3-phase throughout the charge/discharge process. © 2015 Wiley-VCH Verlag GmbH & Co.|
|Appears in Collections:||Journal Articles|
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