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The development of an energy storage system with abundant elements is a key challenge for a sustainable society, and the interest of Na intercalation chemistry is extending throughout the research community. Herein, the impact of Ti integration into NaMnO 2  in a binary system of   x   NaMnO 2 –(  1  –  x  ) TiO 2  (  0.5  ≤  x  ≤  1  ) is systematically examined for rechargeable Na battery applications. Stoichiometric NaMnO 2 , which is classified as an in-plane distorted O′    3-type layered structure, delivers a large initial discharge capacity of approximately 200 mAh g -1 , but insufficient capacity retention is observed, most probably associated with dissolution of Mn ions on electrochemical cycles. Ti-substituted samples show highly improved electrode performance as electrode materials. However, the appearance of a sodium-deficient phase, Na 4 Mn 4 Ti 5 O 18  with a tunnel-type structure, is observed for Ti-rich phases. Among the samples in this binary system, Na 0.8 Mn 0.8 Ti 0.2 O 2  (  x  =  0.8  ), which is a mixture of a partially Ti-substituted O′    3-type layered oxide (Na 0.88 Mn 0.88 Ti 0.12 O 2 ) and tunnel-type Na 4 Mn 4 Ti 5 O 18  as a minor phase elucidated by Rietveld analysis on both neutron and X-ray diffraction patterns, shows good electrode performance on the basis of energy density and cyclability. Both phases are electrochemically active as evidenced by  in situ  X-ray diffraction study, and the improvement of reversibility originates from the suppression of Mn dissolution on electrochemical cycles. From these results, the feasibility of Mn-based electrode materials for high-energy rechargeable Na batteries made from only abundant elements is discussed in detail.

Efficient Stabilization of Na Storage Reversibility by Ti Integration into O′3-Type NaMnO 2

Efficient Stabilization of Na Storage Reversibility by Ti Integration into O′3-Type NaMnO ₂