Unraveling the Role of Earth-Abundant Fe in the Suppression of Jahn-Teller Distortion of P'2-Type Na 2/3 MnO 2 : Experimental and Theoretical Studies.

Layered Na2/3MnO2 suffers from capacity loss due to Jahn-Teller (J-T) distortion by Mn3+ ions. Herein, density functional theory calculations suggest Na2/3[FexMn1-x]O2 suppresses the J-T effect. The Fe substitution results in a decreased oxygenmetaloxygen length, leading to decreases in the b, c lattice parameters but an increase in the a lattice constant. As a result, the capacity retention and rate capability are enhanced with additional redox pair associated with Fe4+/3+. Finally, the thermal properties are improved, with the Fe substitution delaying the exothermic reaction and reducing exothermic heat.