Abstract
Computational and experimental work directed at exploring the electrochemical properties of tetrahedrally coordinated Mn in the +5 oxidation state is presented. Specific capacities of nearly 700 mAh g −1 are predicted for the redox processes of Li x MnO 4 complexes based on two two-phase reactions. One is topotactic extraction of Li from Li 3MnO 4 to form LiMnO 4 and the second is topotactic insertion of Li into Li 3MnO 4 to form Li 5MnO 4. In the experiments, it is found that the redox behavior of Li 3MnO 4 is complicated by disproportionation of Mn 5+ in solution to form Mn 4+ and Mn 7+ and by other irreversible processes; although an initial capacity of about 275 mAh g −1 in lithium cells was achieved. Strategies based on structural considerations to improve the electrochemical properties of MnO 4 n− complexes are given.
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