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A titanium-substituted lithium-excess molyb-denum oxyfluoride, Li2.1?yTi0.2Mo0.7O2F, is synthesized bymechanical milling and tested as a positive electrode materialin a conventional carbonate-based electrolyte or concentratedelectrolyte. Reversibility as the electrode material issignificantly improved by suppression of dissolution of themolybdenum oxyfluoride on electrochemical cycles.Li2.1?yTi0.2Mo0.7O2F delivers a reversible capacity of 265 mAhg?1after 30 cycles at a rate of 50 mA g?1with concentratedelectrolyte. Thisfinding contributes to the development ofhigh-energy and long-cycle-life rechargeable lithium batterieswith lithium-excess metal oxyfluorides in the future.