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Spinel-type Li 4 Ti 5 O 12  is an attractive anode material for lithium-ion battery applications owing to its high specific energy and almost vanishing mechanical strain upon Li-(de)intercalation. The impact of oxygen non-stoichiometry and aliovalent Mg-doping on the defect chemistry of Li 4 Ti 5 O 12  has been characterized by quantitative electron paramagnetic resonance (EPR) spectroscopy. The results obtained demonstrate that the Mg 2+ -ions are amphoterically incorporated at the here studied concentrations on both lithium (Mg Li  • ) and titanium (Mg′′ Ti ) sites. Mg 2+ -doping thus simultaneously results in the formation of donor (Mg Li  • ) and acceptor (Mg′′ Ti ) centers. Furthermore, upon both oxygen deficiency and Mg 2+ -doping, the concentration of `polaronic'-type Ti 3+ -states is increased, accounting for the enhanced electronic conductivity.

zeitschrift für physikalische chemie

Mixed Ionic–Electronic Conducting Li 4 Ti 5 O 12  as Anode Material for Lithium Ion Batteries with Enhanced Rate Capability – Impact of Oxygen Non-Stoichiometry and Aliovalent Mg 2+ -Doping Studied by Electron Paramagnetic Resonance