Abstract

Although Mg–Li hybrid batteries are proposed as an alternative to Mg-batteries, the lack of dual-ion compatible cathodes are limiting their practical application. Herein, we report a high-rate and ultralong-life Mg–Li hybrid battery based on a dual-phase TiO2 cathode. Highly pseudocapacitive hierarchical two-dimensional TiO2 consists of anatase (60%) and bronze (40%) nanocrystallites forming interfaces due to crystal structure mismatch. This dual-phase hierarchical cathode exhibits excellent pseudocapacitance (up to 92%), specific capacities (235 mAh/g @ 25 mA/g), rate performance (120 mAh/g @ 1A/g) cycling stability (~87% after 3000 cycles @ 1A/g) and coulombic efficiency (~100%). These results are vastly superior to the previously reported values for TiO2 based Mg–Li hybrid battery cathodes. Only minimal structural changes are observed during the charge-discharge of two-dimensional TiO2 electrode. Outstanding electrochemical performance of dual-phase TiO2 nanosheet cathode is attributed to the superior pseudocapacitive Mg/Li-ion diffusion through nanointerfaces between anatase and bronze crystallites. While other structural features such as 2D-morphology, ultrathin nature, mesoporosity, and high surface area act as secondary factors. The demonstrated approach for efficient pseudocapacitive Mg/Li-ion intercalation enhanced by nanointerfaces can be further exploited in the development of other high performance electrodes for advanced Mg–Li hybrid batteries.

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