Abstract
AbstractRechargeable magnesium batteries are identified as a promising next‐generation energy storage system, but their development is hindered by the anode−electrolyte−cathode incompatibilities and passivation of magnesium metal anode. To avoid or alleviate these problems, the exploitation of alternative anode materials is a promising choice. Herein, we present titanium pyrophosphate (TiP2O7) as anode materials for magnesium‐ion batteries (MIBs) and investigate the effect of the crystal phase on its magnesium storage performance. Compared with the metastable layered TiP2O7, the thermodynamically stable cubic TiP2O7 displays a better rate capability of 72 mAh g−1 at 5000 mA g−1. Moreover, cubic TiP2O7 exhibits excellent cycling stability with the capacity of 60 mAh g−1 after 5000 cycles at 1000 mA g−1, which are better than previously reported Ti‐based anode materials for MIBs. In situ X‐ray diffraction technology confirms the single‐phase magnesium‐ion intercalation/deintercalation reaction mechanism of cubic TiP2O7 with a low volume change of 3.2%. In addition, the density functional theory calculation results demonstrate that three‐dimensional magnesium‐ion diffusion can be allowed in cubic TiP2O7 with a low migration energy barrier of 0.62 eV. Our work demonstrates the promise of TiP2O7 as high‐rate and long‐life anode materials for MIBs and may pave the way for further development of MIBs.
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