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Spatially Decoupled Charge Compensation Enables Versatile Cation-Anion Co-Intercalation in Layered Metal Oxide
Huabin Kong1, Jianxin Ou1, Lei Fang1
1College of Materials Science and Engineering, Huaqiao University, Xiamen, Fujian, China.
Abstract:
Multivalent cation-anion co-(de)intercalation offers a promising pathway to higher energy densities in multivalent ion batteries. However, its practical realization is challenged by lattice strain and the lack of effective dual charge-compensation strategies. Here, we report a layered vanadium oxide cathode with pre-intercalated melamine ligands (MeVO) that enables a spatially decoupled charge-compensation mechanism-organic ligands serve as redox centers for anions, while metal sites accommodate multivalent cation redox. This design alleviates electrostatic crowding, promotes ion mobility, and preserves structural integrity. Using Mg2 +-TFSI- as a representative system, MeVO delivers a record cycle life of over 36 000 cycles at a loading of approximately 3 mg cm- 2 and an areal capacity of 3.3 mAh cm- 2 at a higher loading of 16.4 mg cm- 2, surpassing leading Mg-ion cathodes. The hybrid structure also supports co-(de)intercalation of various multivalent cations and anions, demonstrating its potential as a versatile intercalation platform for high-performance energy storage.
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