Realizing Dual-Mode\nZinc-Ion Storage of Generic Vanadium-Based\nCathodes via Organic Molecule Intercalation

Intercalation\nengineering is a promising strategy to\npromote zinc-ion\nstorage of layered cathodes; however, is impeded by the complex fabrication\nroutes and inert electrochemical behaviors of intercalators. Herein,\nan organic imidazole intercalation strategy is proposed, where V<sub>2</sub>O<sub>5</sub> and NH<sub>4</sub>V<sub>3</sub>O<sub>8</sub> (NVO) model materials are adopted to verify the feasibility of the\nimidazole intercalator in improving the zinc storage capabilities\nof vanadium-based cathodes. The intercalated imidazole molecules could\nnot only expand interlayer spacing and strengthen structural stability\nby serving as extra “pillars” but also provide extra\ncoordination sites for zinc storage via the coordination reaction\nbetween Zn<sup>2+</sup> and the CN group. This gives rise\nto a dual-mode ion storage mechanism and favorable electrochemical\nperformances. As a result, imidazole-intercalated V<sub>2</sub>O<sub>5</sub> delivers a capacity of 179.9 mAh g<sup>–1</sup> after\n5000 cycles at 20 A g<sup>–1</sup>, while the imidazole-intercalated\nNVO harvests a high capacity output of 170.2 mAh g<sup>–1</sup> after 700 cycles at 2 A g<sup>–1</sup>. This work is anticipated\nto boost the application potentials of vanadium-based cathodes in\naqueous zinc-ion batteries.