Realization of a 594 Wh kg⁻¹ Lithium‐Metal Battery Using a Lithium‐Free V₂O₅ Cathode with Enhanced Performances by Nanoarchitecturing

Abstract To realize a high‐energy lithium metal battery (LMB) using a high‐capacity Li‐free cathode, in this work, nanoplate‐stacked V₂O₅ with dominantly exposed (010) facets and a relatively short [010] length is proposed to be used as a cathode. The V₂O₅ nanostructure can be fabricated via a modified hydrothermal method, including a Li⁺ crystallization inhibitor, followed by heat treatment. In particular, the enlargement of the favorable Li⁺ diffusion pathway in the [010] direction and the formation of a robust hierarchical nanoplate‐stacked structure in the modified V₂O₅ improves the electrochemical kinetics and stability; as a result, the nanoplate‐stacked V₂O₅ electrode exhibits a higher capacity and rate performance (258 mAh g⁻¹ at 50 mA g⁻¹ [0.17 C], 140 mAh g⁻¹ at 1 A g⁻¹ [3.4 C]) and cycling capability (79% capacity retention after 100 cycles at 0.5 C) compared to the previously reported V₂O₅ nanobelt electrode. Notably, the LMB composed of Li//nanoplate‐stacked V₂O₅ full‐cells shows high specific energy densities of 594.1 and 296.2 Wh kg⁻¹ at 0.1 and 1.0 C, respectively, and a high Coulombic efficiency of 99.6% during 50 cycles.