Achieving Electronic Engineering of Vanadium Oxide-Based 3D Lithiophilic Sandwiched-Aerogel Framework for Ultrastable Lithium Metal Batteries

Lithium (Li) metal is one of the most promising anode materials for the next-generation batteries, which owns superior specific capacity and energy density. Unfortunately, lithium dendrites that is formed during the charging/discharging process tends to induce capacity degradation and thus short lifespan. In this study, the vanadium oxide (V₂O₅) and nitrogen-doped vanadium oxide (N−V₂O₃, N−VO_0.9)-modified three-dimensional (3D) reduced graphene oxide ((N)−VO_x@rGO) with tunable electronic properties are demonstrated to enable the dendrite-free Li deposition. The soft lithiophilic rGO as the scaffold can provide sufficient void space for Li storage. Meanwhile, the rigid (N)−VO_x uniformly anchored on rGO can perfectly maintain the 3D structure, which is crucial for Li to enter the inner space of the 3D framework. Consequently, the (N)−VO_x@rGO electrodes achieve dendrite-free electrodeposition under the multifarious deposition capacity and current densities. Compared with the bare lithium electrodes, the asymmetrical cells of (N)-VO_x@rGO anode can cycle stably up to 400 h at 2 mA cm⁻² current density, together with a low nucleation overpotential of ∼20 mV.(Picture