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–VO0.9)-modified three-dimensional (3D) reduced graphene oxide ((N)–VOx@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)–VOx 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)–VOx@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)-VOx@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.