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 (V 2 O 5 ) and nitrogen-doped vanadium oxide (N-V 2 O 3 , 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.