Sustainable and robust graphene cellulose paper decorated with lithiophilic Au nanoparticles to enable dendrite-free and high-power lithium metal anode.

Abstract

Lithium metal anodes (LMAs) with high energy density have recently captured increasing attentions for development of next-generation batteries. However, practical viability of LMAs is hindered by the uncontrolled Li dendrite growth and infinite dimension change. Even though constructing 3D conductive skeleton has been regarded as a reliable strategy to prepare low volume stress LMAs, engineering the renewable and lithiophilic conductive scaffold is still a challenge. Herein, a robust scaffold derived from renewable cellulose paper, which is coated by reduced graphene oxide and decorated with lithiophilic Au nanoparticles, is engineered for LMAs. The graphene cellulose fibres with high surface area can reduce the local current density, while the well-dispersed Au nanoparticles can serve as lithiophilic nanoseeds to lower the nucleation overpotential of\xa0plating. The coupled relationship can guarantee uniform Li nucleation and unique Li spherical growth into 3D carbon matrix. Moreover, the natural cellulose paper possesses outstanding mechanical strength to tolerate the volume stress. In virtue of the modulated deposition behaviour and near-zero volume change, the hybrid LMAs can achieve reversible Li plating/stripping at ultrahigh current density of 10 mA cm-2 as evidenced by high Coulombic efficiency (97.2% after 60 cycles) and ultralong lifespan (1000 cycles) together with ultralow overpotential (25 mV). Therefore, this strategy sheds light on a scalable approach to multiscale design versatile Li host, promising highly stable Li metal battery to be feasible and practical.