Nitrogen-doped graphdiyne nanowall stabilized dendrite-free lithium metal anodes

Abstract

Lithium constitutes an ultimate anode material for Li metal-based batteries (LMBs, e.g., Li–S and Li–air). Nevertheless, the dendritic Li growth during repeated plating/stripping processes would cause fast capacity decay and serious safety concerns. The integration of porous current collectors with carbon nanomaterials has attracted special interest recently in suppression of Li dendrite growth. However, the large amounts of Li plating under high power conditions remain a major challenge for such hosts because most nanocarbons suffer from poor lithiophilicity. Herein, for the first time, nitrogen-doped graphdiyne nanowall-modified copper foam (N-GDY) is prepared as a highly lithiophilic host to achieve high-rate dendrite-free Li plating with high areal capacities. Such a N-GDY host features highly lithiophilic N-containing groups, abundant graphdiyne nanopores and a stable Li plating interface, guaranteeing a quite low nucleation overpotential of 13 mV and a plating/stripping coulombic efficiency of above 99.0% under synergistic conditions with high current density and areal capacity. Hence, the N-GDY@Li anode maintains a dendrite-free morphology and low voltage hysteresis under a harsh working condition for over 350 h, significantly outperforming the counterparts deposited on other carbon films. Furthermore, the N-GDY@Li anode-derived full cells also exhibit enhanced electrochemical performance towards practical applications of advanced LMBs.