Lithium
metal is the most promising anode for lithium batteries,
but the growth of lithium dendrites leads to rapid attenuation of
battery capacity and a series of safety problems during the plating/stripping
process. Utilization of carbon materials for improving the Li metal
anode stability represents a feasible strategy; particularly, the
high affinity for lithium endows graphdiyne (GDY) with a promising
capability for stabilizing Li metal anodes. Herein, vertically aligned
GDY nanowalls (NWs) were uniformly grown on a copper foil, which allowed
for dendrite-free, columnar deposition of lithium, desired for a stable
Li metal anode. The highly lithiophilic GDY NWs afforded plentiful
and evenly distributed active sites for Li nucleation as well as uniform
distribution of Li-ion flux for Li growth, resulting in smooth, columnar
Li deposition. The resultant Li metal electrode based on the Cu-GDY
NWs was able to cycle stably for 500 cycles at 1 mA cm–2 and 2 mA h cm–2 with a high Coulombic efficiency
of 99.2% maintained. A symmetric battery assembled by lithium-loaded
Cu-GDY NWs (Cu-GDY NWs@Li) showed a long lifespan over 1000 h at 1
mA cm–2 and 1 mA h cm–2. Furthermore,
a full cell assembled by Cu-GDY NWs@Li and LiFePO4 was
able to cycle stably for 200 cycles at a high current of 5 C, indicating
the potential applications in practical Li metal batteries at high
rates. This work demonstrated great potential of GDY-based materials
toward applications in Li metal batteries of high safety and high
energy density.