Al-ion
batteries (AIBs) represent promising multivalent-ion battery
alternatives to Li-ion batteries (LIBs). Exploration of cathode materials
is the key to improving the electrochemical performance of AIBs. Here
we demonstrate a promising AIB cathode candidate based on two-dimensional
graphitic carbon nitride (g-C3N4) nanosheets
with reversible de/embedding of [AlCl4]− anions in its special layered porous structure during the cyclic
charge/discharge process. To address the sluggish ion/charge transportation
kinetics that is inherently present in AIBs due to the intrinsically
low conductivity of g-C3N4, we optimize different
synthetic precursors of g-C3N4 including dicyandiamide,
urea, and melamine and, further, develop a facile method for uniformly
coating a N-doped carbon (N–C) coating layer on the optimal
g-C3N4 derived from dicyandiamide. The resultant
AIBs consisting of the g-C3N4@N–C cathode
and Al metal anode in the AlCl3/[EMIm]Cl electrolyte exhibit
an initial capacity of ∼54.9 mAh·g–1 at 0.2 C with a high Coulomb efficiency ∼99.9%, and they
possess long-term cycling over 200 cycles. The underlying charge/discharge
process of AIBs, revealed by the ex situ X-ray diffraction and scanning
electron microscopy analyses, involves the extraction/insertion of
Al species (mainly Al3+, AlCl4
–, and Al2Cl7
–) into the g-C3N4 crystal lattices with the formation of intermediate
Al8C3N4 and (ClCN)3.